Gao et al.

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4 Coupling between the DEAD-box RNA

5 Ded1p and eIF4A

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10 Zhaofeng Gao1, Andrea A. Putnam 1, Heath Bowers 1, Ulf-Peter Guenther1, Xuan Ye 1,

11 Audrey Kindsfather2, Angela K.Hilliker2 & Eckhard Jankowsky1

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15 1 Center for RNA Molecular Biology & Department of Biochemistry

16 School of Medicine, Case Western Reserve University, Cleveland, OH

17 2 Department of Biology, University of Richmond, Richmond, VA

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18 Abstract

19 Eukaryotic translation initiation involves two conserved DEAD-box RNA helicases, eIF4A and

20 Ded1p. Here we show that S. cerevisiae eIF4A and Ded1p directly interact with each other and

21 simultaneously with the scaffolding protein eIF4G. We delineate a comprehensive

22 thermodynamic framework for the interactions between Ded1p, eIF4A, eIF4G, RNA and ATP,

23 which indicates that eIF4A, with and without eIF4G, acts as modulator for activity and substrate

24 preferences of Ded1p, which is the RNA remodeling unit in all complexes. Our results reveal

25 and characterize an unexpected interdependence between the two RNA helicases and eIF4G,

26 and suggest that Ded1p is an integral part of eIF4F, the complex comprising eIF4G, eIF4A, and

27 eIF4E.

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28 Introduction

29 Translation initiation in involves at least 12 distinct protein factors, including

30 two highly conserved DEAD-box RNA helicases, eIF4A and Ded1p (DDX3 in human) (Aitken

31 and Lorsch, 2012; Hinnebusch, 2014; Parsyan et al., 2011). DEAD-box RNA helicases,

32 whose name is inspired by a characteristic (D-E-A-D, in single letter code), are

33 enzymes that utilize ATP to bind and remodel RNA and RNA-protein complexes (Linder and

34 Jankowsky, 2011). While S. cerevisiae eIF4A (~105 copies per cell) is roughly five times more

35 abundant in the cell than Ded1p (Firczuk et al., 2013), both helicases are essential for viability

36 (Linder and Slonimski, 1989; Giaever et al., 2002).

37 eIF4A unwinds RNA duplexes in vitro (Merrick, 2015). In the cell, the interacts

38 with the large scaffolding protein eIF4G that also binds the cap-binding protein eIF4E

39 (Hinnebusch,2014; Parsyan et al., 2011). The complex containing eIF4G, eIF4E and eIF4A is

40 called eIF4F (Merrick, 2015). eIF4A binds to a MIF4G domain of eIF4G (Schütz et al., 2008),

41 and this interaction stimulates RNA- and ATP-binding, and ATP-dependent RNA unwinding

42 activity of eIF4A in vitro (Hilbert et al., 2011; Rajagopal et al., 2012). In translation initiation,

43 eIF4A is thought to be critical for steps during and subsequent to recruitment of the 40S

44 subunit to the mRNA (Parsyan et al., 2011). In S. cerevisiae, eIF4A appears to

45 promote at least one step necessary for the translation of most or all mRNAs (Sen et al., 2015).

46 Ded1p unwinds RNA duplexes in vitro as a trimer, whose formation requires the C-

47 terminus (Putnam et al., 2015). Ded1p also facilitates strand annealing, RNA structure

48 conversions, and the remodeling of RNA-protein complexes (Bowers et al., 2006; Iost et

49 al.,1999; Yang et al., 2007b; Yang and Jankowsky, 2005). Both, Ded1p and human DDX3X

50 interact with the cap binding protein eIF4E (Senissar et al., 2014; Shih et al., 2008), and with

51 eIF4G (Hilliker et al., 2011; Soto-Rifo et al., 2012). Ded1p uses its C-terminus to bind to the C

52 terminus of eIF4G, a region distinct from the eIF4A binding site in eIF4G (Hilliker et al., 2011).

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53 The interaction with eIF4G interferes with Ded1p oligomerization and thus inhibits RNA

54 unwinding by the helicase (Putnam et al., 2015). In translation initiation, Ded1p and DDX3X

55 have been implicated in mRNA recognition by eIF4F, recruitment of the 40S ribosome subunit to

56 the mRNA, the scanning process, start codon selection and joining of the two ribosomal

57 subunits (Sharma and Jankowsky, 2014). Misregulation of DDX3X expression and mutations

58 in the helicase core of DDX3X are associated with tumors, including medulloblastoma, lung-

59 and colorectal cancer and T-cell lymphoma (Bol et al., 2015; Heerma van Voss et al., 2015;

60 Jianget al., 2015; Pugh et al., 2012). DDX3 is also targeted by multiple pathogenic viruses

61 including HIV, HCV, other flaviviridae, poxviridae, and HBV (Valiente-Echeverría et al., 2015).

62 Previous data indicate genetic interactions between eIF4A and Ded1p (de la Cruz et al.,

63 1997; Senissar et al., 2014), and a recent, transcriptome-wide study in yeast shows

64 overlapping, but not identical functions of eIF4A and Ded1p in translation initiation (Sen et al.,

65 2015). While these data suggest a possible link between the two helicases, Ded1p and eIF4A

66 have been generally viewed as separately functioning factors. Despite the central biological

67 roles of the two enzymes, their level of conservation, and their implication in numerous

68 diseases, it is unknown whether and how eIF4A and Ded1p are linked biochemically and

69 physically, and if their functions are coordinated. The answer to these questions is of

70 considerable importance for understanding eukaryotic translation initiation on the molecular

71 level. However, experimentally addressing the link between the two enzymes presents

72 significant challenges. First, as RNA helicases, eIF4A and Ded1p share basic biochemical

73 properties including RNA binding, unwinding, ATP binding and ATP turnover. Therefore,

74 enzymatic readouts are similar and potentially difficult deconvolute. Second, both helicases

75 interact with eIF4G, which also binds RNA. The multitude of possible individual interactions

76 significantly complicates the analyses of coupling between the proteins. Third, interactions

77 between the proteins are likely transient or dynamic, given that both, Ded1p and eIF4A bind and

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78 hydrolyze ATP, which in turn modulates RNA binding by the helicases (Linder and Jankowsky,

79 2011). Functional analysis of dynamic multi-component assemblies is not well developed, even

80 though such RNA-protein complexes are numerous in biology.

81 Here, we have confronted the experimental challenges associated with links between

82 Ded1p, eIF4A, eIF4G, ATP and RNA. Using quantitative biochemical and enzymological

83 approaches, we show that Ded1p and eIF4A directly interact with each other and that both

84 helicases simultaneously interact with eIF4G. We devise an unbiased, comprehensive

85 thermodynamic framework for the interactions between Ded1p, eIF4A, eIF4G, RNA and ATP.

86 This framework indicates that eIF4A, with and without eIF4G, acts as modulator for activity and

87 substrate preferences of Ded1p, and that Ded1p functions as the RNA remodeling unit in

88 complexes with eIF4A. Our observations reveal an unexpected interdependence between both

89 RNA helicases and eIF4G, and suggest that Ded1p is an integral part of the eIF4F complex.

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90 RESULTS

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92 Direct interactions between Ded1p, eIF4A and eIF4G.

93 We identified eIF4A in a screen for genes that suppress a cold-sensitive growth defect

94 conferred by DED1 mutations (ded1-tam, Hilliker et al., 2011). Overexpression of eIF4A

95 partially restored growth at non-permissive temperatures (Figure 1A), suggesting that eIF4A

96 can promote Ded1p's function, but not completely substitute for its tasks. This observation is

97 consistent with the notion that Ded1p and eIF4A have overlapping, but not identical functions in

98 translation initiation (Sen et al., 2015).

99 To further examine the connection between Ded1p and eIF4A in the cell, we tested

100 whether the eIF4A inhibitor hippuristanol exacerbated the temperature-sensitive growth defect

101 associated with the ded1-95 strain (Burckin et al., 2005). Ded1-95 bears a T408I mutation,

102 which impairs RNA binding by Ded1p in vitro (Figure 1- figure supplement 1). Hippuristanol

103 inhibits the activities of eIF4A, but not those of Ded1p (Bordeleau et al., 2006). Here,

104 Hippuristanol diminished growth of the ded1-95 strain, compared to the WT ded1 strain (Figure

105 1B), indicating that targeted inhibition of eIF4A can impact a growth defect associated with a

106 mutation in DED1. Collectively, these observations expand the scope of genetic interactions

107 between the two DEAD-box helicases. However, the data did not reveal the physical nature of

108 the link between Ded1p and eIF4A.

109 To probe physical connections between the two helicases, we performed pull-down

110 experiments with recombinant, purified proteins (Figure 1C,D). Previous data had shown that

111 both helicases bind to distinct regions of the scaffolding protein eIF4G (Hilliker et al., 2011;

112 Merrick, 2015). It was thus important to determine whether Ded1p could directly interact with

113 eIF4A, and to probe whether both proteins could interact simultaneously with eIF4G. Reactions

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114 were performed with RNases to exclude possible RNA bridging of the three RNA binding

115 proteins. EIF4A bound directly to Ded1p (Figure 1C, lanes 2). This observation indicates a

116 direct interaction between the two DEAD-box helicases that does not depend on RNA or

117 another factor. EIF4A increased the amount of eIF4G bound to immobilized Ded1p (Figure 1C,

118 compare lanes 1 and 3). As expected, Ded1p bound to immobilized eIF4G (Figure 1D, compare

119 lanes 5 and 7). Ded1p increased the amount of bound eIF4A to eIF4G (Figure 1D, compare

120 lanes 6 and 7). Together, the data reveal a direct interaction between Ded1p and eIF4A and

121 promotion of Ded1p-eIF4G binding by eIF4A. The observations show that interactions between

122 Ded1p, eIF4G, and eIF4A are not mutually exclusive and suggest that all three proteins can

123 interact simultaneously.

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125 Complexes between Ded1p, eIF4A and eIF4G are unwinding-competent.

126 We next probed whether complexes formed between Ded1p and eIF4A alone or in

127 combination with eIF4G were biochemically active. To this end we measured ATP-dependent

128 RNA unwinding activity for the various protein combinations using an RNA substrate with a 16

129 bp duplex. This substrate was unwound by Ded1p with a much larger apparent rate constant

130 than seen for eIF4A (Figure 1E), consistent with expectations based on previous studies

131 (Rajagopal et al., 2012; Yang et al., 2007a). Nevertheless, addition of eIF4A stimulated the

132 unwinding activity of Ded1p (Figure 1E). Since the weak activity of eIF4A rules out additive

133 effects of the two helicases, the data reveal an impact of eIF4A on the helicase activity of

134 Ded1p, indicating an unwinding-competent eIF4A-Ded1p complex.

135 Addition of eIF4G to Ded1p and eIF4A further increased the unwinding activity seen with

136 only Ded1p and eIF4A (Figure 1E). In contrast, addition of eIF4G to Ded1p alone decreased

137 the rate constant for Ded1p, as previously reported (Putnam et al., 2015). The weak activity of

138 eIF4A with eIF4G precludes additive effects of Ded1p and the eIF4A-eIF4G complex

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139 (Rajagopal et al., 2012). Our data therefore suggest that Ded1p, eIF4A and eIF4G can function

140 together to unwind RNA duplexes.

141 Preparations of eIF4G contained the cap binding protein eIF4E (Hilliker et al., 2011),

142 which is required for stability of eIF4G in vitro (Dominguez et al., 2001). EIF4E had been

143 previously shown to interact with Ded1p, but it did not affect the RNA-stimulated ATPase activity

144 of Ded1p (Senissar et al., 2014). Consistent with these results, we did not detect a significant

145 impact of eIF4E on the unwinding activity of Ded1p (not shown). We therefore did not further

146 investigate the impact of eIF4E alone.

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148 Ded1p is the unwinding module in complexes with eIF4A and eIF4G.

149 We next examined the respective contributions of eIF4A and Ded1p to the unwinding

150 activity when both enzymes were present. We first included hippuristanol in the unwinding

151 reactions (Figure 2A, Figure 2-figure supplement 1). As expected, hippuristanol decreased

152 unwinding activity for eIF4A alone and in combination with eIF4G, but did not significantly

153 impact unwinding of Ded1p alone or in combination with eIF4G (Figure 2A). However,

154 hippuristanol decreased unwinding for Ded1p in the presence of eIF4A, with and without eIF4G,

155 essentially to the level seen with Ded1p alone (Figure 2A). The data suggest that Ded1p is the

156 unwinding module in the complexes with eIF4A, but that functional integrity of eIF4A is

157 important for its impact on Ded1p. This observation provides a rationale for the exacerbating

158 effect of hippuristanol on the growth defect of the ded1-95 mutant strain (Figure 1B). To further

159 probe the role of eIF4A in complexes with Ded1p, we tested the impact of a mutation of the ATP

160 binding site of eIF4A (eIF4AE171A), which abolishes RNA unwinding, as well as ATP binding and

161 hydrolysis (Iost et al., 1999). EIF4AE171A stimulated unwinding by wtDed1p (Figure 2B).

162 However, addition of eIF4G reduced the stimulation to the level roughly seen with Ded1p alone

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163 (Figure 2B). These observations provide additional evidence that Ded1p is the unwinding

164 module in complexes with eIF4A.

165 A mutation in the ATP binding site of Ded1p (Ded1pE307A), which abolishes RNA

166 unwinding, as well as ATP binding and hydrolysis (Hilliker et al., 2011; Iost et al., 1999), did

167 not notably alter the basal unwinding activity of eIF4A alone or with eIF4G (Figure 2C). This

168 observation indicates that unwinding activity of Ded1p dictates the level of activity seen in

169 complexes with eIF4A and eIF4G. Finally, we tested the Ded1pT408I mutation (Figure 2D), which

170 showed lower activity than wtDed1p, but higher unwinding activity than eIF4A alone or in

171 complex with eIF4G (Figure 2B,C,D, compare first points). EIF4A stimulated Ded1pT408I and

172 addition of both, eIF4A and eIF4G, stimulated even more (Figure 2D). Collectively, these data

173 show that Ded1p determines the level of unwinding activity in complexes with eIF4A, further

174 supporting the notion that Ded1p is the unwinding module in the complexes with eIF4A.

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176 The N-terminus of Ded1p is critical for interaction with eIF4A.

177 We next asked which region of Ded1p was critical for the interaction with eIF4A. We

178 removed the C-terminus of Ded1p (Ded1p1-535), which interacts with eIF4G (Hilliker et al.,

179 2011), and measured unwinding activity of Ded1p1-535 with eIF4A, eIF4G, or both (Figure 3A).

180 As expected, eIF4G alone did not notably impact Ded1p1-535,which showed lower unwinding

181 activity than wt Ded1p. EIF4A stimulated Ded1p1-535, and this stimulation was increased by

182 eIF4G (Figure 3A). These observations imply that the C-terminus of Ded1p is not critical for the

183 interaction with eIF4A, even in the presence of eIF4G.

184 We next measured the impact of eIF4A, eIF4G, or both on Ded1p117-604, which lacked the

185 N-terminus. Compared to wt Ded1p, Ded1p117-604 showed reduced unwinding activity (Figure

186 3A). EIF4G alone slightly stimulated Ded1p117-604, consistent with an interaction between eIF4G

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187 and Ded1p117-604. The slight stimulation of Ded1p117-604 by eIF4G, as opposed to the inhibition

188 seen with wtDed1p, likely reflects an increase in RNA affinity of Ded1p117-604 by eIF4G. This

189 increase in affinity is also seen with wtDed1p, but does not result in a stimulation of the wild type

190 protein under identical reaction conditions (Putnam et al., 2015). Most notably, eIF4A no longer

191 stimulated Ded1p117-604, and addition of eIF4G did not increase the activity further (Figure 3A).

192 No direct interaction between Ded1p117-604 and eIF4A was detected in pull down experiments

193 (Figure 3- figure supplement 1A). Together, the data show that the N-terminus of Ded1p is

194 important for the interaction between eIF4A and Ded1p, with and without eIF4G, and further

195 support the notion that eIF4A and Ded1p do not simply act additively.

196 In the cell, deletion of the N-terminus conferred a severe cold-sensitive growth

197 phenotype (Figure 3B), consistent with a prior report (Banroques et al., 2011). Notably,

198 overexpression of eIF4A did not alleviate the cold-sensitive growth defect of Ded1p117-604

199 (Figure 3B), as it had for another Ded1p mutation (Figure 1A). This observation emphasizes

200 the biological significance of the interaction between eIF4A and the N-terminus of Ded1p.

201 In contrast to the N-terminus, the C-terminus of Ded1p was not critical for interaction

202 with eIF4A, even in the presence of eIF4G. Given that the C-terminus is important for

203 trimerization of Ded1p (Putnam et al., 2015), our findings raised the question whether Ded1p in

204 complexes with eIF4A was still able to form trimers. We therefore examined the impact of eIF4A

205 on oligomerization of Ded1p using chemical protein-protein crosslinking (Figure 3C). Without

206 eIF4A, trimer formation of Ded1p was seen (Putnam et al., 2015). With eIF4A, no Ded1p trimer

207 was observed, and a prominent new species emerged with a molecular weight consistent with a

208 predominant one to one Ded1p-eIF4A complex (Figure 3C, Figure 3-figure supplement 1B,

209 1C). The Ded1p dimer species seen in the sample with eIF4A represents remaining Ded1p. The

210 data thus indicate that eIF4A interferes with Ded1p oligomerization, even though the C-terminus

211 of Ded1p is not critical for the complex formation with eIF4A.

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212 Collectively, results shown above and previous data on the Ded1p-eIF4G interaction and

213 Ded1p oligomerization (Putnam et al., 2015) suggest a basic model for the functional

214 architecture of the complexes formed between Ded1p, eIF4A, and eIF4G (Figure 3D). Without

215 eIF4A, Ded1p interacts via its C-terminus with eIF4G. This interaction precludes formation of a

216 Ded1p trimer (Putnam et al., 2015). The main contact between Ded1p and eIF4A involves the

217 N-terminus of Ded1p, even in the presence of eIF4G and eIF4A also interferes with

218 oligomerization of Ded1p.

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220 A quantitative framework for the interactions between Ded1p, eIF4A, eIF4G, RNA, and

221 ATP

222 The data above indicated the existence of multiple complexes formed between Ded1p,

223 eIF4A, and eIF4G. To understand biochemical characteristics of these complexes, their

224 interdependencies, and the roles of ATP and RNA, we set out to establish a mechanistic

225 framework describing the thermodynamic stability of these complexes, their RNA and ATP

226 affinities, and their unwinding activities. To our knowledge, no comparable framework exists for

227 any dynamic complex with multiple RNA binding proteins. To devise an instructive quantitative

228 model, it was important to measure the interactions under conditions where ATP binding and

229 turnover as well as RNA binding and remodeling occurred simultaneously. These conditions are

230 best met in unwinding reactions. We therefore performed a large set of unwinding reactions

231 where we systematically varied concentrations of Ded1p, eIF4A, eIF4G, and ATP.

232 Representative data show, among other trends, scaling of the Ded1p stimulation with ATP and

233 Ded1p concentrations, and biphasic response curves with increasing concentrations of eIF4G

234 (Figure 4-figure supplements 1-4). The data indicate intricate interdependencies between the

235 three proteins, ATP and RNA.

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236 Using the measured unwinding data, we assembled a quantitative model to describe the

237 thermodynamic stability of all complexes formed between Ded1p, eIF4A, and eIF4G, their RNA

238 and ATP affinities, and their unwinding rate constants (Figure 4A). Model building, data fitting

239 strategy and assessment of model quality are described the Methods section, in Figure 4-

240 figure supplements 5,6, and Supplementary files 2,3. The model considers all 28 distinct

241 complexes formed between Ded1p, eIF4A, eIF4G, RNA and ATP (Figure 4A), plus complexes

242 formed by Ded1p during oligomerization (Putnam et al., 2015). 108 individual interactions were

243 modeled and more than 3,000 individual data points were used in the global datafit. Interactions

244 between Ded1p, eIF4A and eIF4G were modeled as one to one interactions, based on the data

245 above (Figure 3C), and on previous data characterizing the Ded1p-eIF4G interaction (Putnam

246 et al., 2015). The model faithfully recapitulates measured unwinding rate constants (Figure 4B,

247 Figure4-figure supplement 6) as well as previously reported ATP affinities for eIF4A and the

248 eIF4A-eIF4G complex (Rajagopal et al., 2012; Mitchell et al., 2010) (Supplementary file 2).

249 The model reveals the formation of a thermodynamically stable complex between

250 Ded1p, eIF4A, and eIF4G, whose stability further increases with ATP, RNA, or both (Figure 5A,

251 Supplementary file 2F). The stability of the Ded1p-eIF4A complex, although lower than for the

252 Ded1p-eIF4A-eIF4G complex, also increases with ATP, RNA, or both (Figure 5A,

253 Supplementary file 2D). In contrast, the Ded1p-eIF4G, and eIF4A-eIF4G complexes are more

254 stabilized by RNA than by ATP (Figure 5A, Supplementary file 2C-E). To independently verify

255 the calculated high stability of the Ded1p-eIF4G-eIF4A complex, we used microscale

256 thermophoresis (MST) (Seidel et al., 2013) to directly measure binding of Ded1p to a pre-

257 formed eIF4G-eIF4A complex in the absence of RNA and ATP. We measured an apparent

258 dissociation constant of K1/2 < 7 nM (Figure 5B), the experimentally accessible lower limit of

259 affinity with the available MST setup. This value is consistent with the corresponding affinity

260 calculated with our model (Supplementary file 2F). Given the high thermodynamic stability of

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261 the Ded1p-eIF4G-eIF4A complex, we suggest to consider Ded1p, like eIF4A, as integral

262 functional part of eIF4F. We note that high thermodynamic stability does not equal persistence

263 of the complex. In fact, the complex between the three proteins is unlikely to be long-lived, given

264 that both eIF4A and Ded1p constantly turn over ATP.

265 Our model further revealed that unwinding rate constants at ATP and protein saturation

266 and RNA affinities at ATP saturation are similar for the Ded1p trimer and for the complexes

267 containing Ded1p and eIF4A (Figure 5C, Supplementary file 2A). Ded1p is stimulated by

268 eIF4A at lower Ded1p concentrations because the complexes with eIF4A bind as single units

269 with hyperbolic binding isotherms, whereas Ded1p oligomerizes cooperatively, which results in

270 a sigmoidal isotherm (Figure 5D, Figure 4-figure supplement 1). Accordingly, stimulation of

271 Ded1p by eIF4A, with or without eIF4G, decreases at higher Ded1p concentration (Figure 4-

272 figure supplements 1A,B). The similar unwinding rate constants at ATP and protein saturation

273 for the Ded1p trimer, the Ded1p-eIF4A and the Ded1p-eIF4A-eIF4G complexes are consistent

274 with the notion that a Ded1p protomer acts as the unwinding unit in the complexes with eIF4A.

275 ATP turnover by Ded1p was not significantly affected by eIF4A and eIF4G (Figure 5-figure

276 supplement 1), supporting the notion that the strand separation by a Ded1p protomer is largely

277 unaffected by eIF4A, with and without eIF4G. The observations suggest that eIF4A and eIF4G

278 function to recruit Ded1p as RNA remodeling unit.

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280 Modulation of Ded1p activity by eIF4A and eIF4G is impacted by substrate architecture.

281 Having dissected biochemical interdependencies between Ded1p, eIF4A and eIF4G, we

282 next tested whether and how the substrate architecture (lengths of duplexes, lengths and

283 orientation of unpaired tails) impacts the degree by which eIF4A, eIF4G, or both, modulate the

284 unwinding activity of Ded1p. We first performed unwinding reactions with substrates containing

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285 different overhang orientations (Figure 6A). We found a modestly enhanced preference of 3’ vs.

286 5' tailed substrates for Ded1p with eIF4A and eIF4G (Figure 6A). This observation is notable,

287 because eIF4G imparts on eIF4A alone a preference for 5’ tailed substrates (Rajagopal et al.,

288 2012) (Figure 6-figure supplement 1).

289 We next examined the impact of the length of the unpaired 3' tail (Figure 6B,C; Figure

290 6-figure supplement 2). To this end, we obtained functional affinities for the various protein

291 complexes for a substrate with 10 nt 3' overhang (Figure 6B). These parameters were

292 calculated from sets of unwinding reactions with the 10 nt tailed substrate with varying

293 concentrations of Ded1p, eIF4A, and eIF4G, analogous to the process described for the

294 substrate with the 25 nt overhang (Figure 6-figure supplement 3). We then compared the

295 functional affinities for the 10 and the 25 nt tailed substrates for each protein complex (Figure

296 6B). For Ded1p alone, affinity increased for a 25 nt vs. a 10 nt tail (Figure 6B, lower panel),

297 consistent with previous observations (Yang et al., 2007a). Addition of eIF4A, eIF4G, or both,

298 increased the relative affinity of the complexes for 25 nt vs. 10 nt tails (Figure 6B). Yet, at low

299 Ded1p concentrations, eIF4A and eIF4G stimulated Ded1p unwinding stronger for a substrate

300 with a 10 nt tail (Figure 6- figure supplement 2), compared to a substrate with a 25 nt tail

301 (Figure 6A). The stronger stimulation for substrates with shorter tails arises from the hyperbolic

302 shape of the functional binding isotherm of the Ded1p-eIF4G-eIF4A complex, compared to the

303 sigmoidal isotherm for the Ded1p trimer (Figure 6C). These data show that activity stimulation

304 can scale with the concentration of components, without a marked change in affinity.

305 Finally, we examined the impact of duplex length on the degree by which eIF4A, eIF4G,

306 or both, modulated the unwinding activity of Ded1p (Figure 6D; Figure 6-figure supplement

307 2). Since duplex length impacts only the unwinding rate constant, but not the substrate affinity

308 (Putnam et al., 2015), we calculated unwinding rate constants at ATP and enzyme saturation

309 for duplexes of different length using our thermodynamic model (Figure 4), and data collected

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310 from substrates with 13, 16, and 19 basepairs and identical 3', 25 nt overhangs (Figure 6D).

311 The shortest duplex was unwound fastest by the eIF4A-Ded1p complex, and slowest by the

312 eIF4A-eIF4G-Ded1p complex. For the longest duplex, this order was reversed (Figure 6D). The

313 scaling of the unwinding rate constants with duplex length correlates with the process of strand

314 separation (Putnam et al., 2015). The data thus indicate that both eIF4A and eIF4G directly

315 affect the strand separation step by the Ded1p protomer. EIF4A most likely increases the time

316 by which partially opened duplex stands are kept apart, while decreasing the number of

317 basepairs opened per strand separation event. In contrast, eIF4G and eIF4A together appear to

318 decrease the time by which partially opened duplex stands are kept apart, while increasing the

319 number of basepairs opened per strand separation event. For substrates containing a 5' tail, no

320 comparable scaling of the stimulation with the duplex length was seen, although the stimulation

321 was somewhat higher for the longer duplex (Figure 6A, Figure 6-figure supplement 2).

322 Collectively, our data show that substrate architecture influences the degree by which unwinding

323 activity of Ded1p is impacted by eIF4A and eIF4G, alone and in combination. Our observations

324 further reveal that eIF4A and eIF4G directly influence the strand separation step of Ded1p

325 (Figure 6D), and that substrate affinity of each protein complex scales with the length of the

326 unpaired tail (Figure 6B,C).

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327 DISCUSSION

328

329 In this study, we demonstrate direct and functional interactions between the DEAD-box

330 helicases eIF4A and Ded1p. Although both helicases have been firmly implicated in translation

331 initiation, they had not been viewed as physically connected. Our data further show that eIF4A

332 and Ded1p simultaneously interact with eIF4G to form a thermodynamically stable complex. The

333 findings reveal a previously unknown physical and functional interconnection between Ded1p,

334 eIF4A and eIF4G, and suggest that Ded1p is an integral functional part of the eIF4F complex.

335 Our data show that Ded1p, eIF4A and eIF4G, all of which bind RNA, can form four

336 discrete complexes (Ded1p-eIF4A, Ded1p-eIF4G, Ded1p-eIF4A-eIF4G, eIF4A-eIF4G) with

337 defined biochemical properties. Most importantly, Ded1p is the primary RNA remodeling unit in

338 all complexes where it is present. Compared to previously described complexes between eIF4A,

339 eIF4G, and eIF4B, the complexes with Ded1p display orders of magnitude more potent RNA

340 remodeling activity than complexes that only contain eIF4A. This observation raises the

341 possibility that remodeling of stable RNA structures in cellular 5'UTRs, which is often attributed

342 to eIF4A, might in fact be carried out by complexes that contain Ded1p.

343 Our data suggest that the various complexes readily form at physiological concentrations

344 of protein, RNA and ATP. Affinities determined with our model and reported cellular

345 concentrations of the proteins, RNA and ATP (Firczuk et al., 2013; Koç et al., 2004;

346 Zenklusen et al., 2008), allowed us to estimate the prevalence of all complexes at

347 concentrations around the physiological concentrations of Ded1p and eIF4G (Figure 7). These

348 calculations suggest that all complexes exist under physiological conditions, thus rationalizing

349 reported co-immunoprecipitation data (Senissar et al., 2014). The calculations further show that

350 at the reported cellular concentrations of Ded1p and eIF4G (~ 1 μM), most of these two proteins

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351 are bound in the Ded1p-eIF4A-eIF4G complex (Figure 7). Almost all of the remaining Ded1p

352 and remaining eIF4G is bound to eIF4A, and only little Ded1p oligomer is present.

353 Variations of both, Ded1p and eIF4G concentrations, even by a factor of only two,

354 significantly alter the prevalence of the respective complexes, with strikingly distinct functional

355 impact for Ded1p and eIF4G. For Ded1p, the changes in the complex ratio have only little

356 impact on helicase activity, since complexes with Ded1p have similar unwinding activities and

357 RNA affinities, although this depends somewhat on the duplex length (Figure 6B,D). Increasing

358 eIF4G concentrations dramatically decreases the fraction of eIF4G that is associated with

359 Ded1p and thus with potent remodeling activity. These observations suggest that Ded1p, in

360 addition to eIF4A, might be important for the function of eIF4G. The data provide a possible

361 rationale for the roughly equal cellular concentration of eIF4G and Ded1p (Firczuk et al., 2013).

362 The Ded1p-eIF4A-eIF4G complex is thermodynamically most stable, suggesting an

363 evolutionary adaptation to favor formation of this complex. For this reason, we suggest to

364 consider Ded1p, like eIF4A, as integral part of eIF4F. Our data highlight a previously unknown

365 role of eIF4A as co-factor for Ded1. This function is consistent with recently discovered

366 overlapping roles of Ded1p and eIF4A in translation initiation (Sen et al., 2015), and with the

367 partial complementation of ded1 mutations by overexpression of eIF4A (Figure 1A). Since the

368 cellular eIF4A concentration exceeds the Ded1p concentration by a factor of approximately five,

369 our findings do not exclude roles of eIF4A in translation initiation that are independent of Ded1p.

370 Our results define a basic functional architecture of the complexes between Ded1p

371 eIF4A and eIF4G (Figure 3D). Most notably, Ded1p utilizes distinct regions to bind to eIF4A and

372 eIF4G. If eIF4A is present, the Ded1p N-terminus is most critical for binding, whereas the Ded1p

373 C-terminus is critical for binding to eIF4G alone. eIF4G and eIF4A allosterically affect the

374 unwinding activity of the Ded1p protomer. In energetic terms, these effects are smaller than the

375 allosteric impact of co-factors on RNA helicases seen in other multi-component complexes,

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Gao et al.

376 such as the TRAMP complex (Jia et al., 2011). However, Ded1p allosterically impacts eIF4A,

377 eIF4G, or both, as reflected in the marked increase in RNA affinity for the two proteins. This

378 increase in the RNA affinity most likely indicates a function of the proteins as RNA binding

379 adaptors for the Ded1p protomer that separates the strands. Unwinding activity and RNA affinity

380 in the Ded1p-eIF4A, and Ded1p-eIF4A-eIF4G complexes depends on the substrate architecture

381 to a moderate degree, but substrate preferences of Ded1p are not drastically altered by eIF4A

382 or by eIF4A-eIF4G.

383 The intricate connection between Ded1p, eIF4G and eIF4A implies that removal of

384 Ded1p or disruption of the interaction between Ded1p and eIF4A profoundly affects RNA

385 remodeling by complexes that contain eIF4A. In addition, complexes containing Ded1p are

386 more sensitive to ATP depletion and inhibition by AMP than complexes containing only eIF4A,

387 because Ded1p has weaker ATP affinity than eIF4A (Putnam et al., 2015; Putnam and

388 Jankowsky, 2013; Rajagopal et al., 2012). Complexes with Ded1p might therefore be more

389 sensitive to the metabolic state of the cell than complexes with only eIF4A (Putnam and

390 Jankowsky, 2013). Broad regulatory potential is thus likely to be associated with the interaction

391 between Ded1p to eIF4A. Consistent with this hypothesis, the Ded1p N-terminus that binds to

392 eIF4A, harbors a multitude of proven and potential sites for post-translational modifications

393 (Sharma and Jankowsky, 2014). Modification of these sites could affect the interaction with

394 eIF4A.

395 Finally, our quantitative analysis of dynamic complexes formed by multiple RNA binding

396 proteins emphasizes that effects of these proteins on each other cannot simply be described as

397 "stimulating" or "inhibiting". Because multiple sub-complexes are often simultaneously present,

398 both in vitro and in the cell, observed effects depend on the concentration of individual proteins,

399 relative to each other and in absolute molar terms, and on ATP and RNA concentrations. For

400 these reasons, frameworks such as the one developed in this study are required to adequately

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Gao et al.

401 describe biochemical features of individual complexes, and to define the interactions between

402 all factors, especially if the complexes are not long lived. Approaches outlined in this work could

403 therefore be useful for the quantitative analysis of other dynamic complexes that contain

404 multiple RNA-binding proteins.

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Gao et al.

405 MATERIALS AND METHODS

406

407 Recombinant Proteins

408 Ded1p and mutant Ded1p proteins

409 Wild type Ded1p with an N-terminal His6-tag (plasmid: pET-22b(+)-DED1, Supplementary file

410 1C) was expressed in E. coli (BL21) and purified and characterized as described (Yang and

411 Jankowsky, 2005).

T408I 412 The plasmid for recombinant Ded1p with N-terminal His6-tag (pEJ13, Supplementary

413 file 1C) was generated by site-directed mutagenesis of pET-22b(+)-DED1with primers X11 and

414 X12 (Supplementary file 1B). The presence of the ded1-95 allele in the transformants was

415 probed for by amplifying plasmid DNA with primers X53 and X54 and subsequent restriction

416 fragment length analysis with DdeI (New England Biolabs) according to the manufacturer’s

417 suggestions. The restriction enzyme cuts only the WT allele but leaves the ded1-95 allele uncut.

418 WT controls were included in the assay to ensure the validity of the reaction conditions.

419 Ded1pT408I was expressed in E. coli (BL21) and purified and characterized as described (Yang

420 and Jankowsky, 2005).

E307A E307A 421 The plasmid for Ded1p (N-terminal His6-tag, pET-22b(+)-DED1 , Supplementary

422 file 1C) was a gift from Dr. Patrick Linder (Geneva, Switzerland, Iost et al., 1999). Ded1pE307A

423 was expressed in E. coli (BL21) and purified and characterized as described wt Ded1p

424 described (Yang and Jankowsky, 2005).

425 To produce recombinant HA-tagged Ded1p (Ded1p-HA, N-terminal His6-tag and C-terminal

426 HA3-tag, plasmid:pET-22b(+)-His-Ded1-HA), DED1 from yeast genomic DNA was amplified by

427 PCR with primers zfDD10 and zfDD11 (Supplementary file 1B). The PCR product was gel

428 purified, digested with HindIII and PstI, and ligated into the plasmid pBlueScript II KS(+).

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Gao et al.

429 Tandem triple HA tags were inserted with PCR amplification of the new plasmid with the primers

430 zfDD12 and zfDD13 (Supplementary file 1B). The resulting pBS II KS(+)-DED1-HA plasmid

431 was digested with NheI and HindIII and the ~2.0 kb fragment containing the coding sequence

432 for His6-Ded1p-HA3 was gel purified. The pET-22b(+)-DED1 plasmid was digested with NheI

433 and HindIII and the ~7.0 kb product containing the backbone of pET-22b(+) was gel purified.

434 The two gel purified fragments were ligated to form pET-22b(+)-His-Ded1-HA. The coding

435 sequence in the plasmid was verified by sequencing. The plasmid was transfected into E.coli

436 (BL21), and recombinant Ded1p-HA was expressed, purified, and characterized as wild type

437 Ded1p.

438 Ded1p1-535 (C-terminus deleted, pET-22b(+)-His- DED11-535) was expressed in E. coli (BL21)

439 and purified and characterized as described (Hilliker et al., 2011).

440 To produce recombinant Ded1p117-604 (N-terminus deleted) the fragment for DED1117-604 was

441 amplified with the primers zfDD14 and zfDD15 (Supplementary file 1B), using the plasmid

442 pET-22b(+)-DED1 as PCR template. The PCR product was gel purified, digested with XhoI and

443 SacI, and ligated into the pET-22b(+)-His6-thrombin-SUMO plasmid (gift from Dr. Derek Taylor,

444 Case Western Reserve University, Cleveland, OH) at the 3’-end of SUMO sequence. The

445 coding sequence in the resulting plasmid (pET-22b(+)-SUMO- DED1117-604) was verified by

446 sequencing. Subsequently, the plasmid was introduced into E.coli (DE3). Expressed His-

447 SUMO-Ded1p117-604 protein was purified through a Nickel column (PrepEaseHis-tagged protein

448 purification resin high specificity, USB), and the eluted protein was incubated with His-tagged

449 SUMO protease at 8ºC overnight in order to remove the His-SUMO-tag. The solution was briefly

450 incubated with Nickel resin to absorb the His-SUMO tag and the His-tagged SUMO protease.

451 Ded1p117-604 in the supernatant was further purified through a P11 phosphocellulose column

452 (Whatman). Protein was stored in 50 mM Tris-HCl (pH 8.0), 2 mM DTT, 1 mM EDTA, 0.1 %

453 (v/v) Triton-X 100, 30% (v/v) glycerol and 300 mM NaCl. Protein homogeneity and concentration

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Gao et al.

454 were determined by SDS-PAGE and Coomassie Blue staining, with diluted BSA (Roche) and

455 wild-type Ded1p in known concentrations as standards.

456

457 eIF4G protein

458 Expression and purification of eIF4G [(pET41a(+)-GST-S•Tag-eIF4G1-His) and (pET21b(+)-

459 eIF4E)] were previously described (Hilliker et al., 2011).

460

461 eIF4A and mutant eIF4A proteins

462 pET-28a(+) plasmid encoding an N-terminally His6-tagged wild-type yeast eIF4A (pET-28a(+)-

463 eIF4A) was a gift from Dr. Michael Altmann (Bern, Switzerland) (Schütz et al., 2008). To

464 generate plasmid pET-28a(+)-eIF4AE171A, two pairs of primers (zfDD16, zfDD17, zfDD18 and

465 zfDD19) were used to introduce the E171A mutation into plasmid pET-28a(+)-eIF4A by the

466 SLIM-PCR procedure according to (Chiu, et al., 2004, 2008). eIF4A and eIF4AE171A were

467 purified as described (Hilliker et al., 2011), and stored in 50 mM Tris-HCl (pH 8.0), 2 mM DTT,

468 1 mM EDTA, 0.1 % Triton-X 100, 30% glycerol and 200 mM NaCl.

469 To create the plasmid for the recombinant GST-eIF4A purification, the eIF4A coding

470 sequence was amplified from pET-28a(+)-eIF4A with the primers zfDD20 and zfDD21,

471 subsequently was digested with SacII and XhoI, and ligated into the pET-41a(+) plasmid to

472 generate the pET-41a(+)-eIF4A plasmid (Supplementary file 1C). GST-His6-eIF4A was

473 expressed in E. coli (DE3). The protein was purified through a Nickel column (USB), a

474 glutathione sepharose 4B column (GE health care) and a size-exclusion NAP-25 column

475 (BioRad). Purified protein was stored in 50 mMTris-HCl (pH 8.0), 2 mM DTT, 1 mM EDTA, 0.1

476 % Triton-X 100, 30% glycerol and 200 mMNaCl.

477

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478 RNA oligonucleotides

479 RNA oligonucleotides were purchased from DHARMACON. were radiolabeled and

480 duplex substrates were prepared and characterized as described (Yang and Jankowsky,

481 2005). For sequences see Supplementary file 1A.

482

483 Complementation of ded1-tam by eIF4A overexpression

484 Yeast strains are listed in Supplementary file 4. A high copy suppressor screen of cold

485 sensitive ded1-tam allele (Hilliker et al., 2011) was performed using a yeast genomic tiling

486 library of overexpression vectors (Jones et al., 2008; GE Healthcare #YSC5103). The putative

487 suppressors included DED1 or TIF2 within the 10-kb genomic inserts. Plasmids containing

488 either wild type DED1 (pRP1555) or the mutant ded1-tam (pRP048) were transformed into a

489 DED1 yeast shuffle strain containing a chromosomal deletion of DED1 and wild type copy of

490 DED1 on a URA3-marked plasmid (yRP2799; Hilliker et al., 2011). Transformants were grown

491 on selective media before counter-selection against the URA3-marked plasmid on 5-fluoroorotic

492 acid (5-FOA; Boeke et al., 1987). These strains, now containing the newly transformed copy of

493 ded1 as an exclusive copy, were transformed with either an empty vector (pGP564; GE

494 Healthcare #YSC5034) or a plasmid overexpressing either DED1, TIF1, or TIF2 (pAKH776,

495 757, 775, or 756) on a LEU2-marked vector. Transformants were grown on selective media with

496 2% dextrose. Cells were grown to mid-log phase in selective media with 2% glucose. The

497 cultures were pin replicated at identical concentrations onto YPDA media and incubated at 30 or

498 16°C. All of the strains grew like wild type at 30°C.

499 High copy plasmids containing either TIF1, TIF2, and DED1 ORFs and roughly 500

500 nucleotides up- and downstream of the ORF were made via recombination in yeast. TIF2, and

501 DED1 genes were amplified from the genomic tiling plasmids that suppressed the ded1 mutant

502 alleles (GE Healthcare #YSC5103). The TIF1 gene was amplified from genomic DNA of the

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Gao et al.

503 BY4741 S. cerevisiae strain. Primers (Supplementary file 1B) contained a 40 nt overhang

504 complementary to the ends of the insertion site in the vector backbone (pGP564). The vector

505 was linearized by digestion with BamHI and XmaI. Gel purified PCR product and linearized

506 vector were transformed into BY4741 and plated on media selective for the circularized vector.

507 Circularized plasmids were isolated from yeast via the Zymoprep Yeast Plasmid Miniprep II kit

508 (Zymo Research, #D2004) and transformed into DH5α competent E. coli (NEB, #C2987) to

509 amplify plasmids. Plasmid inserts were confirmed by sequencing the entire insert.

510

511 Growth measurements with Hippuristanol

512 For growth studies with hippuristanol, a plasmid with the ded1-95 allele (Ded1pT408I,

513 pEJ4, Supplementary file 1C) was created. Genomic DNA was amplified with primers X7 and

514 X8 from a yeast strain containing the WT copy of the HIS3 gene (yJC300, gift from Dr. Jeff

515 Coller, Cleveland, OH) and subsequently subcloned (Invitrogen, Carlsbad, CA). The ded1-95

516 allele was introduced into pEJ4 by site-directed mutagenesis with primers X11 and X12

517 generating pEJ6. pEJ4 and pEJ6 were linearized and used to transform BY4741 by standard

518 lithium chloride transformation yielding yeast strains yEJ1 and yEJ3, respectively. Presence of

519 the ded1-95 allele in the yeast strain was verified by amplifying genomic DNA and subsequent

520 restriction fragment length analysis as described above for pEJ13.

521 Hippuristanol was a gift from Dr. Jerry Pelletier (McGill University, Canada). WT and

0 522 ded1-95 yeast strains were grown in YPD at 30 C, diluted (V = 1.8 mL) to 0.1 OD600 and grown

0 523 for an additional 3 hours to 0.4 OD600. Cultures were shifted to 37 C, and grown for 45 min at

524 370C. Hippuristanol in DMSO was added to final concentrations of 1 µM, 5µM, 10 µM and

525 20µM. For control reactions, DMSO alone (0.2% v/v) was added. Cells were further grown for

° 526 45 min at 37 C. Growth was subsequently followed for 2 hours by measuring OD600. The growth

527 rate is reported, normalized to the growth rate of the corresponding strain without Hippuristanol.

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Gao et al.

528

529 Complementation with DED1117-604

530 The plasmid for complementation with DED1117-604 (N-terminus deleted, plasmid pEJ10) was

531 constructed from pRP1555 (HIS3/CEN) (Hilliker et al., 2011), using primers Ded116delFt/Rs

532 and Ded116delRt/Fs (Supplementary file 1B). The plasmid insert was confirmed by

533 sequencing the insert. The ded1-null strain yRP2799 (MATa ura3Δ0 leu2Δ0 lys2Δ0 his3Δ1

534 met15Δ0 ded1::KANMX pRP1560) was transformed with HIS3-marked wild type DED1

535 (pRP1555), or DED1117-604 (pEJ10). As an additional control we also transformed yRP2799 with

536 an empty HIS3-marked plasmid (pRS413). Transformants were streaked on media lacking

537 histidine and further screened on a 5-FOA containing plate. These strains were transformed

538 with either empty vector (pGP564; GE Healthcare #YSC5034) or a plasmid overexpressing TIF1

539 (pAKH775) on a LEU2-marked vector. Transformants were grown on selective media with 2%

540 dextrose. Cells were grown to mid-log phase in selective media with 2% glucose. The cultures

541 were pin replicated at identical concentrations onto YPDA media and incubated at 30 or 16°C.

542 At 37°C, no significant growth differences between wtDED1 and DED1117-604 were observed.

543

544 Pull-down Assays

545 In vitro pull‐down measurements were essentially performed as described (Putnam et al.,

546 2015). For the pull-down assays with immobilized eIF4G , 5 µL bed volume of DynaBeads®

547 Protein G (ThermoFisher Scientific # 10003D) was pre-equilibrated with 200 µL helicase

548 reaction buffer [40 mM Tris–HCl (pH 8.0), 0.5 mM MgCl2, 2 mM DTT,0.01% (v/v) IGEPAL CA-

549 630] complemented with 100 mM NaCl (HRB-Na100 buffer) at room temperature for 30 min.

550 The pre-equilibrated beads were then incubated with 4 µg anti-S•Tag monoclonal antibody

551 (Novagen, Cat. # 71549) and 420 µg BSA (Roche) in a 25 µL reaction at 8°C overnight. Protein

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Gao et al.

552 binding reactions (100 µL) included 300 nM S•Tag-eIF4G, 300 nM Ded1p, 1,500 nM eIF4A, 20

553 µg/mL RNases A,B (Roche), as indicated. 3 µL of the protein reaction volume was removed and

554 used as input. The remainder of the reaction volume was rotated at 8ºC overnight, and

555 subsequently mixed with the 25 µL equilibrated beads. After further incubation of one hour with

556 rotation, the beads were washed four times with RIPA buffer (50 mMTris, pH 7.5, 1% IGEPAL

557 CA-630, 0.25% sodium deoxycholate, 0.1% SDS, 200 mM NaCl, 1mM EDTA, 1mM PMSF).

558 Proteins were eluted with Laemmli buffer (Biorad), and denatured at 95°C for 3 min. Proteins

559 were resolved on the NuPAGE Novex 4-12% Bis-Tris protein gels (1.0 mm) in MOPS buffer

560 (pH7.7, Life Technology), and visualized by Western blot with primary antibodies against Ded1p

561 (α-Ded1p, polyclonal antibody, raised against full length Ded1p, dilution 1:6,000), monoclonal

562 anti- S•Tag antibody (Novagen, cat. # 71549), and anti-eIF4A polyclonal antibody (Santa Cruz,

563 prod. # sc-27227).

564 For the pull-down assays with immobilized Ded1p-HA, 1,200 nM Ded1p-HA was incubated

565 with 0.2 µg anti-HA monoclonal antibody (Roche, cat. # 11867423001, clone 3F10) and pre-

566 equilibrated DynaBeads® Protein G (Life Technologies) (5 µL bed volume) in a 100 µL reaction

567 at 8ºC for three hours. The beads were then washed three times with the HRB-Na100 buffer to

568 remove unbound Ded1p-HA protein, and subsequently mixed with 300 nM S•Tag-eIF4G, 1,500

569 nM eIF4A, 20 µg/mL RNases A,B (Roche), as indicated, in a volume of 100 µL. 3 µL of the

570 reaction volume (including beads) was removed and used as input. The remainder of the

571 reaction volume was incubated under rotation overnight at 8ºC. Beads were washed with the

572 HRB-Na100 buffer for three times. Proteins were eluted with Laemmli buffer (Biorad), and

573 denatured at 95°C for 3 min. Proteins were resolved on NuPAGENovex 4-12% Bis-Tris protein

574 gels (1.0 mm) in MOPS buffer (pH 7.7, Life Technology), and visualized by Western blot with

575 primary antibodies against Ded1p (α-Ded1p, polyclonal antibody, raised against full length

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Gao et al.

576 Ded1p, dilution 1:6,000), monoclonal anti-S-Tag antibody, and anti-eIF4A polyclonal antibody

577 (Santa Cruz, prod. # sc-27227).

578 For the pull-down assays with GST-eIF4A or GST immobilized, 300 µL of the protein-binding

579 reaction was set up with 1500 nM GST-eIF4A or GST, 1500 nM Ded1p117-604 or Ded1p1-535, 20

580 µg/mL RNases A,B (Roche), as indicated. 30 µL of the protein-binding reaction was removed as

581 input. The reminder was incubated with rotation overnight at 8ºC in presence of 5 µg/µL BSA

582 (Roche), and was further mixed and incubated with the pre-equilibrated 40 µL (bed volume)

583 glutathione sepharose 4B resin(GE healthcare) at 8ºC for one hour. The beads were washed

584 four times with the RIPA buffer. Proteins were eluted with Laemmli Sample Buffer (Biorad), and

585 denatured at 95°C for 3 min. Proteins were resolved on the NuPAGE®Novex® 4-12% Bis-Tris

586 mini protein gels (1.0mm thick) in MOPS running buffer (pH7.7) (Life Technology), and

587 visualized either by Western blot with primary antibodies against Ded1p (α-Ded1p, polyclonal

588 antibody, raised against full length Ded1p, dilution 1:6,000), or by Coomassie Blue staining for

589 the GST-tagged proteins.

590

591 RNA Duplex Unwinding

592 Unwinding reactions were performed under a pre‐steady‐state regime as previously described

593 (Yang and Jankowsky, 2005). Briefly, Ded1p was incubated with 0.5 nM radiolabeled RNA for

594 5 min in reaction buffer, and reactions were initiated with ATP/Mg2+. Where applicable, eIF4G,

595 eIF4A, or both were included. Aliquots were removed at indicated times, and reactions were

596 stopped and applied to 15% nondenaturing PAGE. Gels were dried and RNAs visualized and

597 quantified with a Molecular Dynamics Phosphorimager and the ImageQuant 5.2 software

598 (Molecular Dynamics). Observed rate constants were calculated as described, considering

599 simultaneously occurring strand annealing (Yang and Jankowsky, 2005).

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Gao et al.

600

601 Protein-protein crosslinking

602 In vitro protein‐protein crosslinking with formaldehyde was essentially performed as described

603 (Putnam et al., 2015),with Ded1p (0.3 µM), eIF4A (2 µM for Figure 3C, or indicated

604 concentrations in Figure 3-figure supplement 1B), RNA (2 µM, 16bp, 25 nt 3’-overhang) and

605 0.5 mM ADPNP-MgCl2 in buffer used in unwinding reactions. Formaldehyde [1% (v/v)] was

606 added, and incubated at room temperature for 30 minutes. Crosslinking was quenched with 0.5

607 mMTris-Glycine (pH 6.8). Proteins were applied to and resolved on the NuPAGENovex 4-12%

608 Bis-Tris protein gels (1.5 mm) in MOPS buffer (pH7.7, Life Technology). Proteins were

609 visualized by Western blot with polyclonal antibody against Ded1p.

610

611 Microscale Thermophoresis

612 EIF4A was labeled with Alexa Fluor 647 NHS ester (ThermoFisher Scientific # A37573)

613 according to the supplied protocol. Excess dye was removed by buffer exchange into 50 mM

614 Tris-HCl (pH 8.0), 2 mM DTT, 1 mM EDTA, 0.1 % Triton-X 100, 30% glycerol and 100 mM NaCl

615 using Zebaspin desalting columns (0.5mL, 7K MWCO, ThermoFisher Scientific # 89882). The

616 protein concentration was determined by SDS-PAGE and Coomassie Blue staining, with the

617 diluted BSA (Roche) and unlabeled eIF4A in known concentration as standards.

618 Microscale thermophoresis measurements were performed at room temperature on a

619 Monolith NT.115 system (NanoTemper Technologies) with standard treated glass capillaries

620 (NanoTemper Technologies). Buffers were identical to those used in unwinding reactions,

621 complemented with 0.5 µg/µL BSA (Roche) and 0.05% (v/v) Tween, to prevent absorption of the

622 proteins to the glass capillaries, and with 25 µg/mL RNase A (USB) to remove residual RNA.

623 20% IR-laser power was used to locally generate the temperature jump in the capillaries.

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Gao et al.

624 Fluorescence change in the heated field was monitored with 20% LED power. Laser on and off

625 times were set at 30 seconds and 5 seconds, respectively. The eIF4A-eIF4G complex was

626 formed for at least 10 minutes prior to the addition of Ded1p. Measurements were performed

627 multiple times, averages of individual points were calculated and the resulting binding isotherm

628 was fitted with the quadratic binding equation.

629

630 Thermodynamic model and data fit

631 Kinetic modeling was performed with KINETK EXPLORER (Kintek, Austin, TX) (Johnson et al.,

632 2009a; Johnson et al., 2009b) using data obtained in this and earlier studies (Putnam et al.,

633 2015). The thermodynamic framework to describe the interactions between Ded1p, eIF4A,

634 eIF4G, RNA, and ATP was built on the previously established kinetic framework for duplex

635 unwinding by the Ded1p oligomer (Putnam et al., 2015). eIF4A and eIF4G only interact with a

636 Ded1p monomer (Figure 3). The resulting framework contains 108 binding reactions, listed in

637 Supplementary file 2. The model was constrained by considering energy conservation. That

638 is, the change in free energy for transition of one complex into another is independent of the

639 reaction pathway. In addition, we incorporated the experimentally determined RNA affinity of

640 eIF4G (Putnam et al., 2015). We further considered that the comparably weak RNA

641 independent ATPase activity of Ded1p was not affected by eIF4G and eIF4A to a measurable

642 degree (data not shown). This notion allowed us to use the Ded1p affinity for ATP in the

643 absence of RNA for multiple Ded1p complexes. Collectively, these considerations enabled us to

644 describe the entire framework in 16 groups of thermodynamically linked binding steps

645 (Supplementary file 3).

646 Ten complexes are theoretically capable of unwinding: Ded1p, eIF4A, eIF4-eIF4G, Ded1p-

647 eIF4G, Ded1p-eIF4A (with ATP bound to Ded1p, eIF4A, or both), Ded1p-eIF4A-eIF4G (with

648 ATP bound to Ded1p, eIF4A, or both). Given that eIF4AE171A (ATPase deficient) was able to

29

Gao et al.

649 stimulate unwinding by Ded1p, while Ded1pE307A (ATPase deficient) did not stimulate unwinding

650 by eIF4A (Figure 2), we considered ATP binding to eIF4A irrelevant for the unwinding activity of

651 the Ded1p-eIF4A complex. In the presence of eIF4G, ATP binding by eIF4A was required for

652 the impact on Ded1p (Figure 2). We therefore considered the Ded1p-eIF4A-eIF4G complex

653 with ATP bound to both helicases as active unwinding complex. Collectively, these

654 considerations simplified the number of unwinding complexes to six: Ded1p, eIF4A, eIF4-eIF4G,

655 Ded1p-eIF4G, Ded1p-eIF4A (with ATP bound to Ded1p independent of ATP binding to eIF4A),

656 Ded1p-eIF4A-eIF4G (with ATP bound to Ded1p and eIF4A). We did not include ATP hydrolysis

657 steps in our analysis for any complex, except for Ded1p alone, for which we had previously

658 characterized the respective steps (Putnam et al., 2015).

659 Global data fitting was performed using Kintek Global Explorer. 20 datasets for unwinding of

660 the 16 bp duplex with 3’-25 ntssRNA overhang were fit simultaneously. A dataset includes all

661 time courses for titration of 1 component (e.g., protein or ATP) with other components held

662 constant. For each complex at least one dataset was included for a titration of each component

663 (e.g., Ded1-eIF4G: 1 Ded1p titration, 1 eIF4G titration, 1 ATP titration).Datasets were as follows:

664 Ded1p-eIF4A (4 datasets), Ded1p-eIF4G (3 datasets), eIF4A-eIF4G (4 data sets), and Ded1p-

665 eIF4A-eIF4G (9 datasets). Multiple iterations were performed until the best fit to all data sets

666 was achieved. Data were fit assuming that all binding steps for Ded1p with eIF4A, and eIF4G

667 were in rapid equilibrium. Parameters for the best fit values are reported in Supplementary file

668 2. Variables not well constrained by the data are reported as limits. Errors are not always

669 symmetrically distributed around the best fit value (Figure 4-figure supplement 5). Uncertainty

670 in each parameter is presented as a range calculated at the 95% confidence interval. To

671 visually assess the quality of fit, experimental data were plotted versus values predicted with the

672 model (Figure 4B).

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Gao et al.

673 ACKNOWLEDGEMENTS

674 We thank Dr. Jerry Pelletier (McGill Univ., Montreal) for Hippuristanol, Dr. Derek Taylor (Case

675 Western Reserve University, Cleveland) for SUMO plasmids, Dr. Michael Altmann (Univ. Bern,

676 Berne) for the plasmid containing wild-type His-tagged eIF4A, Dr. Jeff Coller (Case Western

677 Reserve University, Cleveland) for yeast strains, Dr. Yinghua Chen and the Protein Expression

678 Purification Crystallization and Molecular Biophysics Core (Case Western Reserve University,

679 Cleveland)for assistance with MST measurements, Sukanya Srinivasan (Case Western

680 Reserve University, Cleveland) for assistance with protein purification, and Drs. Michael Harris

681 and William Merrick (Case Western Reserve University, Cleveland) for helpful discussions.

682

683

684 CONFLICT OF INTEREST STATEMENT

685 The authors declare no conflicting interest.

31

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839 FIGURE CAPTIONS

840

841 Figure 1

842 Direct interactions between Ded1p, eIF4A and eIF4G.

843 (A) Effect of EIF4A (TIF1,TIF2) overexpression (o/e) on growth of the DED1-tam allele. Yeast

844 with either wild type DED1 (WT), or DED1-tam (tam) as sole copy of DED1 were transformed

845 with a high copy plasmid containing either no insert (none) or TIF1, TIF2, or DED1. Serial

846 dilutions of each strain were spotted at identical concentrations on selective media and grown at

847 16°C.

848 (B) Impact of increasing concentrations of the eIF4A inhibitor hippuristanol on growth of yeast

849 with either wild type DED1 (WT), or the temperature sensitive ded1-95 (Ded1pT408I, Figure 1-

850 figure supplement 1) allele as the sole copy. Growth rates were measured at 37°C and

851 normalized to the growth rate without inhibitor. Error bars represent one standard deviation of

852 three independent measurements.

853 (C) Pull-down of purified eIF4A, eIF4G, or both, with immobilized HA-tagged Ded1p. Reactions

854 were performed in the presence of RNases. EIF4G contained an S-tag. Input (IN) lanes show 3%

855 of total reaction volume. Pull-down (PD) lanes show entire sample. Relative band intensities

856 (pull-down compared to input): reaction 1, Ded1p: 460% ± 18%, eIF4G: 31% ± 12%; reaction 2:

857 Ded1p: 413% ± 58%, eIF4A: 96% ± 55%; reaction 3, Ded1p: 592% ± 113%, eIF4G: 74% ± 9%,

858 eIF4A: 25% ± 21%. Errors represent one standard deviation of multiple independent

859 experiments.

860 (D) Pull-down of purified eIF4A, Ded1p, or both, with immobilized, S-tagged eIF4G. Reactions

861 were performed in the presence of RNases. Input (IN) lanes show 3% of total reaction volume.

862 Pull-down (PD) lanes show entire sample. Relative band intensities (pull-down compared to

863 input): reaction 5, eIF4G: 440% ± 113%, Ded1p: 14% ± 7%; reaction 6: eIF4G: 280% ± 29%,

39

Gao et al.

864 eIF4A: 3% ± 2%; reaction 7, eIF4G: 473% ± 27%, Ded1p: 33% ± 11%, eIF4A: 15% ± 5%. Errors

865 represent one standard deviation of multiple independent experiments.

866 (E) Unwinding activity of Ded1p, eIF4A, with and without eIF4G, and in combination.

867 Representative unwinding reaction with 0.5 nM RNA duplex (16 bp, 25 nt 3’-overhang, for

868 sequences see Supplementary file 1A), 0.1 µM Ded1p, 0.1 µM eIF4G, 2 µM eIF4A, 4 mM ATP

869 (0.2 % v/v DMSO). Lines represent the best fit to the integrated first order rate law.

870

871 See also Figure 1-figure supplement 1 and Supplementary file 1A.

872

873

874 Figure 1-figure supplement 1

T408I 875 Ded1p is deficient in RNA binding.

T408I ATP (A) ATP affinity of Ded1p and WT Ded1p. Apparent ATP affinities (K ) of WT Ded1p and 876 1/2

T408I 877 Ded1p for ATP at 30°C and 37°C were measured through RNA-stimulated ATPase activity

878 of the proteins with the substrate containing a 16 bp duplex and 25 nt unpaired 3' overhang

ATP (Putnam and Jankowsky, 2013). Values for K were calculated by fitting ATP titrations to 879 1/2

880 the MichaelisMenten model (Putnam and Jankowsky, 2013). kcat for ATP did not notably differ

T408I 881 between Ded1p and WT Ded1p (data not shown).

T408I RNA (B) RNA affinity for Ded1p andWT Ded1p. Apparent RNA affinities (K ) of WT Ded1p 882 1/2

T408I 883 and Ded1p for RNA at 30°C and 37°C were measured through RNA-stimulated ATPase

RNA activity of the proteins as in panel A. Values for K were calculated by fitting RNA titrations 884 1/2

885 to the Michaelis Menten model (Putnam and Jankowsky, 2013). The data indicate an RNA

T408I 886 binding defect in Ded1p .

887

40

Gao et al.

888 Figure 2

889 Ded1p is the unwinding module in complexes with eIF4A and eIF4G.

890 (A) Impact of hippuristanol on unwinding activity of Ded1p, eIF4A, with and without eIF4G, and

891 in combination. Reactions were performed as in Figure 1E with 0.2% (v/v) DMSO and 20 μM

Hippuristanol, as indicated. Left panel: Observed unwinding rate constants (k ). For 892 unw

893 representative unwinding reactions see Figure 2-figure supplement 1. Error bars represent

894 one standard deviation of at least three independent measurements. Right panel: decrease or

increase of k by hippuristanol. 895 unw

E171A 896 (B) Impact of eIF4A (100 nM) on unwinding activity of Ded1p (100 nM) with or without

897 eIF4G (100 nM), measured as in Figure 1E, but without DMSO. Left panel: Observed

unwinding rate constants (k ). Error bars represent one standard deviation of at least three 898 unw

independent measurements. Right panel: increase of k , compared to reaction without 899 unw

E171A 900 eIF4A .

E307A 901 (C) Impact of Ded1p on unwinding activity of eIF4A with or without eIF4G, measured as in

Figure 2B. Left panel: Observed unwinding rate constants (k ). Error bars represent one 902 unw

standard deviation of at least three independent measurements. Right panel: increase of k , 903 unw

E307A 904 compared to reaction without Ded1p .

T408I 905 (D) Impact of eIF4A on unwinding activity of Ded1p with or without eIF4G, measured as in

Figure 2B. Left panel: Observed unwinding rate constants (k ). Error bars represent one 906 unw

standard deviation of at least three independent measurements. Right panel: increase of k , 907 unw

908 compared to reaction without eIF4A.

909

910 See also Figure 2-figure supplement 1

911

41

Gao et al.

912

913 Figure 2-figure supplement 1

914 Reaction progress curves for Figure 2A.

915 Representative unwinding reactions for Figure 2A, with (A) Ded1p, (B) Ded1p and eIF4A, (C)

916 Ded1p, eIF4A, and eIF4G, (D) Ded1p and eIF4G, (E) eIF4A, (F) eIF4A and eIF4G. In each

917 panel, open shapes represent reactions without hippuristanol; filled shapes represent reactions

918 with hippuristanol. Lines represent the best fit to the integrated first order rate law.

919

920

921 Figure 3

922 The N‐terminus of Ded1p is critical for the interaction with eIF4A.

1-535 923 (A) Impact of eIF4A on unwinding activity of Ded1p (C‐terminus deleted, upper panels) and

117-604 924 Ded1p (N‐terminus deleted, lower panels) with or without eIF4G, measured as in Figure

2B. Left panel: Observed unwinding rate constants (k ). Error bars represent one standard 925 unw

deviation of at least three independent measurements. Right panel: increase of k , compared 926 unw

927 to reactions with Ded1p alone.

117-604 928 (B) Effect of the deletion of the N‐terminus of Ded1p (Ded1p ), without or with EIF4A (TIF1)

929 overexpression (o/e), on growth in yeast at 30°C and 16°C.

930 (C) Formaldehyde crosslinking of Ded1p without and with eIF4A in the presence of RNA (16 bp,

931 25 nt 3’‐ overhang) and ADPNP. Mobilities of the Ded1p trimer, dimer, monomer, and the

932 Ded1p‐eIF4A complex are indicated. Proteins were visualized by western blot (α‐Ded1p).

933 (D) Schematic model for the basic functional architecture of Ded1p‐eIF4A and

934 Ded1p‐eIF4A‐eIF4G complexes. Ovals represent the helicase cores of Ded1p (red) and eIF4A

42

Gao et al.

935 (green). C‐ and N‐termini of Ded1p and eIF4G are marked. The dotted lines between the N-

936 termini in the Ded1p trimer indicate interactions between the N-termini that contribute to

937 oligomrization.

938

939 See also Figure 3-figure supplement 1 and Supplementary file 1A.

940

941

942 Figure 3-figure supplement 1

943 Direct interaction between eIF4A and the amino terminus of Ded1p.

117-604 1-535 944 (A) Pull-down of purifed Ded1p or Ded1p , with immobilized GST-eIF4A.

117-604 1-535 945 (1500 nM GST-eIF4A or GST, 1500 nM Ded1p or Ded1p , and 20 µg/mL RNases A at

946 8°C). Ded1p was probed with the α-Ded1p antibody. Deletion of the N-terminus eliminates the

947 interaction between Ded1p and eIF4A. Input (IN) lanes show 10% of total reaction volume. Pull-

948 down (PD) lanes show entire sample. The relative band intensities (pull-down compared to input)

949 for the reaction with GST-eIF4A and Ded1p1-535: GST-eIF4A: 160% ± 17%, Ded1p1-535: 3% ± 1%.

950 Errors represent one standard deviation of multiple independent experiments. No signal for

951 Ded1p117-604 was detected in the pull-down.

952 (B) Formaldehyde crosslinking of Ded1p, with increasing concentrations of eIF4A, in the

953 presence of RNA (16 bp, 25 nt 3’‐ overhang) and ADPNP. Mobilities of the Ded1p trimer, dimer,

954 monomer, and the Ded1p‐eIF4A complex are indicated. Proteins were visualized by western

955 blot (α‐Ded1p). Increasing concentrations of eIF4A diminish the Ded1p trimer and dimer species.

956 (C) Formaldehyde crosslinking of Ded1p1-535 without and with eIF4A in the presence of RNA

957 (16bp, 25 nt 3’-overhang) and ADPNP. This experiment was performed to directly verify the

958 weak interaction between Ded1p and eIF4A detected by pull-down in panel (A). Deletion of C-

959 terminus of Ded1p diminishes formation of the Ded1p trimer (Putnam et al., 2015). Mobilities of

43

Gao et al.

960 the Ded1p dimer, monomer, and the Ded1p-eIF4A complex are indicated. Ded1p was visualized

961 by western blot (α-Ded1p).

962

963

964 Figure 4

965 Thermodynamic framework for the interactions between Ded1p, eIF4A and eIF4G.

966 (A) Graphic representation of the framework. Ovals represent the complexes containing Ded1p

967 (D), eIF4A (A), eIF4G (G), RNA (R), ATP (T). D3 indicates the Ded1p timer (Putnam et al.,

968 2015). Black lines mark a transition from one complex to another through binding of one of the

components. Colored squares indicate the calculated equilibrium dissociation constant (K ) for 969 1/2

970 the transition, as shown in the legend at the lower right. For visual reasons, the framework does

971 not depict specific states for ATP-bound eIF4A. Equilibrium constants for all individual

972 transitions are listed in Supplementary file 2.

973 (B) Observed apparent unwinding rate constants versus those calculated with the model in

974 panel (A). Measured and calculated rate constants from different reaction conditions are listed

975 without reference to the specific reaction conditions, solely to visualize the overall agreement

976 between observed and calculated values. For fitting parameters see Figure 4-figure

977 supplement 5 and Supplementary file 2. The black line represents a diagonal, R2 is the

978 correlation coefficient for a linear fit of the shown data to this line. Error bars mark the 95%

979 confidence interval for the observed values.

980

981 See also Figure 4-figure supplements 1-6 and Supplementary files 2,3.

44

Gao et al.

982 Figure 4-figure supplement 1

983 Impact of the Ded1p concentration on the modulation of its unwinding activity by eIF4A

984 and eIF4G.

985 All unwinding reactions were performed as in Figure 2B at the indicated Ded1p, eIF4A and

eIF4G, and ATP concentrations. Apparent rate constants (k ) represent the mean of at least 986 unw

987 three independent measurements. Error bars indicate one standard deviation.

988 (A‐C) Upper panels: Impact of eIF4A (A), eIF4A and eIF4G (B) and eIF4G alone (C) at

989 increasing Ded1p concentration at 4 mM ATP. Lines represent the best fit to a binding isotherm.

Note the different scale of the y‐axis in (C). Lower panels: Fold increase or decrease of k at 990 unw

991 each Ded1p concentration over the reaction with Ded1p alone.

992 (D) Hill coefficients calculated from Ded1p binding isotherms (A-C) in the presence of the

993 indicated combinations of eIF4G and eIF4A.

994

995

996 Figure 4-figure supplement 2

997 Impact of eIF4A concentration on the modulation of Ded1p unwinding activity by eIF4A

998 and eIF4G.

999 All unwinding reactions were performed as in Figure 2B at the indicated Ded1p, eIF4A and

eIF4G, and ATP concentrations. Apparent rate constants (k ) represent the mean of at least 1000 unw

1001 three independent measurements. Error bars indicate one standard deviation.

1002 (A‐C) Impact of increasing concentrations of eIF4A at fixed Ded1p concentration (A), and fixed

1003 Ded1p and two different eIF4G concentrations (B,C) at 4 mM ATP. Lines represent the best fit

1004 to a binding isotherm.

45

Gao et al.

1005 (D) Impact of increasing concentrations of eIF4A on unwinding in the absence and presence of

1006 eIF4G, without Ded1p. The corresponding curve in the presence of only Ded1p is shown as

1007 dotted line for reference.

1008

1009

1010 Figure 4-figure supplement 3

1011 Impact of eIF4G concentration on the modulation of Ded1p unwinding activity by eIF4A

1012 and eIF4G.

1013 All unwinding reactions were performed as in Figure 2B at the indicated Ded1p, eIF4A and

eIF4G, and ATP concentrations. Apparent rate constants (k ) represent the mean of at least 1014 unw

1015 three independent measurements. Error bars indicate one standard deviation.

1016 (A‐C) Impact of increasing concentrations of eIF4G at fixed Ded1p concentration at 4 mM ATP,

1017 and increasing concentrations of eIF4A, as indicated. Lines represent a trend, dashed lines

1018 mark the maximal observed unwinding rate constant.

1019 (D) Impact of increasing concentrations of eIF4G on Ded1p (100 nM, no eIF4A) activity in the

1020 presence of 4 mM ATP. Note the scale of y and x-axis.

1021

1022

1023 Figure 4-figure supplement 4

1024 Impact of ATP concentration on the modulation of Ded1p unwinding activity by eIF4A

1025 and eIF4G.

1026 All unwinding reactions were performed as in Figure 2B at the indicated Ded1p, eIF4A and

eIF4G, and ATP concentrations. Apparent rate constants (k ) represent the mean of at least 1027 unw

1028 three independent measurements. Error bars indicate one standard deviation.

46

Gao et al.

1029 (A‐C) Upper panels: Impact of ATP on reactions with fixed concentrations of Ded1p and eIF4A

1030 (A), Ded1p, eIF4A, and eIF4G (B), and Ded1p and eIF4G (C). Lines represent the best fit to a

1031 binding isotherm. Note the different scale of the y‐axis in (C). Lower panels: Fold increase or

decrease of k by eIF4A, eIF4G, or both, over the reaction with Ded1p alone. 1032 unw

1033 (D) Upper panels: Impact of ATP on the unwinding reaction with Ded1p and the ATP-binding

E171A 1034 deficient eIF4A (black solid line, open diamonds). The reactions with Ded1p and WT eIF4A

1035 (dotted line, filled diamonds) (A) and with Ded1p alone (dotted line, no symbols) (A) are shown

E171A as reference. Lower panels: Fold increase or decrease of k by WT eIF4A, or eIF4A , over 1036 unw

1037 the reaction with Ded1p alone. (E) Upper panels: Impact of ATP on the unwinding reaction with

E171A 1038 Ded1p, eIF4G and the ATP-binding deficient eIF4A (black line, open squares). The

1039 reactions with Ded1p, eIF4G and WT eIF4A (dotted line, filled squares) (B) and with Ded1p

1040 alone (dotted line, no symbols) (B) are shown as reference. Lower panels: Fold increase or

E171A decrease of k by eIF4G with WT eIF4A or eIF4A , over the reaction with Ded1p alone. 1041 unw

1042 (E) Upper panels: Impact of ATP on the unwinding reaction with Ded1p, eIF4G and the ATP-

E171A 1043 binding deficient eIF4A (black line, open squares). The reactions with Ded1p, eIF4G and

1044 WT eIF4A (dotted line, filled squares) (B) and with Ded1p alone (dotted line, no symbols) (B)

are shown as reference. Lower panels: Fold increase or decrease of k by eIF4G with WT 1045 unw

E171A 1046 eIF4A or eIF4A , over the reaction with Ded1p alone.

1047

1048

1049 Figure 4-figure supplement 5

1050 Relative Chi square values (Χ2) for variations of two representative parameters.

1051 Left panel: Ded1p binding to pre-formed eIF4A-eIF4G complex; right panel: ATP binding to

1052 Ded1p-eIF4G-eIF4A-RNA complex) . The two examples were chosen to illustrate a case where

47

Gao et al.

1053 both, increase and decrease in the parameter (K1/2) relative to the optimal value results in a

1054 poorer fit (left panel), and for a case where only a decrease of the parameter, but not an

1055 increase result in a poorer fit (right fit). Cases for the latter scenario are restricted to ATP

1056 binding and marked in the Supplementary file 2 with an ">" sign. Relative Χ2 represent the Χ2

1057 obtained for the entire thermodynamic model for the parameter on the X axis divided by the

1058 smallest (optimal) Χ2. For the optimal parameter, the relative Χ2 = 1. Dotted lines mark the 95%

1059 confidence interval. This interval is given for each parameter in the Supplementary file 2.

1060 Values for Χ2 represent the quality of the fit for the varied parameter to the entire

1061 thermodynamic model (Figure 4A).

1062

1063

1064 Figure 4-figure supplement 6

1065 The thermodynamic model adequately describes observed data for each subset of

1066 complexes.

Correlation between observed and calculated unwinding rate constants (k ) for subsets of the 1067 unw

2 1068 complexes, as indicated. R is the correlation coefficient of a linear fit of the data in each panel

1069 to a diagonal (black line). Error bars mark the 95% confidence interval for the calculated data.

1070 For fitting parameters see Supplementary file 2.

1071

1072

1073

1074

48

Gao et al.

1075 Figure 5

1076 Functional parameters of complexes with Ded1p, eIF4A, or both.

1077 (A) Free energies ΔG° for complexes formed between Ded1p, eIF4A, eIF4G, RNA (25 nt 3‘-

1078 overhang, 16 bp duplex) and ATP in the combinations shown, calculated with the model in

1079 Figure 4A.

1080 (B) MST measurement of Ded1p binding to eIF4A-eIF4G (30 nM eIF4G, 36 nM Cy5-labeled

1081 eIF4A, increasing concentrations of Ded1p as indicated, 25 μg/mL RNase A, 23°C). Datapoints

1082 show the change in fluorescence signal at the indicated Ded1p concentrations, normalized to

1083 the signal without Ded1p. Error bars indicate one standard deviation of multiple independent

1084 measurements. Datapoints were fitted with the quadratic form of the binding isotherm (K'1/2 < 6.6

1085 nM).

(max) (C) Unwinding rate constants (k , ATP and protein saturation, RNA: 25 nt 3' overhang, 16 1086 unw

(RNA) bp duplex) and RNA affinity (K , ATP saturation) for complexes formed between Ded1p, 1087 1/2

1088 eIF4A, eIF4G, and, for comparison, for Ded1p and eIF4A, calculated with the model in Figure

1089 4A.

1090 (D) Unwinding rate constants (RNA: 25 nt 3' overhang, 16 bp duplex) for the Ded1p timer, the

1091 Ded1p‐eIF4A, and the Ded1p‐eIF4A‐eIF4G complex as function of the Ded1p concentration

1092 (ATP saturation, eIF4 A = 2000 nM, eIF4G = 100 nM), calculated with the model in Figure 4A.

1093

1094 See also Figure 5-figure supplement 1.

1095

1096

1097 Figure 5-figure supplement 1

1098 ATPase activity of complexes formed between Ded1p, eIF4A, and eIF4G at RNA and ATP

1099 saturation.

49

Gao et al.

1100 ATPase reactions were performed with Ded1p (100nM), eIF4A (2000 nM), eIF4G (100 nM), as

1101 indicated, and with RNA (16bp, 25nt 3’-overhang, 40 µM) and ATP (4 mM). Initial rates for the

1102 ATPase reactions (V0) under these conditions represent ATP turnover numbers (equivalent to

1103 kcat). Values were measured as described (Putnam and Jankowsky, 2013).

1104

1105

1106 Figure 6

1107 Impact of the substrate architecture on the functional parameters of complexes with 1108 Ded1p, eIF4A, and eIF4G

1109 (A) Impact of eIF4A, eIF4G, or both, on the unwinding activity of Ded1p with 5' and 3' tailed

1110 substrates (16 bp, 25 nt 3’- or 5’-tail), and blunt-end, shown schematically at the left (numbers

1111 indicate nucleotides in unpaired overhang and basepairs in duplex region). Reactions were

performed as in Figure 2B. Sliding point graphs show observed unwinding rate constants (k , 1112 unw

1113 average of at least three independent measurements), error bars mark one standard deviation.

Bar graphs mark increase or decrease of k , compared to the reaction with only Ded1p for 1114 unw

1115 each substrate.

(B) Upper panel: Affinities (K ) for RNA substrates with 10 nt and 25 nt unpaired regions 3' to 1116 1/2

1117 the duplex (16 bp) for Ded1p, eIF4A, eIF4G alone and in combination as indicated, calculated

1118 with the model shown in Figure 4A, and with data obtained with two substrates containing

1119 either 10 or 25 nt overhangs. For modeling parameters see Figure 6-figure supplements 2-3,

Supplementary file 2 and Materials and Methods. Lower panel: Fold change in K between 1120 1/2

1121 the substrates with 10 and 25 nt unpaired regions.

1122 (C) Upper panel: Apparent unwinding rate constants (kunw, ATP = 4 mM, eIF4A = 100 nM, eIF4G

1123 = 100 nM) for Ded1p alone and for the Ded1p‐eIF4A‐eIF4G complex on RNA substrates with 10

1124 or 25 nt overhangs, 3' to a 16 bp duplex, as function of increasing Ded1p concentration,

1125 calculated with the model shown in Figure 4A, and with data obtained with two substrates

50

Gao et al.

containing either 10 or 25 nt overhangs. Lower panel: Fold change in k for reactions with 1126 unw

1127 Ded1p‐eIF4A‐eIF4G, compared to reactions with Ded1p alone for both substrates.

1128 (D) Unwinding rate constants at ATP and protein saturation for RNA substrates with 25 nt 3'

1129 overhangs and 13, 16, and 19 bp duplexes, for Ded1p, the Ded1p‐eIF4A complex and the

1130 Ded1p‐eIF4A‐eIF4G complex, calculated with the model shown in Figure 4.

1131

1132 For modeling parameters see Figure 4-figure supplements 5,6; Figure 6-figure supplement

1133 2, Supplementary files 2,3 and Methods.

1134

1135 See also Figure 6-figure supplements 1,3

1136

1137

1138 Figure 6-figure supplement 1

1139 Stimulation of unwinding activity of eIF4A by eIF4G with an RNA with a 5' tail.

1140 Unwinding reactions were performed in buffer used for all other unwinding reactions at 26°C

1141 with 100 nM eIF4A, 300nM eIF4G, 3 mM ATP, 10 nM RNA (13 bp, 25 nt overhang, 5' to duplex)

1142 and 3 μM unlabeled top strand (13 nt), made from DNA. For sequences see Supplementary

1143 file 1A.

1144

1145

1146 Figure 6-figure supplement 2

1147 Substrate architecture affects the modulation of Ded1p activity by eIF4A and eIF4G.

1148 (A‐I) Impact of eIF4A, eIF4G, or both on the unwinding activity of Ded1p with different

1149 substrates, shown schematically at the left (numbers indicate nucleotides in unpaired overhang

1150 and basepairs in duplex region). Reactions were performed as in Figure 2B. Sliding point

51

Gao et al.

graphs show observed unwinding rate constants (k , average of at least three independent 1151 unw

1152 measurements), error bars mark one standard deviation. Bar graphs show increase or decrease

of k , compared to the reaction with only Ded1p for each substrate. 1153 unw

1154

1155

1156 Figure 6-figure supplement 3

Correlation between observed and calculated unwinding rate constants (k ) for the 16 1157 unw

1158 bp substrate with 10 nt 3' tail.

2 1159 R is the correlation coefficient for the linear fit of the data to a diagonal (black line). Error bars

1160 mark the 95% confidence interval for the calculated data.

1161

1162

1163 Figure 7.

1164 Calculated prevalence of complexes formed between Ded1p, eIF4A and eIF4G at

1165 physiological protein concentrations. Fraction of Ded1p (left) and eIF4G (right) present in the

1166 various complexes with eIF4A, eIF4G, or both, at three different Ded1p and eIF4G

1167 concentrations around their reported physiological concentrations of ~ 1 μM (RNA = 6 μM, ATP

1168 = 2.5 mM). Relative abundance of the complexes were calculated with the binding parameters

1169 obtained from the thermodynamic framework (Figure 4A, Supplementary file 2).

1170

1171 See also Figure 4 and Supplementary file 2.

52