arXiv:1307.2008v1 [cond-mat.mes-hall] 8 Jul 2013 etdbn tutr:teΓ the Γ the above structure: band verted structure. in topological its prove and Bulk spectra, strained nature ARPES of the the analyze states we from surface letter, come this of to In always ARPES. seem energy low states surface evidences topological cleanest surface the the for However, of materials. properties these physical of states the of number a vealed sur- re- have as spectroscopy[13], such far-infrared orbital magnetometry[12], tools, magnetotransport[6], experimental studies[11], other STM-AFM materi- of face real number A as insulators als. topological Bismuth-Antimony[1– established have firmly on Land- Bismuth-Selenide[6–10] 5], choice. Bismuth-Telluride[4, experiments of 3], tool ARPES a Spec- mark as PhotoEmission together. appeared probes Resolved (ARPES) bound Angle poor troscopy states, be are to surface proved spin of ori- experiments and transport spin-orbit momentum While remark- their pairs. where display reflecting in gin states textures, appear Dirac magnetic only 2D able surface to can these opposed states as Moreover, Dirac particles, odd topo- where Dirac an dimensional of systems in three species consist the of states of number surface unconventional case these the the insulators, pre- order of logical In whose signature topological states, unique order. this a surface bulk of is robust spin- nature hallmark of strong cise the appearance a the of by is One induced order orbit. topological a sessing hnMruyTluie hssrisoesasalgap small a larger opens 0.3% strains is This Tel- constant epitax- Telluride. Cadmium Mercury the lattice a than which in from Telluride achieved substrate, Mercury be luride of can growth the This ial to three-dimensional strain 20]. bi-axial a a material[19, into applying by or insulator well[18], topological quantum carriers the a two- confining a inside by into turned insulator be spin-Hall can dimensional semi-metal this 17], papers[16, ukMruyTluiei eimtlwt nin- an with semi-metal a is Telluride Mercury Bulk pos- matter of states new are Insulators Topological oooia ufc ttso tandMercury-Telluride strained of states surface Topological lve Crauste, Olivier 1 6 esrmns h iprino ufc ttsfr Dirac a form states Γ surface the of of dispersion The measurements. ASnmes 32.t 96.i 03.65.Vf 79.60.-i, 73.20.At, numbers: also all PACS has dispersion intensity linear electron a photo-emitted keeps the and of bands dichroism hole heavy the within ntttNel ....adUiesteJsp ore,B Fourier, Universit´e Joseph and N´eel, C.N.R.S. 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Laurent and 18 ietebto aflies half bottom the hile cm ol ee ,France 9, Cedex noble te France ette, rbdb ARPES by probed 4 8 − ai Carpentier, David 3 ih oe(Γ hole light eepeae nadto to addition in prepared were 8 1 a , LH HgTe 8 , HH n h Γ the and ) 5 8 6 = ≈ , adbut band HH a 150nm, CdTe . band. 46 A). ˚ = 8 2

−1 −1 a) b) c) ky (Å ) ky (Å ) −0.10 .0 0 .1−0.10 .0 0 .1 0.1 0.1 ) 1 eV − 0.0 0.0 (Å 08 . x 0 k

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−0.1 −0.1 − Γ 6 0.1 0.1 ) 1 eV − 0.0 0.0 (Å 24 . x 0 k

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−0.1 −0.1 − −0.10 .0 0 .1−0.10 .0 0 .1 −1 −1 ky (Å ) ky (Å )

FIG. 1: High resolution ARPES spectra for a maximally strained [100] HgTe/vacuum interface in the vicinity of the Γ-point measured at room temperature. a) Energy-momentum intensity spectrum after background substraction. b) The second derivative of the intensity data which band positions are less faithful enhances the contrast. c) Intensity spectrum at different energies. Raw data on the left and its second derivative on the right. The cone structure has a circular section up to ≈ 0.4 eV. un-doped reference samples, in order to raise the bulk gies shown on the panel c) are circular up to energies 0.4 chemical potential. eV below the Dirac point. From the experimental slope The samples surfaces were cleaned in a dedicated Ul- of the cone structure, the surface state band velocity is 5 1 tra High Vacuum preparation chamber by a low-energy found to be vF ≈ 5 × 10 m.s− . This value agrees with Ar-ion sputtering at grazing angles to remove the sur- the lowest order expansion for the energy close to the in-situ Dirac point in the Kane model (~v ≈ α P ), where the face oxide. The sharp dots observed in the LEED F √6 spectra showed that the surface was clean enough for the parameter α ≈ 0.9 for HgTe (the Kane parameters are ARPES experiments[15]. The samples were subsequently defined in the supplementary material). The same sam- transferred to the ARPES chamber in Ultra-High Vac- ple was also probed at different incident photon energies uum. The position of the Fermi level was determined hν. Varying the incident photon energy, shifts the bind- with a reference gold sample placed on the same sample ing energy of bulk bands according to their kz dispersion. holder. Here, the cone position is unaffected, emphasizing that We first present the high-resolution spectra in the this cone structure comes from a surface state with no kz vicinity of the Γ-point for an un-doped sample. On the dispersion (see supplementary material, Fig. 1S). This is panel a) of Fig. 1, the intensity of the ARPES spec- a powerful check which discriminates between 2D and 3D trum is shown for a incident photon energy hν = 20 eV. states. Surface state spectra were also collected over the We retrieve the surface projection of the two volume va- entire Brillouin zone. In the Γ-K direction, the surface lence bands Γ8,HH and Γ6 (deep blue) and, with more state spectrum becomes diffuse at energies of 0.8 eV be- intensity, a linear cone structure, which broadens as one low the Fermi level. On the other hand, in the Γ-X direc- moves away from its apex. The second derivative spec- tion, the surface state spectra remain linear all the way trum shown on panel b) enhances the contrast in the the the X point (Supplementary material Fig. 2S), where ARPES intensity. Within the experimental accuracy the its energy is 3.4 eV below the Dirac point, i.e. well below cone apex coincide with the top of the Γ8,HH band and the Γ6 band: in this direction, the surface state robust- lies 0.1 eV below the Fermi level. On the raw ARPES ness goes well beyond the usual topological protection ar- spectrum shown in panel a) the cone structure extends guments. The ARPES spectra of doped samples are quite in the gap with a decreasing intensity, as those states are similar to the one presented in Fig. 1, i.e. the electro- populated mostly through the room-temperature thermal chemical potential at the top surface appears to be little activation. The cone section for different binding ener- 3

18 3 affected at the doping level used (10 cm− -measured by an ex-situ SIMS analysis- which is equivalent to a surface 13 2 density of 10 cm− for a 100 nm thick slab). Previous theoretical studies[21, 22] of HgTe surface states do not account quantitatively with our experimen- tal findings in some of their salient features: weak hybri- dation between surface states and the Γ8,HH valence band at small k and a Dirac point which lies very close to the top of the Γ8,HH valence band. Considering the successes of the Kane model[23], for which all the parameters[24] are known for HgTe, we computed the surface and bulk states of 2D interfaces between a maximally strained HgTe slab and vacuum (resp. CdTe) within the 8 bands (Γ6, 1/2, Γ8, 3/2, 1/2 and Γ7, 1/2) Kane model. The in- terfaces± were± described± by interpolating± smoothly over a finite width w the Kane parameters between their val- ues in HgTe for 0 L. The corresponding Schr¨odinger equation is discretized only in the z direction and nu- merically solved, determining surfaces and bulk states at once. The results are carefully shown to be independent of the discretization constant a over the range of energy and momenta considered. The results are shown in Fig. 2 : the surface states, originating from the inversion be- 1 tween the two S = 2 bands Γ6 and Γ8,LH, are the only states present in the gap. For the Kane parameters used, the energy of the Dirac point is ǫD = −30 meV below the Γ8,LH and is similar for a CdTe/HgTe interface. At FIG. 2: Surface (black) and bulk bands (Γ8,LH orange, Γ8,HH 6 k = 0 (ǫD), the surface states do not couple to the Γ8,HH magenta, Γ red) dispersions in the vicinity of the Γ point computed with a discretized Kane model along the z axis for band, and are weakly affected by the Γ8,HH band at small a HgTe – vacuum interface interface one lattice constant wide k below ǫ . They disappear gradually for larger k, con- D (w). The black dots are the computed surface states energies. sistent with the observed broadening in the experiment. Their dispersion is linear with the same band velocity as in the experiment. As observed experimentally, half of the surface states dispersion and (ii) a significant dichro- the Dirac cone lies inside the Γ8,HH valence band while ism (up to 20%) is observed in the bulk Γ8,HH band. the other half continues in the stress gap. These results on strained HgTe differ from the circu- A hallmark of topological insulators is the helical spin lar dichroism ARPES data on Bi2Se3 compound [9, 10] structure of surface states induced by the strong spin- where a dominant signature of surface states was ob- orbit coupling. Such textures have been observed directly served. The relationship between the circular dichroism using spin-resolved ARPES.[2, 3, 25] A less direct way to and the spectral spin densities of low energy bands is probe this helical spin-texture is through the induced cir- complex and depends on the incident photon energies[26]. cular dichroism in ARPES.[9, 10]. Circular dichroism is Hence, a quantitative description of circular dichroism defined as the asymmetry between the ARPES intensity may involve processes with higher energy bands which for left (L) and right (R) circular polarization require ab-initio calculations for a proper treatment. On

IR(ǫ, k) − IL(ǫ, k) the other hand if we assume that such a relationship ex- C(ǫ, k)= . (1) ists, Wang et al. [9] have shown that the dependence of IR(ǫ, k)+ IL(ǫ, k) the ARPES polarization asymmetry on the band polar- It is plotted in Fig. 3 (the geometry is specified in the izations, hSxi and hSzi is inset) as a function of ky for kx = 0 and an incident light 2 beam at ≈ 45◦ with respect to the normal to the sample. C(ǫ,k,φ)= −a cos φhSz(ǫ, k)i +4ab sin φhSx(ǫ, k)i, (2) By symmetry, the circular dichroism must cancel in the ky = 0 plane as observed for incident photon energies for a circularly polarized light beam incident in the x-z Ekin > 15.9 eV. plane at an angle φ with respect to the normal to the The most salient features of the experimental data of sample. The matrix elements a and b depends on surface Fig. 3 are (i) the absence of dichroism from the surface symmetries of the material [9]. This formula is consis- states, signaled by the white lines (no dichroism) along tent with the experimental data of Fig.3 if the coefficient 4

Left useful comments on the ARPES analysis. This work was funded by the EU contract GEOMDISS and the ANR 0 45 -0.2 grant SemiTopo. z y x Γ -0.2 8ΗΗ

[1] D. Hsieh, D. Qian, L. Wray, Y. Xia, Y. S. Hor, R. J. -0.4 Cava, and M. Z. Hasan, Nature 452, 970 (2008). intensity intensity

C [2] D. Hsieh, Y. Xia, L. Wray, D. Qian, A. Pal, J. H. Dil, J. Osterwalder, F. Meier, G. Bihlmayer, C. L. Kane, 323 Binding energy (eV) Binding energy -0.6 et al., Science , 919 (2009). [3] D. Hsieh, L. Wray, D. Qian, Y. Xia, J. H. Dil, F. Meier, -0.2 L. Patthey, J. Osterwalder, G. Bihlmayer, Y. S. Hor, et al., New Journal of Physics 12, 125001 (2010). -0.8 -0.3 -0.2 -0.1 0 0.10.2 0.3 [4] Y. L. Chen, J. G. Analytis, J. H. Chu, Z. K. Liu, S. K. Mo, X. L. Qi, H. J. Zhang, D. H. Lu, X. Dai, Z. Fang, k y (ŀ) et al., Science 325, 178 (2009). [5] M. Hajlaoui, E. Papalazarou, J. Mauchain, G. Lantz, −1 FIG. 3: Circular dichroism measured at kx = 0A˚ . The N. Moisan, D. Boschetto, Z. Jiang, I. Miotkowski, Y. P. 12 largest contribution to the dichroism comes from the Γ8,HH Chen, A. Taleb-Ibrahimi, et al., Nano Letters , 3532 valence volume band. The surface states appear here as white (2012). lines (no dichroism). The inset shows an incident left polar- [6] J. G. Analytis, R. D. McDonald, S. C. Riggs, J.-H. Chu, ◦ 6 ized light beam at 45 with respect to the sample surface. G. S. Boebinger, and I. R. Fisher, Nature Physics , 960 (2010). [7] K. Kuroda, M. Arita, K. Miyamoto, M. Ye, J. Jiang, A. Kimura, E. E. Krasovskii, E. V. Chulkov, H. Iwasawa, b vanishes for the [100] HgTe surface. This explains the T. Okuda, et al., Physical Review Letters 105, 076802 weak circular dichroism contribution of the surface states, (2010). whose spin polarization normal to the surface hSz(ǫ, k)i [8] P. D. C. King, R. C. Hatch, M. Bianchi, R. Ovsyannikov, vanishes at low energy. An interpretation along these C. Lupulescu, G. Landolt, B. Slomski, J. H. Dil, D. Guan, 107 lines also relates the observed dichroism of the valence J. L. Mi, et al., Physical Review Letters , 096802 band Γ to its pseudo-spin polarization whose possi- (2011). 8,HH [9] Y. H. Wang, D. Hsieh, D. Pilon, L. Fu, D. R. Gardner, ble origins are well known[23]. The first common source 107 + Y. S. Lee, and N. Gedik, Physical Review Letters , is the Rashba effect [23, 27] : the Ar beam used in the 207602 (2011). surface cleaning leaves a partially charged HgTe surface [10] S. Park, J. Han, C. Kim, Y. Koh, C. Kim, H. Lee, [28], inducing a surface electric field F . In addition, the H. Choi, J. Han, K. Lee, N. Hur, et al., Physical Review Dresselhaus coupling present in centro-asymmetric crys- Letters 108, 046805 (2012). tals is here further enhanced by the strain deformation [11] T. Hanaguri, K. Igarashi, M. Kawamura, H. Takagi, and 82 at the surface[29]. With these asymmetric couplings, the T. Sasagawa, Physical Review B , 081305 (2010). [12] A. Taskin and Y. Ando, Physical Review B 80, 085303 two Γ8,HH spin-bands can acquire a sizable pseudospin (2009). polarization near the valence band maximum. This spin [13] M. Orlita, K. Masztalerz, C. Faugeras, M. Potem- structure has implications for the design of spintronic de- ski, E. G. Novik, C. Brune, H. Buhmann, and L. W. vices. In the stress gap, the only charge carriers are the Molenkamp, Physical Review B 83, 115307 (2011). helical surface states. On the other hand, for negative en- [14] http://www.sychrotron-soleil.fr/Cassiopee. ergies the coexistence between a partially spin-polarized [15] The surface roughness was measured with an AFM on the heavy-holes and helical surface states is less favorable for oxydized sample surface after this experiment and found to be of the order of ≈ 2 nm, i.e. ≈ three monolayers. applications. [16] B. A. Bernevig, T. L. Hughes, and S. C. Zhang, Science In summary, we have observed the surface states of 314, 1757 (2006). stressed Mercury Telluride, confirming its topological in- [17] L. Fu and C. Kane, Physical Review B 76, 045302 (2007). sulating nature. It has some quite unique features: the [18] M. Konig, S. Wiedmann, C. Brune, A. Roth, H. Buh- Dirac point sits at the top of the heavy hole band, some- mann, L. W. Molenkamp, X. L. Qi, and S. C. Zhang, 318 thing which was also noticed in transport experiment for Science , 766 (2007). [19] C. Brune, C. Liu, E. G. Novik, E. M. Hankiewicz, samples oriented in the [100][19] and the [211][20] direc- H. Buhmann, Y. L. Chen, X. L. Qi, Z. X. Shen, S. C. tion. Combined with the very low residual bulk conduc- Zhang, and L. W. Molenkamp, Physical Review Letters, tion in the stress gap, this is one of 106, 126803 (2011). the most interesting system for fundamental and applica- [20] C. Bouvier, X. Baudry, P. Ballet, T. Meunier, R. Kramer, tive studies. and L. P. L´evy, ArXiv p. 12.... (2012). The authors would like to thank H. Cercelier for his [21] X. Dai, T. Hughes, X.-L. Qi, Z. Fang, and S.-C. Zhang, 5

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