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Infrared Spectroscopv and Crystal Chemistry of The 55 The CanadinnMineralo gist Vol.32,pp. 55-68 (1994) INFRAREDSPECTROSCOPV AND CRYSTALCHEMISTRY OFTHE BERYL GROUP CARLO AITSICCHIO Centrodi Stadioper gli Equilibrt Sperimentaliin Minerali e Rocce,Consiglio Naziotmle delle Ricerche, P.leA. Moro 5, 00185Roma, Italy ODINO GRTIBESSI Dipartimentodi Scienzed.ellaTena. Universitddegli Srudidi Roma "ln Sapienza",P.le A. Moro 5, 00185Romn, Italy PIERREZECCHINI Iaboratoire de Cristallographieet ChimieMinlrale, Universitt de Franche Comtd,25030Besangon Cedex, France ABSTRACT The infrared spectraof 27 natural and two syntheticsamples of powderedberyl were measuredat room (25oC)and liquid nitrogen (-180"C) temper,rtures.Water moleculesoccur in two different orientations(type I and type il), for which absorption bandsare clearly visible a[ low temperatures.The ratio ofthe absorbancesdue to type-Il and type-I O-H stretchingmodes at 36A0n698 and 366013698cm-l show a positive correlation with Na content, and show that high concentradonof alkalis is responsiblefor the type-tr configuration.The presenceof hydroxyl gtoups,in a H2O (type II) - Na - (OH) configuration,is proposedfor alkalirich beryl on the basis of the 3658 cm-l absorbance.The absorptionfrequencies for different samples of beryl are correlatedwith structuraland compositionalparameters. Unsubstituted beryl, beryl with substitutionsin the octahedralsite, and beryl with substifutionsin the tetrahedralsite, are clearly discriminatedusing absorptionbands in the range 106G-1020cm-I. The relationshipshelp to reconcilecontroversies conceming the proper assignmentof absorptionfrequencies to structuraldetails. Keywords:beryl, crystal chemistry,infrared spectrum,HrO orientation. SotvruIarng Le spectreinfrarouge de vingt-sept 6chantillons natuels et de deux 6chantillons synth6tiquesde b6ry1ont 6td mesur6s i temt'rature ambiatrte(25'C) ainsi qu'i la temp€raturede l'azote liquide (-180"C). Les moldculesd'eau setrouvent dans une de deux orientationsdiff6rentes (dites de type I et de type tr); leurs bandesd'absorption sont renduestrds 6videntesdans les spectresobtenus h bassetemp6rature. Le rapport des absorptionsdues au mode d'6tirement de la liaison O-H de type I et de type II, 3600/3698et 366013698cm-I, montrentune corr6lationpositive avec la teneuren Na, et ddmontrentque la teneur6lev6een alcalins est responsablede la prdsencede mol6culesd'eau de fype II. Des groupesd'hydroxyle dans une configurationH2O (type II) - Na - (OH) seraientresponsables de l'absorption i 3658 cm-r dansle b6ryl enrichi en alcalins. Les frdquencesd'absorption dans les diff6rents6chantillons de b6ry1sont analys6esen fonction des paramdtresstructuraux et compositionnels.Nous pouvonsdistinguer facilement le b6ryl sans substitution,le b6ryl ayant une substitution impliquant le site l coordinenceocta6drique, et le b6ry1ayant une substitutionimpliquant le site b coordinencet6tra6drique, en utilisant les bandesd'absorption dans I'intervalle 1060-1020cm-l. lrs relationsque nous d6crivonscontribuent i 6claicir les aspects controvers6sde I'attribution desfr6quences d'absorption aux caractaresstructuraux. (Traduit par la R6daction) Mots-clls: b6ry1,chimie crislalline, spectreinfrarouge, orientation des mol6cules d'eau. INTR0DUc"iloN of the cla ratio, bond distances,and site occu- pancieson the position of vibration bands.This Substitutionsinvolving tetrahedrallyand octa- type of analysis can help to characterizemate' hedrally coordinatedcations and the presenceof rials commonly found in very small amounts. channelconstituents (e.g., H2O, Na, OH) influ- We also proposea solutionto discrepanciesin ence the infrared (IR) absorptionspectrum of the assignmentof the IR bandsto Be-O and ring beryl, In this paper, we explore the influence Si-O-Si bonds. Downloaded from http://pubs.geoscienceworld.org/canmin/article-pdf/32/1/55/3435639/55.pdf by guest on 28 September 2021 56 THE CANADIAN MINERALOGIST The availabilityof a largenumber of beryl samples TAALE .I. CHEMICALCOMPOSMON OF BERYLSAMPLES that coverthe fulI rangeof chemicalvariation recog- nized to date invited a systematicstudy by infrared- sio2 64.36 63.65 @.7E absorptionspectroscopy in order to characterizefully Al:o: t3.99 17.54 14.u t}te broadly variablecrystal chemistryof beryl. In a Cr2Oj 0.32 0.1I previous paper (Aurisicchio er al. 1988), FeO f.il 0.07 a.72 we re- MgO 2.68 evaluatedthe complexcrystal-chemistry of beryl on MnO *t the basis of new chemicaldata and X-ray refinements Tio2 0.22 of the structureof beryl samplesof BeO 13.03 11.37 13.11 diffLrentcompo- Li2o 0.05 o.97 0.04 sitionsand from different sources.Our evaluation CaO 0.23 showedthat the main substitutionsinvolve divalenr Na2O 2.03 1.60 1.64 (Fe2+, Kro o.z2 and trivalent ions Mn2+nMg2+, Fe3+, Cr3+), CVO 0.33 2.57 as well as Vs+ and Ti4+for Al in the octahedrally Rbzo 0.06 coordinatedsite and Li for Be in the tetrahedrally L.O.r 2.00 1.97 2.01 Total [email protected] t00.26 99.61 coordinated(7') site. Substitutionsgiving rise to chargeimbalance require the incorporationof alkali Nmben oliom on the basis of 18 atoms of orygen ions (Na) into the channelinthe2a position,between si 6.016 6.025 6.033 the stackedsix-membered Si rings, whereasCs, Rb, Al 1.541 1.957 t.628 andK enterthe 2Dposition, at the centerofeach ring. Cr A.O24 0.008 The HrO moleculesfit in the 2a re3+ o.oo9 0.006 0.008 sitesonly. The effects Fd+ o.o7i 0.048 of thesesubstitutions on the cell pafirmetersled to the Mg 0.373 : o:r definition of two solid-solutionsseries on the basis Mn 0.006 of the cla ratio: Ti 0.015 i) octahedrallysubstituted beryl, with Be 2.Y25 2.585 ^:^ cla valuesfrom 0.991to 0.996,with substitutionsin Li 0.019 0.369 0.015 the O site: Me3+Al_tor Rr*rnuoorMe2*I_rAl*,,and Ca 0.o23 (ii) Na 0.368 0.294 0.296. tetrahedrallysubstituted beryl, with c/a valuesin K_ 0.027 o:* therange from 0.999to 1.003,with substitutionsin the Cs 0.013 0.103 ?' site:Ry+"r.*",Li+fl-rBe-,. Rb 0.002 ctq 0.9927 0.9986 0.9938 The two seriesdepart, with oppositeslope, from oonormal" (1.e.,unsubstituted) beryl (c/a in the range 0.9974.998), Sampl€831 snd gt havebeen analyzedby lhe authorclollofllng tho which showsa composirionclose to the same lechniqu€8as d6orlb€d ln Aurlslcchloel al. (1988). Sando ideal stoichiometry,with a very low degreeof substi- @ wa8 analyzedby lhe wst-{hemloal method In $o Geoohemhlry tution in both sites(cl Figs.5 and 6 in Infit|J|€ ol the Alademla Slnie, Gulymg, Chlna. Deh: bdw llmll Aurisicchioer ot dstsc{on; # by ohtrge balm@; L.O.l.:16 on lgntdon. al. 1988). tn the frst series,a increasesfrom 9.22 ro 9.27 A, and the c parameterremains approximately constant.In contrast,in the secondseries, the para- metera remainsapproximately constant, but c increasesfrom 9.20 to 9,24 A. Two endmembers can TABLEA DESCHPnONANO L@AUTIES OF BEFYLSPECIIdENS be derived from the abovevariations awav from unsubstituted"normal" berylAlrBerSiuO,r. - zHrO: N'SAMPLE LOCALITY N'SAMPLE LOCALITV RlAlMe2+Be1Si6O1s.zH2O, Ill oCtahedrally I Dukblue CslsfemMioe 1? V$ypde S.Pi@ircanpo, substitutedberyl, and PigtIMq bl@ Tusny,Italy Tusny, Italy 18 Psle pift Mr. Bity regio4 [2] Rf Al2BerLiSi6O,r.zHrO,rerrahedrally subsrituted 2 Liglnbl@ Calefemmine, MadagM beryl, Pi(rMt4 19 Ligbtblue M@c@tu, T|r@y, Iraly @ of 20 Sdiru Mne, whereRt+ = Na, Cs,Rb, K, in the sequenceof decreas- 3 DIL blue South Mom Cmdonq B@il aned Pi€dnort, ltaly 20 Pale pilk ltrsw G@iC ing averageabundances, as proposed by Bakakjnet al. 4 Dsrkg@ Mingon" SMValey, rinof t9 SalinoMne, (1970). aed Pakise B@il 5 Ligh g@ Val Vig@, Pi€dfron! 22 Hr*, Nuitu r€gio4 Italy lvlni lvtle, A&t!i 6 BIue Mohaveco.,Arizo!4 23 G|@ Habaclml E>csRn/GNTAL lon7rs Smithenid ,511ib69; Aeiis Indimio! 24 Ct@ l[onu4 Aebdia 7 Pink-rcd aned Wai W8h Momie 26 Lieln gr@ Urslr Mou.daiB IR spectraof two syntheticand 2l natural samples @rc B@vd Co. U&l Rlsia 8 Piok-red aned W8h Wah Mouuainc 27 Piok Mujee lfee of beryl from differentsources, chemically character- rin Bavq Co., Ub[ Z€nb€is izedby Aurisicchio (1988), 10 Ddkgr@ Muo,Colombia 28 P8lepink PalaNdng et at. are the subjectof ll Palegr@ Jos,Nigqis Califomir this investigation.Beryl samples#31, #32 and #33 12 Blue K6oi, Zinbabw 3l Dak g|a . Sada T@ifir, 13 Ligh blue MNink4 Bnzil arenerr acquisitionssince the 1988paper appeared. Urals Mmils, R!$ia 32 Whib ltukotohai The first (#31) 15 Verypde Cecrig@hi, piikilh ,(egia! c1li!8 is an emeraldfrom the St. Teresifla bl@ Vsldosla, 33 Dukg@ q€belzabatb,. mine, Brazil; #32 is a beryl transitionalfrom oonormal', Piednplt,ttaly EgDl 16 Ye[@ Fonvictorianel4 St Colorls S]dhaic to the tetrahedrallysubstituted variety from the ?lnbabve 52 Darkgrd Synhdio Downloaded from http://pubs.geoscienceworld.org/canmin/article-pdf/32/1/55/3435639/55.pdf by guest on 28 September 2021 CRYSTAL CHEIVtrSTRYOF THE BERYL GROTJP 57 Koktokay pegmatite,Xinjiang, China,and #33 is an The spectracollected at the temperatureof liquid emeraldfrom Djebel Zabarah,Egypt (Grubessiet al. nitrogenshowed the best resolutionof specific absorp- 1990).Anal''tical dataare given in Table 1. Table2 is tion bands,permitting better insight into the spectra. a list of all the samples,with details of color and The actual IR spectracan be obtained from the provenance.For the chemical composition,structural authors.Correlations with structuralparameters are parametersand mineral associationsof the samples basedon a smaller number of points becauseonly other than the three new ones, the reader is referred 15 samplesof beryl were analyzedby single-crystal to Tables3 and4 in Aurisicchio et al. (1988). X-ray diffraction. Infrared-absorptionspectra were
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