Combined Solid-State NMR and Molecular Dynamics Study of the Structure of Strontiuln-Aluminosilicate glasses

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Combined Solid-State NMR and Molecular Dynamics

Study of the Structure of Strontiuln-Aluminosilicate

glasses

Thibault Charpentier, Kirill Okhotnikov, Pierre Florian, Franck Fayon,

Alexey Navikov, Louis Hennet, Daniel Neuville

To cite this version:

Thibault Charpentier, Kirill Okhotnikov, Pierre Florian, Franck Fayon, Alexey Navikov, et al..

Com-bined Solid-State NMR and Molecular Dynamics Study of the Structure of Strontiuln-Aluminosilicate

glasses. 15th International Conference on the Physics of Non-Crystalline Solids, Jul 2018, St Malo,

France. �cea-02340733�

Combined Solid-State NMR and Molecular

Dynamics Study of the Structure of

Strontiuln-Aluminosilicate glasses

Thibault Charpenticr*l, Kirill Okhotnikm,l, Pi<'rre Florian

_{Franck Fayon}

_Alexey

Navikov

_{Louis Hennet}

_{and Daniel Neu,\'ille:}

l:-\BIBE. CE A, C:-\HS, Univer"ité Paris-Saday, CEA Saclay, France (LSDHl\l) CEA ~~ Fhul('c

2CNRS, CE.MHTl UPH:30ï!), Uniy, Orlôam;, France (CEl\ITHl) CNHS: UPH:3079 FblIlCl'

:~Institl1t dl' Physique du Globe de Paris (IPGP) UlliveI'sité dl' la HôlIuioll. Université Paris VII -Paris Diderot, 11"0 PARIS, 1:-\ SU , C:-\H S : Ul\1H ïl!)4 ~ IPGP, 1 rue .Jussieu, 752:38 Paris cedex 05

Ulliversité Paris Diderot. Bùt. Lamarck A case postale 7011, 75205 Paris CEDEX la, France

Abstract

Solid-statc NIIlll Ims finnly established itself as il method of choice for pl'Ovidillg key information D:Jr the elucidatioll of glass atomic-scale structure. Recently, 11 Il1C'thodolog,), bascd 011 the cOl1lbinatÎol1 of DFT-:-\:tvIH cnlenlatiollS with molecuÎêu- d)11mnics simulat.ions

has cmerged as a sigllificHllt stcp for the improveIllent of the detailed interpretation of ex-pcrimcntal N:dH spectra. Usillg this approach, Wl' have illvestigated the structure of

alumÎ-Ilosilicale Si02-AI20:3-SrO based glass compositions whidl are largel.\' 11l1explored systems. Glasses on the colllpellsation lille A120;3 = SrO. wcre stlldied wit.h 170. 29Si and 27AI solid statf' N:\U1 al high (11.7 T) and very-high (20.0 Tl magnt'tic lü'lds, together \Vith I1(,U-troll diffraction spectroscopy. ClassÎcal and ab-initio molecnlm dynamics (!\ID) simulations were perfonlled and combil1cd with ealclliatiolls of NlvIH parametel's wit.h th(~ DFT-GIPA\V rnethod. Computed N:\IH parametcrs wcre linked t.o local st.ructural featlll'cs to establish rclatiorLships between experimcntal NIliR spectra and t.he underlyillg topologieal disorder (in terms of chcmical and geollletrical disorder) . Nl-.IH fingerprint.s of debated unit.s s11eh as tricoordinatcd oxygcn atolllS Gould be predictecl with the aims t.o assess their existenee from expcrÎlllclltal data. In agreement with expt'riml'utal N.MR dat.a, AID sinmlations prediet that éùulllinilllll is prcdomimtlltly tet.rahedrally coordinated for aIl t.he st.uclied compositions \Vith a sumll fi'actioll of AlOi> nnits rallgillg n'Olll 2-5%. VariatiollS of the 29Si NI'dH spectra, and to il less extent of 27 Al spectra, could be quantitatively correlated to t.ht' Al/Si mixing. In parnllel, the AI/Si cOllncctivitîes were illvestigated llsing <lchanct'd NMH techniques euahlîng the l'l'solution of the 20Si NI\1H spectrum in tcrms of Qll(mAI) unÎts (i.e., Qll colluected to

III AI units). SÎnmlations of 170 N~lH cxperiIlleuts 1'ro111 our first.-pril1ciples mcthodology combinccl to 170-27AI correlation experimcllts allmvpcl extradions of AI-O-SL Al-O-AI and Si-O-Si peaks which were found to be strcmgly oyerlapping in experimelltal ID and 2D 170 l'lIAS NMR spcctra.

Keywords: Allllninosilicat.e. N\IH, I11D, DFT, Glass structure • Speaker