Searching for correlations between vibrational spectral features and structural parameters of silicate glass network
Abstract
Infrared (IR) and Raman spectroscopic features of silicate glasses are usually interpreted based on the analogy with those of smaller molecules, molecular clusters, or crystalline counterparts; this study tests the accuracy and validity of these widely cited peak assignment schemes by comparing vibrational spectral features with bond parameters of the glass network created by molecular dynamics (MD) simulations. A series of sodium silicate glasses with compositions of [Na2O]x[Al2O3]2[SiO2]98-x with x = 7, 12, 17, and 22 were synthesized and analyzed with IR and Raman. A silica glass substrate and a crystalline quartz were also analyzed for comparison. Glass structures with the same compositions were generated with MD simulations using three types of potentials: fixed partial charge pairwise (Teter), partial diffuse charge potential (MGFF), and bond order-based charge transfer potential (ReaxFF). The comparison of simulated and experimental IR spectra showed that, among these three potentials tested, ReaxFF reproduces the concentration dependence of spectral features closest to the experimentally observed trend. Hence, the bond length and angle distributions as well as Si–Qn species and ring size distributions of silica and sodium silicate glasses were obtained from ReaxFF-MD simulations and further compared with the peak assignment or deconvolution schemes—which have been widely used since 1970s and 1980s—(a)more »
- Authors:
-
- Pennsylvania State Univ., University Park, PA (United States)
- Univ. of North Texas, Denton, TX (United States)
- Corning Research and Development Corp., Corning, NY (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD); Pennsylvania State Univ., University Park, PA (United States); Univ. of North Texas, Denton, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Corning STEM Fellowship Program
- OSTI Identifier:
- 1600991
- Alternate Identifier(s):
- OSTI ID: 1598694
- Grant/Contract Number:
- SC0016584; DMR‐1609170
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Ceramic Society
- Additional Journal Information:
- Journal Volume: 103; Journal Issue: 6; Journal ID: ISSN 0002-7820
- Publisher:
- American Ceramic Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; infrared spectroscopy; molecular dynamics; Raman spectroscopy; sodium silicate glass; vibrational modes
Citation Formats
Liu, Hongshen, Hahn, Seung Ho, Ren, Mengguo, Thiruvillamalai, Mahadevan, Gross, Timothy M., Du, Jincheng, Duin, Adri C. T., and Kim, Seong H. Searching for correlations between vibrational spectral features and structural parameters of silicate glass network. United States: N. p., 2020.
Web. doi:10.1111/jace.17036.
Liu, Hongshen, Hahn, Seung Ho, Ren, Mengguo, Thiruvillamalai, Mahadevan, Gross, Timothy M., Du, Jincheng, Duin, Adri C. T., & Kim, Seong H. Searching for correlations between vibrational spectral features and structural parameters of silicate glass network. United States. https://doi.org/10.1111/jace.17036
Liu, Hongshen, Hahn, Seung Ho, Ren, Mengguo, Thiruvillamalai, Mahadevan, Gross, Timothy M., Du, Jincheng, Duin, Adri C. T., and Kim, Seong H. Sat .
"Searching for correlations between vibrational spectral features and structural parameters of silicate glass network". United States. https://doi.org/10.1111/jace.17036. https://www.osti.gov/servlets/purl/1600991.
@article{osti_1600991,
title = {Searching for correlations between vibrational spectral features and structural parameters of silicate glass network},
author = {Liu, Hongshen and Hahn, Seung Ho and Ren, Mengguo and Thiruvillamalai, Mahadevan and Gross, Timothy M. and Du, Jincheng and Duin, Adri C. T. and Kim, Seong H.},
abstractNote = {Infrared (IR) and Raman spectroscopic features of silicate glasses are usually interpreted based on the analogy with those of smaller molecules, molecular clusters, or crystalline counterparts; this study tests the accuracy and validity of these widely cited peak assignment schemes by comparing vibrational spectral features with bond parameters of the glass network created by molecular dynamics (MD) simulations. A series of sodium silicate glasses with compositions of [Na2O]x[Al2O3]2[SiO2]98-x with x = 7, 12, 17, and 22 were synthesized and analyzed with IR and Raman. A silica glass substrate and a crystalline quartz were also analyzed for comparison. Glass structures with the same compositions were generated with MD simulations using three types of potentials: fixed partial charge pairwise (Teter), partial diffuse charge potential (MGFF), and bond order-based charge transfer potential (ReaxFF). The comparison of simulated and experimental IR spectra showed that, among these three potentials tested, ReaxFF reproduces the concentration dependence of spectral features closest to the experimentally observed trend. Hence, the bond length and angle distributions as well as Si–Qn species and ring size distributions of silica and sodium silicate glasses were obtained from ReaxFF-MD simulations and further compared with the peak assignment or deconvolution schemes—which have been widely used since 1970s and 1980s—(a) correlation between the IR peak position in the Si–O stretch region (1050-1120 cm-1) and the Si–O–Si bond angle; (b) deconvolution of the Raman bands in the Si–O stretch region with the Qn speciation; and (c) assignment of the Raman bands in the 420-600 cm-1 region to the bending modes of (SiO)n rings with different sizes (typically, n = 3-6). The comparisons showed that none of these widely used methods is congruent with the bond parameters or structures of silicate glass networks produced via ReaxFF-MD simulations. This result invokes that the adequacy of these spectral interpretation methods must be questioned. Alternative interpretations are proposed, which are to be tested independently in future studies.},
doi = {10.1111/jace.17036},
journal = {Journal of the American Ceramic Society},
number = 6,
volume = 103,
place = {United States},
year = {Sat Jan 25 00:00:00 EST 2020},
month = {Sat Jan 25 00:00:00 EST 2020}
}
Web of Science
Works referenced in this record:
A molecular dynamic calculation of the structure of sodium silicate glasses
journal, December 1979
- Soules, T. F.
- The Journal of Chemical Physics, Vol. 71, Issue 11
Channel Formation and Intermediate Range Order in Sodium Silicate Melts and Glasses
journal, July 2004
- Meyer, A.; Horbach, J.; Kob, W.
- Physical Review Letters, Vol. 93, Issue 2
The structure of sodium silicate glass
journal, December 1990
- Huang, Chengde; Cormack, A. N.
- The Journal of Chemical Physics, Vol. 93, Issue 11
Dynamics of Sodium in Sodium Disilicate: Channel Relaxation and Sodium Diffusion
journal, March 2002
- Horbach, Jürgen; Kob, Walter; Binder, Kurt
- Physical Review Letters, Vol. 88, Issue 12
11B NMR studies and structural modeling of Na2OB2O3SiO2 glasses of high soda content
journal, October 1983
- Dell, W. J.; Bray, P. J.; Xiao, S. Z.
- Journal of Non-Crystalline Solids, Vol. 58, Issue 1
Network connectivity in aluminoborosilicate glasses: A high-resolution 11B, 27Al and 17O NMR study
journal, November 2005
- Du, Lin-Shu; Stebbins, Jonathan F.
- Journal of Non-Crystalline Solids, Vol. 351, Issue 43-45
Neutron scattering from vitreous silica. V. The structure of vitreous silica: What have we learned from 60 years of diffraction studies?
journal, November 1994
- Wright, Adrian C.
- Journal of Non-Crystalline Solids, Vol. 179
Vibrational spectra of simple silicate glasses
journal, January 1970
- Gaskell, P. H.
- Discussions of the Faraday Society, Vol. 50
Infrared Absorption Spectra of Sodium Silicate Glasses from 4 to 30μ
journal, December 1964
- Hanna, Rinoud; Su, G-J.
- Journal of the American Ceramic Society, Vol. 47, Issue 12
Infrared Reflectance Spectrometer for Liquids at High Temperatures
journal, May 1969
- Sweet, John R.; White, William B.
- Applied Spectroscopy, Vol. 23, Issue 3
The infrared transmission spectra of four silicate glasses before and after exposure to water
journal, October 1990
- Husung, Roy D.; Doremus, Robert H.
- Journal of Materials Research, Vol. 5, Issue 10
Specular reflectance (SR) and attenuated total reflectance (ATR) infrared (IR) spectroscopy of transparent flat glass surfaces: A case study for soda lime float glass
journal, November 2015
- Amma, Shin-ichi; Luo, Jiawei; Pantano, Carlo G.
- Journal of Non-Crystalline Solids, Vol. 428
Structural investigation of silica gel films by infrared spectroscopy
journal, October 1990
- Almeida, Rui M.; Pantano, Carlo G.
- Journal of Applied Physics, Vol. 68, Issue 8
Normal mode assignments in vitreous silica, germania and beryllium fluoride
journal, July 1971
- Bell, R. J.; Dean, P.; Hibbins-Butler, D. C.
- Journal of Physics C: Solid State Physics, Vol. 4, Issue 10
Longitudinal and Transverse Optical Lattice Vibrations in Quartz
journal, September 1967
- Scott, J. F.; Porto, S. P. S.
- Physical Review, Vol. 161, Issue 3
Raman Spectra of α and β Cristobalite
journal, November 1972
- Bates, John B.
- The Journal of Chemical Physics, Vol. 57, Issue 9
Phonons in amorphous silica
journal, September 1977
- Laughlin, R. B.; Joannopoulos, J. D.
- Physical Review B, Vol. 16, Issue 6
Theory of the vibrational spectra of some network and molecular glasses
journal, April 1975
- Brawer, Steven
- Physical Review B, Vol. 11, Issue 8
Raman spectroscopic investigation of the structure of silicate glasses. III. Raman intensities and structural units in sodium silicate glasses
journal, October 1981
- Furukawa, Toshiharu; Fox, Karen E.; White, William B.
- The Journal of Chemical Physics, Vol. 75, Issue 7
Quantitative Analysis of Glass Structure with the Use of Infrared Reflection Spectra
journal, May 1974
- Sanders, D. M.; Person, W. B.; Hench, L. L.
- Applied Spectroscopy, Vol. 28, Issue 3
Complex refractive index of silica, silicate, borosilicate, and boroaluminosilicate glasses – Analysis of glass network vibration modes with specular-reflection IR spectroscopy
journal, August 2018
- Luo, Jiawei; Smith, Nicholas J.; Pantano, Carlo G.
- Journal of Non-Crystalline Solids, Vol. 494
Vibrational Properties of Calcium Phosphate Compounds. 1. Raman Spectrum of β-Tricalcium Phosphate
journal, April 1997
- de Aza, P. N.; Santos, C.; Pazo, A.
- Chemistry of Materials, Vol. 9, Issue 4
Wall-related Raman scattering in ferroelastic lead phosphate Pb 3 (PO 4 ) 2
journal, September 2001
- Mihailova, B.; Bismayer, U.; Engelhardt, A.
- Journal of Physics: Condensed Matter, Vol. 13, Issue 41
Thermal infrared (vibrational) spectroscopy of Mg–Fe olivines: A review and applications to determining the composition of planetary surfaces
journal, March 2010
- Hamilton, Victoria E.
- Geochemistry, Vol. 70, Issue 1
Raman Spectra of Amorphous Si and Related Tetrahedrally Bonded Semiconductors
journal, March 1971
- Smith, J. E.; Brodsky, M. H.; Crowder, B. L.
- Physical Review Letters, Vol. 26, Issue 11
Phonons in glasses: From molecular to band-like modes
journal, April 1977
- Sen, P. N.; Thorpe, M. F.
- Physical Review B, Vol. 15, Issue 8
Correlation of silica glass properties with the infrared spectra
journal, January 1997
- Agarwal, Anand; Tomozawa, Minoru
- Journal of Non-Crystalline Solids, Vol. 209, Issue 1-2
Asymmetric peak line shape of infrared dielectric function spectra for thermally grown silicon dioxide films
journal, December 2000
- Ishikawa, Kenji; Suzuki, Kunihiro; Okamura, Shigeru
- Journal of Applied Physics, Vol. 88, Issue 12
Band limits and the vibrational spectra of tetrahedral glasses
journal, April 1979
- Galeener, Frank L.
- Physical Review B, Vol. 19, Issue 8
Molecular dynamics study of correlations between IR peak position and bond parameters of silica and silicate glasses: Effects of temperature and stress
journal, September 2017
- Luo, Jiawei; Zhou, Yuxing; Milner, Scott T.
- Journal of the American Ceramic Society, Vol. 101, Issue 1
Correlation between IR peak position and bond parameter of silica glass: Molecular dynamics study on fictive temperature (cooling rate) effect
journal, June 2018
- Luo, Jiawei; Zhou, Yuxing; Pantano, Carlo G.
- Journal of the American Ceramic Society, Vol. 101, Issue 12
Raman spectroscopic investigation of the structure of silicate glasses. I. The binary alkali silicates
journal, September 1975
- Brawer, Steven A.; White, William B.
- The Journal of Chemical Physics, Vol. 63, Issue 6
Raman investigation of ring configurations in vitreous silica
journal, July 1981
- Sharma, Shiv K.; Mammone, Joseph F.; Nicol, Malcolm F.
- Nature, Vol. 292, Issue 5819
Planar rings in vitreous silica
journal, May 1982
- Galeener, Frank L.
- Journal of Non-Crystalline Solids, Vol. 49, Issue 1-3
Four-membered rings in silica and aluminosilicate glasses
journal, April 1996
- Sykes, Dan; Kubicki, J. D.
- American Mineralogist, Vol. 81, Issue 3-4
Molecular orbital calculations of vibrations in three-membered aluminosilicate rings
journal, January 1993
- Kubicki, J. D.; Sykes, D.
- Physics and Chemistry of Minerals, Vol. 19, Issue 6
Polymerization of aqueous silica in H2O–K2O solutions at 25–200°C and 1bar to 20kbar
journal, April 2011
- Hunt, Jonathan D.; Kavner, Abby; Schauble, Edwin A.
- Chemical Geology, Vol. 283, Issue 3-4
Vibrational mode frequencies of H 4 SiO 4 , D 4 SiO 4 , H 6 Si 2 O 7 , and H 6 Si 3 O 9 in aqueous environment, obtained from ab initio molecular dynamics
journal, October 2012
- Spiekermann, Georg; Steele-MacInnis, Matthew; Kowalski, Piotr M.
- The Journal of Chemical Physics, Vol. 137, Issue 16
Ab initio molecular orbital calculations on the electronic structure of sodium silicate glasses
journal, July 1991
- Uchino, Takashi; Iwasaki, Matae; Sakka, Tetsuo
- The Journal of Physical Chemistry, Vol. 95, Issue 14
Study of Some Binary Silicate Glasses by Means of Reflection in Infrared
journal, May 1953
- Simon, I.; McMAHON, H. O.
- Journal of the American Ceramic Society, Vol. 36, Issue 5
Characterization of Ion Distributions Near the Surface of Sodium-Containing and Sodium-Depleted Calcium Aluminosilicate Melts
journal, January 2006
- Corrales, L. Rene; Du, Jincheng
- Journal of the American Ceramic Society, Vol. 89, Issue 1
Molecular Dynamics Simulation of the Structure and Hydroxylation of Silica Glass Surfaces
journal, September 2005
- Du, Jincheng; Cormack, Alastair N.
- Journal of the American Ceramic Society, Vol. 88, Issue 9
Development of a ReaxFF Reactive Force Field for NaSiO x /Water Systems and Its Application to Sodium and Proton Self-Diffusion
journal, July 2018
- Hahn, Seung Ho; Rimsza, Jessica; Criscenti, Louise
- The Journal of Physical Chemistry C, Vol. 122, Issue 34
Dissociative Chemisorption of Water onto Silica Surfaces and Formation of Hydronium Ions
journal, February 2008
- Mahadevan, T. S.; Garofalini, S. H.
- The Journal of Physical Chemistry C, Vol. 112, Issue 5
Evaluating Water Reactivity at Silica Surfaces Using Reactive Potentials
journal, April 2018
- Mahadevan, Thiruvilla S.; Du, Jincheng
- The Journal of Physical Chemistry C, Vol. 122, Issue 18
Non‐Newtonian viscous flow in glass
journal, June 1982
- Simmons, Joseph H.; Mohr, Robert K.; Montrose, C. J.
- Journal of Applied Physics, Vol. 53, Issue 6
Precise XPS depth profile of soda–lime–silica float glass using C60 ion beam
journal, October 2011
- Yamamoto, Yuichi; Yamamoto, Kiyoshi
- Optical Materials, Vol. 33, Issue 12
Hydration of soda-lime silicate glass, effect of alumina
journal, January 1983
- Wassick, T. A.; Doremus, R. H.; Lanford, W. A.
- Journal of Non-Crystalline Solids, Vol. 54, Issue 1-2
The medium range structure of sodium silicate glasses: a molecular dynamics simulation
journal, December 2004
- Du, J.; Cormack, A. N.
- Journal of Non-Crystalline Solids, Vol. 349
ReaxFF: A Reactive Force Field for Hydrocarbons
journal, October 2001
- van Duin, Adri C. T.; Dasgupta, Siddharth; Lorant, Francois
- The Journal of Physical Chemistry A, Vol. 105, Issue 41
The ReaxFF reactive force-field: development, applications and future directions
journal, March 2016
- Senftle, Thomas P.; Hong, Sungwook; Islam, Md Mahbubul
- npj Computational Materials, Vol. 2, Issue 1
Reactive Potentials for Advanced Atomistic Simulations
journal, July 2013
- Liang, Tao; Shin, Yun Kyung; Cheng, Yu-Ting
- Annual Review of Materials Research, Vol. 43, Issue 1
Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995
- Plimpton, Steve
- Journal of Computational Physics, Vol. 117, Issue 1
Dynamics of Confined Reactive Water in Smectite Clay–Zeolite Composites
journal, February 2012
- Pitman, Michael C.; van Duin, Adri C. T.
- Journal of the American Chemical Society, Vol. 134, Issue 6
Infrared spectroscopy of surfaces of glasses containing alkali ions
journal, September 1980
- Doremus, Robert H.
- Journal of Non-Crystalline Solids, Vol. 41, Issue 1
Kramers-Kronig analysis applied to reflection-absorption spectroscopy
journal, August 1997
- Yamamoto, Kiyoshi; Ishida, Hatsuo
- Vibrational Spectroscopy, Vol. 15, Issue 1
Quantitative analysis of the effect of disorder-induced mode coupling on infrared absorption in silica
journal, July 1988
- Kirk, C. T.
- Physical Review B, Vol. 38, Issue 2
Effects of surface initial condition on aqueous corrosion of glass-A study with a model nuclear waste glass
journal, September 2018
- Liu, Hongshen; Ngo, Dien; Ren, Mengguo
- Journal of the American Ceramic Society, Vol. 102, Issue 4
Longitudinal Optical Vibrations in Glasses: Ge and Si
journal, November 1976
- Galeener, F. L.; Lucovsky, G.
- Physical Review Letters, Vol. 37, Issue 22
Vibrational modes in amorphous silicon dioxide
journal, November 2000
- Gunde, Marta Klanjšek
- Physica B: Condensed Matter, Vol. 292, Issue 3-4
Comparison of model potentials for molecular-dynamics simulations of silica
journal, September 2005
- Herzbach, Daniel; Binder, Kurt; Müser, Martin H.
- The Journal of Chemical Physics, Vol. 123, Issue 12
Local structures of MD-modeled vitreous silica and sodium silicate glasses
journal, May 2001
- Yuan, Xianglong; Cormack, A. N.
- Journal of Non-Crystalline Solids, Vol. 283, Issue 1-3
Isotope Effects in Water: Differences of Structure, Dynamics, Spectrum, and Proton Transport between Heavy and Light Water from ReaxFF Reactive Force Field Simulations
journal, September 2018
- Zhang, Weiwei; Chen, Xing; van Duin, Adri C. T.
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 18
Structure and diffusion of ZnO–SrO–CaO–Na2O–SiO2 bioactive glasses: a combined high energy X-ray diffraction and molecular dynamics simulations study
journal, January 2013
- Xiang, Ye; Du, Jincheng; Skinner, Lawrie B.
- RSC Advances, Vol. 3, Issue 17
Structural Origin of the Thermal and Diffusion Behaviors of Lithium Aluminosilicate Crystal Polymorphs and Glasses
journal, May 2016
- Ren, Mengguo; Du, Jincheng
- Journal of the American Ceramic Society, Vol. 99, Issue 8
Composition – structure – property relationships in alkali aluminosilicate glasses: A combined experimental – computational approach towards designing functional glasses
journal, February 2019
- Ren, Mengguo; Cheng, Justin Y.; Jaccani, Siva Priya
- Journal of Non-Crystalline Solids, Vol. 505
Structural features of sodium silicate glasses from reactive force field‐based molecular dynamics simulations
journal, October 2019
- Deng, Lu; Urata, Shingo; Takimoto, Yasuyuki
- Journal of the American Ceramic Society, Vol. 103, Issue 3
Planar rings in glasses
journal, November 1982
- Galeener, F. L.
- Solid State Communications, Vol. 44, Issue 7
Ion implantation- and radiation-induced structural modifications in amorphous SiO2
journal, January 1993
- Devine, R. A. B.
- Journal of Non-Crystalline Solids, Vol. 152, Issue 1
Si–O–Si bond angle and torsion angle distribution in vitreous silica and sodium silicate glasses
journal, May 2003
- Yuan, Xianglong; Cormack, A. N.
- Journal of Non-Crystalline Solids, Vol. 319, Issue 1-2
Kramers-Kronig Analysis of Reflectance Measured at Oblique Incidence
journal, January 1967
- Berreman, Dwight W.
- Applied Optics, Vol. 6, Issue 9
On the theory of homogeneous and inhomogeneous line broadening. An exactly solvable model
journal, January 1981
- Knapp, E. W.; Fischer, S. F.
- The Journal of Chemical Physics, Vol. 74, Issue 1
The structure of soda-silica glasses: A mas NMR study
journal, November 1984
- Dupree, R.; Holland, D.; McMillan, P. W.
- Journal of Non-Crystalline Solids, Vol. 68, Issue 2-3
A review of the structures of oxide glasses by Raman spectroscopy
journal, January 2015
- Yadav, Avadhesh Kumar; Singh, Prabhakar
- RSC Advances, Vol. 5, Issue 83
The structural groups of alkali silicate glasses determined from 29Si MAS-NMR
journal, January 1991
- Maekawa, Hideki; Maekawa, Takashi; Kawamura, Katsuyuki
- Journal of Non-Crystalline Solids, Vol. 127, Issue 1
Raman-Scattering Selection-Rule Breaking and the Density of States in Amorphous Materials
journal, July 1970
- Shuker, Reuben; Gammon, Robert W.
- Physical Review Letters, Vol. 25, Issue 4
Optical Phonons in Amorphous Silicon Oxides. I. Calculation of the Density of States and Interpretation of LoTo Splittings of Amorphous Sio2
journal, June 1983
- Lehmann, A.; Schumann, L.; Hübner, K.
- physica status solidi (b), Vol. 117, Issue 2
Raman spectroscopy of graphene and graphite: Disorder, electron–phonon coupling, doping and nonadiabatic effects
journal, July 2007
- Ferrari, Andrea C.
- Solid State Communications, Vol. 143, Issue 1-2, p. 47-57
Thermal stability studies of CVD-grown graphene nanoribbons: Defect annealing and loop formation
journal, February 2009
- Campos-Delgado, J.; Kim, Y. A.; Hayashi, T.
- Chemical Physics Letters, Vol. 469, Issue 1-3
Dissociative Chemisorption of Water onto Silica Surfaces and Formation of Hydronium Ions
journal, May 2009
- Mahadevan, Thiruvilla; Garofalini, Stephen
- The Journal of Physical Chemistry C, Vol. 113, Issue 25
Composition – structure – property relationships in alkali aluminosilicate glasses: A combined experimental – computational approach towards designing functional glasses
text, January 2018
- Ren, Mengguo; Cheng, Justin Y.; Jaccani, Siva Priya
- Unpublished
Channel Formation and Intermediate Range Order in Sodium Silicate Melts and Glasses
text, January 2004
- Meyer, A.; Horbach, J.; Kob, W.
- arXiv