Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite
International audience The attenuated total reflectance (ATR) spectra of two calcite samples have been measured using Ge and diamond internal reflection elements. One of the samples was obtained by precipitation from solution and displays sub-micrometer sized particles. The second sample was obtaine...
Published in: | European Journal of Mineralogy |
---|---|
Main Authors: | , , , , |
Other Authors: | , , , , , , |
Format: | Article in Journal/Newspaper |
Language: | English |
Published: |
HAL CCSD
2019
|
Subjects: | |
Online Access: | https://hal.science/hal-02130238 https://hal.science/hal-02130238/document https://hal.science/hal-02130238/file/balan-19-calcite-line-broadening.pdf https://doi.org/10.1127/ejm/2018/0030-2802 |
id |
ftinsu:oai:HAL:hal-02130238v1 |
---|---|
record_format |
openpolar |
institution |
Open Polar |
collection |
Institut national des sciences de l'Univers: HAL-INSU |
op_collection_id |
ftinsu |
language |
English |
topic |
calcite infrared spectroscopy ATR multi-phonon effective medium [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] [SDU.STU.MI]Sciences of the Universe [physics]/Earth Sciences/Mineralogy |
spellingShingle |
calcite infrared spectroscopy ATR multi-phonon effective medium [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] [SDU.STU.MI]Sciences of the Universe [physics]/Earth Sciences/Mineralogy Balan, Etienne Aufort, Julie Saldi, Giuseppe Brouder, Christian Lazzeri, Michele Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite |
topic_facet |
calcite infrared spectroscopy ATR multi-phonon effective medium [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] [SDU.STU.MI]Sciences of the Universe [physics]/Earth Sciences/Mineralogy |
description |
International audience The attenuated total reflectance (ATR) spectra of two calcite samples have been measured using Ge and diamond internal reflection elements. One of the samples was obtained by precipitation from solution and displays sub-micrometer sized particles. The second sample was obtained by grinding a single-crystal of calcite (''Iceland spar'' variety). Theoretical spectra were obtained by computing the reflection coefficient of the interface between the ATR internal reflection element and a homogeneous effective medium representing the powder sample. The dielectric properties of the effective medium have been determined from those of bulk calcite using the Bruggeman approach which is adequate for standard powders with intermediate fractions of solid and empty porosity. Although this modeling approach provides a quantitative interpretation of the broadening of strong absorption bands in the calcite ATR spectra, it fails to reproduce the apparent splitting of the strong nu3 CO3 band. This problem was solved by combining the electrostatic modeling approach with a semi-quantum model of the dielectric tensor of bulk calcite, which allows for a frequency-dependent damping of the nu3 CO3 excitation. The frequency-dependence is ascribed to a multiphonon-related resonance in the nu3 CO3 phonon self-energy at a frequency close to its transverse optical frequency. The combination of approaches exposed in the present study makes it possible to discriminate among physically different processes affecting the powder infrared spectra of calcite, some being related to the long-range nature of electrostatic interactions in polar materials and others being related to atomic-scale anharmonic interactions between vibrational modes. |
author2 |
Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC) Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement IRD : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS) Géosciences Environnement Toulouse (GET) Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3) Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP) Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales Toulouse (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France-Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales Toulouse (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France-Centre National de la Recherche Scientifique (CNRS) Cluster of Excellence MATISSE led by Sorbonne UniversitésCARBORIC (ANR-13-BS06-0013-06) |
format |
Article in Journal/Newspaper |
author |
Balan, Etienne Aufort, Julie Saldi, Giuseppe Brouder, Christian Lazzeri, Michele |
author_facet |
Balan, Etienne Aufort, Julie Saldi, Giuseppe Brouder, Christian Lazzeri, Michele |
author_sort |
Balan, Etienne |
title |
Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite |
title_short |
Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite |
title_full |
Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite |
title_fullStr |
Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite |
title_full_unstemmed |
Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite |
title_sort |
line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite |
publisher |
HAL CCSD |
publishDate |
2019 |
url |
https://hal.science/hal-02130238 https://hal.science/hal-02130238/document https://hal.science/hal-02130238/file/balan-19-calcite-line-broadening.pdf https://doi.org/10.1127/ejm/2018/0030-2802 |
genre |
Iceland |
genre_facet |
Iceland |
op_source |
ISSN: 0935-1221 European Journal of Mineralogy https://hal.science/hal-02130238 European Journal of Mineralogy, 2019, 31 (1), pp.73-81. ⟨10.1127/ejm/2018/0030-2802⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.1127/ejm/2018/0030-2802 hal-02130238 https://hal.science/hal-02130238 https://hal.science/hal-02130238/document https://hal.science/hal-02130238/file/balan-19-calcite-line-broadening.pdf doi:10.1127/ejm/2018/0030-2802 |
op_rights |
info:eu-repo/semantics/OpenAccess |
op_doi |
https://doi.org/10.1127/ejm/2018/0030-2802 |
container_title |
European Journal of Mineralogy |
container_volume |
31 |
container_issue |
1 |
container_start_page |
73 |
op_container_end_page |
81 |
_version_ |
1785585880380997632 |
spelling |
ftinsu:oai:HAL:hal-02130238v1 2023-12-17T10:32:18+01:00 Line-broadening and anharmonic effects in the attenuated total reflectance infrared spectra of calcite Balan, Etienne Aufort, Julie Saldi, Giuseppe Brouder, Christian Lazzeri, Michele Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC) Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement IRD : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS) Géosciences Environnement Toulouse (GET) Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3) Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP) Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales Toulouse (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France-Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales Toulouse (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France-Centre National de la Recherche Scientifique (CNRS) Cluster of Excellence MATISSE led by Sorbonne UniversitésCARBORIC (ANR-13-BS06-0013-06) 2019-02-21 https://hal.science/hal-02130238 https://hal.science/hal-02130238/document https://hal.science/hal-02130238/file/balan-19-calcite-line-broadening.pdf https://doi.org/10.1127/ejm/2018/0030-2802 en eng HAL CCSD Copernicus info:eu-repo/semantics/altIdentifier/doi/10.1127/ejm/2018/0030-2802 hal-02130238 https://hal.science/hal-02130238 https://hal.science/hal-02130238/document https://hal.science/hal-02130238/file/balan-19-calcite-line-broadening.pdf doi:10.1127/ejm/2018/0030-2802 info:eu-repo/semantics/OpenAccess ISSN: 0935-1221 European Journal of Mineralogy https://hal.science/hal-02130238 European Journal of Mineralogy, 2019, 31 (1), pp.73-81. ⟨10.1127/ejm/2018/0030-2802⟩ calcite infrared spectroscopy ATR multi-phonon effective medium [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] [SDU.STU.MI]Sciences of the Universe [physics]/Earth Sciences/Mineralogy info:eu-repo/semantics/article Journal articles 2019 ftinsu https://doi.org/10.1127/ejm/2018/0030-2802 2023-11-22T17:45:14Z International audience The attenuated total reflectance (ATR) spectra of two calcite samples have been measured using Ge and diamond internal reflection elements. One of the samples was obtained by precipitation from solution and displays sub-micrometer sized particles. The second sample was obtained by grinding a single-crystal of calcite (''Iceland spar'' variety). Theoretical spectra were obtained by computing the reflection coefficient of the interface between the ATR internal reflection element and a homogeneous effective medium representing the powder sample. The dielectric properties of the effective medium have been determined from those of bulk calcite using the Bruggeman approach which is adequate for standard powders with intermediate fractions of solid and empty porosity. Although this modeling approach provides a quantitative interpretation of the broadening of strong absorption bands in the calcite ATR spectra, it fails to reproduce the apparent splitting of the strong nu3 CO3 band. This problem was solved by combining the electrostatic modeling approach with a semi-quantum model of the dielectric tensor of bulk calcite, which allows for a frequency-dependent damping of the nu3 CO3 excitation. The frequency-dependence is ascribed to a multiphonon-related resonance in the nu3 CO3 phonon self-energy at a frequency close to its transverse optical frequency. The combination of approaches exposed in the present study makes it possible to discriminate among physically different processes affecting the powder infrared spectra of calcite, some being related to the long-range nature of electrostatic interactions in polar materials and others being related to atomic-scale anharmonic interactions between vibrational modes. Article in Journal/Newspaper Iceland Institut national des sciences de l'Univers: HAL-INSU European Journal of Mineralogy 31 1 73 81 |