Stoichiometric tuning of lattice flexibility and Na diffusion in NaAlSiO4: quasielastic neutron scattering experiment andab initiomolecular dynamics simulations

Mayanak K. Gupta; Ranjan Mittal; Sajan Kumar; Baltej Singh; Niina H. Jalarvo; Olivier Delaire; Rakesh Shukla; Srungarpu N. Achary; Alexander I. Kolesnikov; Avesh K. Tyagi; Samrath L. Chaplot

doi:10.1039/d1ta03296h

Stoichiometric tuning of lattice flexibility and Na diffusion in NaAlSiO₄: quasielastic neutron scattering experiment andab initiomolecular dynamics simulations

Mayanak K. Gupta, Ranjan Mittal, Sajan Kumar, Baltej Singh, Niina H. Jalarvo, Olivier Delaire, Rakesh Shukla, Srungarpu N. Achary, Alexander I. Kolesnikov, Avesh K. Tyagi, Samrath L. Chaplot

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Abstract

We have performed quasielastic neutron scattering (QENS) experiments up to 1243 K andab initiomolecular dynamics (AIMD) simulations to investigate the Na diffusion in various phases of NaAlSiO₄(NASO), namely, low-carnegieite (L-NASO; trigonal), high-carnegieite (H-NASO; cubic) and nepheline (N-NASO; hexagonal) phases. The QENS measurements reveal Na ions localized diffusion behavior in L-NASO and N-NASO, but long-range diffusion behavior in H-NASO. The AIMD simulation supplemented the QENS measurements and showed that excess Na ions in H-NASO enhance the host network flexibility and activate the AlO₄/SiO₄tetrahedra rotational modes. These framework modes enable the long-range diffusion of Na across a pathway of interstitial sites. The simulations also show Na diffusion in Na-deficient N-NASO through vacant Na sites along the hexagonalc-axis.

Original language	English
Pages (from-to)	16129-16136
Number of pages	8
Journal	Journal of Materials Chemistry A
Volume	9
Issue number	29
DOIs	https://doi.org/10.1039/d1ta03296h
State	Published - Aug 7 2021

Funding

The use of the ANUPAM super-computing facility at BARC is acknowledged. SLC acknowledges the financial support of the Indian National Science Academy for the INSA Senior Scientist position. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The use of the ANUPAM super-computing facility at BARC is acknowledged. SLC acknowledges the nancial support of the Indian National Science Academy for the INSA Senior Scientist position. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.

Funders	Funder number
Office of Science
Oak Ridge National Laboratory
Indian National Science Academy
Bhabha Atomic Research Centre

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Gupta, M. K., Mittal, R., Kumar, S., Singh, B., Jalarvo, N. H., Delaire, O., Shukla, R., Achary, S. N., Kolesnikov, A. I., Tyagi, A. K., & Chaplot, S. L. (2021). Stoichiometric tuning of lattice flexibility and Na diffusion in NaAlSiO₄: quasielastic neutron scattering experiment andab initiomolecular dynamics simulations. Journal of Materials Chemistry A, 9(29), 16129-16136. https://doi.org/10.1039/d1ta03296h

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title = "Stoichiometric tuning of lattice flexibility and Na diffusion in NaAlSiO4: quasielastic neutron scattering experiment andab initiomolecular dynamics simulations",

abstract = "We have performed quasielastic neutron scattering (QENS) experiments up to 1243 K andab initiomolecular dynamics (AIMD) simulations to investigate the Na diffusion in various phases of NaAlSiO4(NASO), namely, low-carnegieite (L-NASO; trigonal), high-carnegieite (H-NASO; cubic) and nepheline (N-NASO; hexagonal) phases. The QENS measurements reveal Na ions localized diffusion behavior in L-NASO and N-NASO, but long-range diffusion behavior in H-NASO. The AIMD simulation supplemented the QENS measurements and showed that excess Na ions in H-NASO enhance the host network flexibility and activate the AlO4/SiO4tetrahedra rotational modes. These framework modes enable the long-range diffusion of Na across a pathway of interstitial sites. The simulations also show Na diffusion in Na-deficient N-NASO through vacant Na sites along the hexagonalc-axis.",

author = "Gupta, {Mayanak K.} and Ranjan Mittal and Sajan Kumar and Baltej Singh and Jalarvo, {Niina H.} and Olivier Delaire and Rakesh Shukla and Achary, {Srungarpu N.} and Kolesnikov, {Alexander I.} and Tyagi, {Avesh K.} and Chaplot, {Samrath L.}",

note = "Publisher Copyright: {\textcopyright} The Royal Society of Chemistry 2021.",

year = "2021",

month = aug,

day = "7",

doi = "10.1039/d1ta03296h",

language = "English",

volume = "9",

pages = "16129--16136",

journal = "Journal of Materials Chemistry A",

issn = "2050-7488",

publisher = "Royal Society of Chemistry",

number = "29",

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Gupta, MK, Mittal, R, Kumar, S, Singh, B, Jalarvo, NH, Delaire, O, Shukla, R, Achary, SN, Kolesnikov, AI, Tyagi, AK & Chaplot, SL 2021, 'Stoichiometric tuning of lattice flexibility and Na diffusion in NaAlSiO₄: quasielastic neutron scattering experiment andab initiomolecular dynamics simulations', Journal of Materials Chemistry A, vol. 9, no. 29, pp. 16129-16136. https://doi.org/10.1039/d1ta03296h

TY - JOUR

T1 - Stoichiometric tuning of lattice flexibility and Na diffusion in NaAlSiO4

T2 - quasielastic neutron scattering experiment andab initiomolecular dynamics simulations

AU - Gupta, Mayanak K.

AU - Mittal, Ranjan

AU - Kumar, Sajan

AU - Singh, Baltej

AU - Jalarvo, Niina H.

AU - Delaire, Olivier

AU - Shukla, Rakesh

AU - Achary, Srungarpu N.

AU - Kolesnikov, Alexander I.

AU - Tyagi, Avesh K.

AU - Chaplot, Samrath L.

PY - 2021/8/7

Y1 - 2021/8/7

N2 - We have performed quasielastic neutron scattering (QENS) experiments up to 1243 K andab initiomolecular dynamics (AIMD) simulations to investigate the Na diffusion in various phases of NaAlSiO4(NASO), namely, low-carnegieite (L-NASO; trigonal), high-carnegieite (H-NASO; cubic) and nepheline (N-NASO; hexagonal) phases. The QENS measurements reveal Na ions localized diffusion behavior in L-NASO and N-NASO, but long-range diffusion behavior in H-NASO. The AIMD simulation supplemented the QENS measurements and showed that excess Na ions in H-NASO enhance the host network flexibility and activate the AlO4/SiO4tetrahedra rotational modes. These framework modes enable the long-range diffusion of Na across a pathway of interstitial sites. The simulations also show Na diffusion in Na-deficient N-NASO through vacant Na sites along the hexagonalc-axis.

AB - We have performed quasielastic neutron scattering (QENS) experiments up to 1243 K andab initiomolecular dynamics (AIMD) simulations to investigate the Na diffusion in various phases of NaAlSiO4(NASO), namely, low-carnegieite (L-NASO; trigonal), high-carnegieite (H-NASO; cubic) and nepheline (N-NASO; hexagonal) phases. The QENS measurements reveal Na ions localized diffusion behavior in L-NASO and N-NASO, but long-range diffusion behavior in H-NASO. The AIMD simulation supplemented the QENS measurements and showed that excess Na ions in H-NASO enhance the host network flexibility and activate the AlO4/SiO4tetrahedra rotational modes. These framework modes enable the long-range diffusion of Na across a pathway of interstitial sites. The simulations also show Na diffusion in Na-deficient N-NASO through vacant Na sites along the hexagonalc-axis.

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DO - 10.1039/d1ta03296h

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AN - SCOPUS:85111446649

SN - 2050-7488

VL - 9

SP - 16129

EP - 16136

JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

IS - 29

ER -

Stoichiometric tuning of lattice flexibility and Na diffusion in NaAlSiO₄: quasielastic neutron scattering experiment andab initiomolecular dynamics simulations

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