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

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

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.

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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

@article{40080f39c2654d17b6dfe8985377d752,

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",

}

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.

UR - https://www.scopus.com/pages/publications/85111446649

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DO - 10.1039/d1ta03296h

M3 - Article

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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