Neutron scattering and neural-network quantum molecular dynamics investigation of the vibrations of ammonia along the solid-to-liquid transition

Linker, T. M.; Krishnamoorthy, A.; Daemen, L. L.; Ramirez-Cuesta, A. J.; Nomura, K.; Nakano, A.; Cheng, Y. Q.; Hicks, W. R.; Kolesnikov, A. I.; Vashishta, P. D.

doi:10.1038/s41467-024-48246-9

Title: Neutron scattering and neural-network quantum molecular dynamics investigation of the vibrations of ammonia along the solid-to-liquid transition

Journal Article · 08 May 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-48246-9 · OSTI ID:2349125

Linker, T. M.; Krishnamoorthy, A.; Daemen, L. L.;

; Nomura, K.;

;

; Hicks, W. R.;

;

Abstract Vibrational spectroscopy allows us to understand complex physical and chemical interactions of molecular crystals and liquids such as ammonia, which has recently emerged as a strong hydrogen fuel candidate to support a sustainable society. We report inelastic neutron scattering measurement of vibrational properties of ammonia along the solid-to-liquid phase transition with high enough resolution for direct comparisons to ab-initio simulations. Theoretical analysis reveals the essential role of nuclear quantum effects (NQEs) for correctly describing the intermolecular spectrum as well as high energy intramolecular N-H stretching modes. This is achieved by training neural network models using ab-initio path-integral molecular dynamics (PIMD) simulations, thereby encompassing large spatiotemporal trajectories required to resolve low energy dynamics while retaining NQEs. Our results not only establish the role of NQEs in ammonia but also provide general computational frameworks to study complex molecular systems with NQEs.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; AC05-00OR22725

OSTI ID:: 2349125

Alternate ID(s):: OSTI ID: 2351012

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (64)

Vibrational Spectroscopy with Neutrons: A Review of New Directions Parker, Stewart F.; Lennon, David; Albers, Peter W. Applied Spectroscopy, Vol. 65, Issue 12 https://doi.org/10.1366/11-06456	journal	December 2011
Perspective: Machine learning potentials for atomistic simulations Behler, Jörg The Journal of Chemical Physics, Vol. 145, Issue 17 https://doi.org/10.1063/1.4966192	journal	November 2016
FIGURE 1 in Species of Macrostomum (Macrostomorpha: Macrostomidae) from the coastal region of Lima, Peru, with comments on M. rostratum Papi, 1951 Reyes, Jhoe; Brusa, Francisco Zenodo https://doi.org/10.5281/zenodo.1084057	image	January 2017
Accurate and Numerically Efficient r ² SCAN Meta-Generalized Gradient Approximation Furness, James W.; Kaplan, Aaron D.; Ning, Jinliang The Journal of Physical Chemistry Letters, Vol. 11, Issue 19 https://doi.org/10.1021/acs.jpclett.0c02405	journal	September 2020
How to remove the spurious resonances from ring polymer molecular dynamics Rossi, Mariana; Ceriotti, Michele; Manolopoulos, David E. The Journal of Chemical Physics, Vol. 140, Issue 23 https://doi.org/10.1063/1.4883861	journal	June 2014
LiquidLib: A comprehensive toolbox for analyzing classical and ab initio molecular dynamics simulations of liquids and liquid-like matter with applications to neutron scattering experiments Walter, Nathan P.; Jaiswal, Abhishek; Cai, Zhikun Computer Physics Communications, Vol. 228 https://doi.org/10.1016/j.cpc.2018.03.005	journal	July 2018
On the Anomalous Line-Shapes in the Ammonia Inversion Spectrum at High Pressures Anderson, P. W. Physical Review, Vol. 75, Issue 9 https://doi.org/10.1103/PhysRev.75.1450.2	journal	May 1949
Seeing real-space dynamics of liquid water through inelastic x-ray scattering Iwashita, Takuya; Wu, Bin; Chen, Wei-Ren Science Advances, Vol. 3, Issue 12 https://doi.org/10.1126/sciadv.1603079	journal	December 2017
Lattice Dynamics of Ammonia Zeng, W. Y.; Anderson, A. physica status solidi (b), Vol. 162, Issue 1 https://doi.org/10.1002/pssb.2221620107	journal	November 1990
Energy-Efficient Ammonia Production from Air and Water Using Electrocatalysts with Limited Faradaic Efficiency Hollevoet, Lander; De Ras, Michiel; Roeffaers, Maarten ACS Energy Letters, Vol. 5, Issue 4 https://doi.org/10.1021/acsenergylett.0c00455	journal	March 2020
Hydrogen bonding in solid ammonia from ab initio calculations Fortes, A. D.; Brodholt, J. P.; Wood, I. G. The Journal of Chemical Physics, Vol. 118, Issue 13 https://doi.org/10.1063/1.1555630	journal	April 2003
Dielectric Constant of Liquid Water Determined with Neural Network Quantum Molecular Dynamics Krishnamoorthy, Aravind; Nomura, Ken-ichi; Baradwaj, Nitish Physical Review Letters, Vol. 126, Issue 21 https://doi.org/10.1103/PhysRevLett.126.216403	journal	May 2021
SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS Granroth, G. E.; Kolesnikov, A. I.; Sherline, T. E. Journal of Physics: Conference Series, Vol. 251 https://doi.org/10.1088/1742-6596/251/1/012058	journal	November 2010
The microscopic origin of the anomalous isotopic properties of ice relies on the strong quantum anharmonic regime of atomic vibration Cherubini, Marco; Monacelli, Lorenzo; Mauri, Francesco The Journal of Chemical Physics, Vol. 155, Issue 18 https://doi.org/10.1063/5.0062689	journal	November 2021
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
First-principles modeling of molecular crystals: structures and stabilities, temperature and pressure: First-principles modeling of molecular crystals Hoja, Johannes; Reilly, Anthony M.; Tkatchenko, Alexandre Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 7, Issue 1 https://doi.org/10.1002/wcms.1294	journal	December 2016
Determination of the phonon spectrum from coherent neutron scattering by polycrystals Breuer, N. Zeitschrift für Physik, Vol. 271, Issue 3 https://doi.org/10.1007/BF01677937	journal	September 1974
E(3)-equivariant graph neural networks for data-efficient and accurate interatomic potentials Batzner, Simon; Musaelian, Albert; Sun, Lixin Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-29939-5	journal	May 2022
Inelastic neutron scattering studies of hydrogen bonding in ices Li, Jichen The Journal of Chemical Physics, Vol. 105, Issue 16 https://doi.org/10.1063/1.472525	journal	October 1996
Exploring far-from-equilibrium ultrafast polarization control in ferroelectric oxides with excited-state neural network quantum molecular dynamics Linker, Thomas; Nomura, Ken-ichi; Aditya, Anikeya Science Advances, Vol. 8, Issue 12 https://doi.org/10.1126/sciadv.abk2625	journal	March 2022
Ab Initio Calculation of Vibrational Absorption and Circular Dichroism Spectra Using Density Functional Force Fields Stephens, P. J.; Devlin, F. J.; Chabalowski, C. F. The Journal of Physical Chemistry, Vol. 98, Issue 45, p. 11623-11627 https://doi.org/10.1021/j100096a001	journal	November 1994
Structural, electronic, and dynamical properties of liquid water by ab initio molecular dynamics based on SCAN functional within the canonical ensemble Zheng, Lixin; Chen, Mohan; Sun, Zhaoru The Journal of Chemical Physics, Vol. 148, Issue 16 https://doi.org/10.1063/1.5023611	journal	April 2018
i-PI 2.0: A universal force engine for advanced molecular simulations Kapil, Venkat; Rossi, Mariana; Marsalek, Ondrej Computer Physics Communications, Vol. 236 https://doi.org/10.1016/j.cpc.2018.09.020	journal	March 2019
The formulation of quantum statistical mechanics based on the Feynman path centroid density. IV. Algorithms for centroid molecular dynamics Cao, Jianshu; Voth, Gregory A. The Journal of Chemical Physics, Vol. 101, Issue 7 https://doi.org/10.1063/1.468399	journal	October 1994
DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6 https://doi.org/10.6028/jres.114.025	journal	November 2009
B3LYP augmented with an empirical dispersion term (B3LYP-D*) as applied to molecular crystals Civalleri, Bartolomeo; Zicovich-Wilson, Claudio M.; Valenzano, Loredana CrystEngComm, Vol. 10, Issue 4 https://doi.org/10.1039/B715018K	journal	January 2008
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Molecular Origin of the Vibrational Structure of Ice I _h Moberg, Daniel R.; Straight, Shelby C.; Knight, Christopher The Journal of Physical Chemistry Letters, Vol. 8, Issue 12 https://doi.org/10.1021/acs.jpclett.7b01106	journal	May 2017
From Single Hydrogen Bonds to Extended Hydrogen‐Bond Wires: Low‐Dimensional Model Systems for Vibrational Spectroscopy of Associated Liquids Olschewski, Martin; Knop, Stephan; Lindner, Jörg Angewandte Chemie International Edition, Vol. 52, Issue 37 https://doi.org/10.1002/anie.201210009	journal	July 2013
The effect of recoil on the inelastic neutron scattering spectra of molecular vibrations Tomkinson, J. Chemical Physics, Vol. 127, Issue 1-3 https://doi.org/10.1016/0301-0104(88)87142-8	journal	November 1988
Photoelectron spectra of alkali metal–ammonia microjets: From blue electrolyte to bronze metal Buttersack, Tillmann; Mason, Philip E.; McMullen, Ryan S. Science, Vol. 368, Issue 6495 https://doi.org/10.1126/science.aaz7607	journal	June 2020
Van der Waals density functionals applied to solids Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos Physical Review B, Vol. 83, Issue 19 https://doi.org/10.1103/PhysRevB.83.195131	journal	May 2011
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao Scripta Materialia, Vol. 108 https://doi.org/10.1016/j.scriptamat.2015.07.021	journal	November 2015
Raman spectra of molecular crystals. Ammonia and 3-deutero-ammonia Binbrek, O. S.; Anderson, A. Chemical Physics Letters, Vol. 15, Issue 3 https://doi.org/10.1016/0009-2614(72)80205-7	journal	August 1972
Theory of Slow Neutron Scattering by Liquids. I Rahman, A.; Singwi, K. S.; Sjölander, A. Physical Review, Vol. 126, Issue 3 https://doi.org/10.1103/PhysRev.126.986	journal	May 1962
Raman spectral analysis of liquid ammonia and aqueous solution of ammonia Ujike, Tomoko; Tominaga, Yasunori Journal of Raman Spectroscopy, Vol. 33, Issue 6 https://doi.org/10.1002/jrs.881	journal	January 2002
Chemical accuracy for the van der Waals density functional Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos Journal of Physics: Condensed Matter, Vol. 22, Issue 2 https://doi.org/10.1088/0953-8984/22/2/022201	journal	December 2009
Van der Waals Density Functional for General Geometries Dion, M.; Rydberg, H.; Schröder, E. Physical Review Letters, Vol. 92, Issue 24 https://doi.org/10.1103/PhysRevLett.92.246401	journal	June 2004
Resolution of VISION, a crystal-analyzer spectrometer Seeger, Philip A.; Daemen, Luke L.; Larese, John Z. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 604, Issue 3 https://doi.org/10.1016/j.nima.2009.03.204	journal	June 2009
Progress in green ammonia production as potential carbon-free fuel Chehade, Ghassan; Dincer, Ibrahim Fuel, Vol. 299 https://doi.org/10.1016/j.fuel.2021.120845	journal	September 2021
Ab initio thermodynamics of liquid and solid water Cheng, Bingqing; Engel, Edgar A.; Behler, Jörg Proceedings of the National Academy of Sciences, Vol. 116, Issue 4 https://doi.org/10.1073/pnas.1815117116	journal	January 2019
Higher-accuracy van der Waals density functional Lee, Kyuho; Murray, Éamonn D.; Kong, Lingzhu Physical Review B, Vol. 82, Issue 8 https://doi.org/10.1103/PhysRevB.82.081101	journal	August 2010
Ab initio theory and modeling of water Chen, Mohan; Ko, Hsin-Yu; Remsing, Richard C. Proceedings of the National Academy of Sciences, Vol. 114, Issue 41 https://doi.org/10.1073/pnas.1712499114	journal	September 2017
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Does Ammonia Hydrogen Bond? Nelson, David D.; Fraser, Gerald T.; Klemperer, William Science, Vol. 238, Issue 4834 https://doi.org/10.1126/science.238.4834.1670	journal	December 1987
Strongly Constrained and Appropriately Normed Semilocal Density Functional Sun, Jianwei; Ruzsinszky, Adrienn; Perdew, John P. Physical Review Letters, Vol. 115, Issue 3 https://doi.org/10.1103/PhysRevLett.115.036402	journal	July 2015
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Microscopic structure of low temperature liquid ammonia: A neutron diffraction experiment Ricci, M. A.; Nardone, M.; Ricci, F. P. The Journal of Chemical Physics, Vol. 102, Issue 19 https://doi.org/10.1063/1.469016	journal	May 1995
From ab initio quantum chemistry to molecular dynamics: The delicate case of hydrogen bonding in ammonia Boese, A. Daniel; Chandra, Amalendu; Martin, Jan M. L. The Journal of Chemical Physics, Vol. 119, Issue 12 https://doi.org/10.1063/1.1599338	journal	September 2003
Plane-wave pseudopotential implementation and performance of SCAN meta-GGA exchange-correlation functional for extended systems Yao, Yi; Kanai, Yosuke The Journal of Chemical Physics, Vol. 146, Issue 22 https://doi.org/10.1063/1.4984939	journal	June 2017
Regeneration of Ammonia Borane Spent Fuel by Direct Reaction with Hydrazine and Liquid Ammonia Sutton, A. D.; Burrell, A. K.; Dixon, D. A. Science, Vol. 331, Issue 6023 https://doi.org/10.1126/science.1199003	journal	March 2011
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Convenient, room-temperature liquid ammonia routes to metal chalcogenides Henshaw, Geoff; Parkin, Ivan P.; Shaw, Graham A. Journal of the Chemical Society, Dalton Transactions, Issue 2 https://doi.org/10.1039/A605665B	journal	January 1997
Simulation of Inelastic Neutron Scattering Spectra Directly from Molecular Dynamics Trajectories Cheng, Y. Q.; Kolesnikov, A. I.; Ramirez-Cuesta, A. J. Journal of Chemical Theory and Computation, Vol. 16, Issue 12 https://doi.org/10.1021/acs.jctc.0c00937	journal	November 2020
DFT-MD and vibrational anharmonicities of a phosphorylated amino acid. Success and failure Cimas, Alvaro; Gaigeot, Marie-Pierre Physical Chemistry Chemical Physics, Vol. 12, Issue 14 https://doi.org/10.1039/b924025j	journal	January 2010
Simulation of Inelastic Neutron Scattering Spectra Using OCLIMAX Cheng, Y. Q.; Daemen, L. L.; Kolesnikov, A. I. Journal of Chemical Theory and Computation, Vol. 15, Issue 3 https://doi.org/10.1021/acs.jctc.8b01250	journal	January 2019
RXMD: A scalable reactive molecular dynamics simulator for optimized time-to-solution Nomura, Ken-ichi; Kalia, Rajiv K.; Nakano, Aiichiro SoftwareX, Vol. 11 https://doi.org/10.1016/j.softx.2019.100389	journal	January 2020
Hydrogen Bonding in Liquid Ammonia Krishnamoorthy, Aravind; Nomura, Ken-ichi; Baradwaj, Nitish The Journal of Physical Chemistry Letters, Vol. 13, Issue 30 https://doi.org/10.1021/acs.jpclett.2c01608	journal	July 2022
Structure of powder deuteroammonia between 2 and 180 K revisited: A refinement of the neutron diffraction pattern taking into account molecular reorientations: analysis of the diffuse intensity Leclercq, Françoise; Damay, Pierre; Foukani, Mohammed The Journal of Chemical Physics, Vol. 102, Issue 11 https://doi.org/10.1063/1.469489	journal	March 1995
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales Thompson, Aidan P.; Aktulga, H. Metin; Berger, Richard Computer Physics Communications, Vol. 271 https://doi.org/10.1016/j.cpc.2021.108171	journal	February 2022
Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
Frequency distribution function of solid ammonia Goyal, P. S.; Dasannacharya, B. A.; Thaper, C. L. physica status solidi (b), Vol. 50, Issue 2 https://doi.org/10.1002/pssb.2220500232	journal	April 1972
Ring-Polymer Molecular Dynamics: Quantum Effects in Chemical Dynamics from Classical Trajectories in an Extended Phase Space Habershon, Scott; Manolopoulos, David E.; Markland, Thomas E. Annual Review of Physical Chemistry, Vol. 64, Issue 1 https://doi.org/10.1146/annurev-physchem-040412-110122	journal	April 2013

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