Angela F Harper, Tabea Huss, Simone Koecher, Christoph Scheurer
We present for the first time a multiscale machine learning approach to jointly simulate atomic structure and dynamics with the corresponding solid state Nuclear Magnetic Resonance (ssNMR) observables. We study the use-case of spin-alignment echo (SAE) NMR for exploring Li-ion diffusion within the solid state electrolyte material Li3PS4 (LPS) by calculating quadrupolar frequencies of 7Li. SAE NMR probes long-range dynamics down to microsecond-timescale hopping processes. Therefore only a few machine learning force field schemes are able to capture the time- and length scales required for accurate comparison with experimental results. By using a new class of machine learning interatomic potentials, known as ultra-fast potentials (UFPs), we are able to efficiently access timescales beyond the microsecond regime. In tandem, we have developed a machine learning model for predicting the full 7Li electric field gradient (EFG) tensors in LPS. By combining the long timescale trajectories from the UFP with our model for 7Li EFG tensors, we are able to extract the autocorrelation function (ACF) for 7Li quadrupolar frequencies during Li diffusion. We extract the decay constants from the ACF for both crystalline β-LPS and amorphous LPS, and find that the predicted Li hopping rates are on the same order of magnitude as those predicted from the Li dynamics. This demonstrates the potential for machine learning to finally make predictions on experimentally relevant timescales and temperatures, and opens a new avenue of NMR crystallography: using machine learning dynamical NMR simulations for accessing polycrystalline and glass ceramic materials.
{"title":"Tracking Li atoms in real-time with ultra-fast NMR simulations","authors":"Angela F Harper, Tabea Huss, Simone Koecher, Christoph Scheurer","doi":"10.1039/d4fd00074a","DOIUrl":"https://doi.org/10.1039/d4fd00074a","url":null,"abstract":"We present for the first time a multiscale machine learning approach to jointly simulate atomic structure and dynamics with the corresponding solid state Nuclear Magnetic Resonance (ssNMR) observables. We study the use-case of spin-alignment echo (SAE) NMR for exploring Li-ion diffusion within the solid state electrolyte material Li<small><sub>3</sub></small>PS<small><sub>4</sub></small> (LPS) by calculating quadrupolar frequencies of <small><sup>7</sup></small>Li. SAE NMR probes long-range dynamics down to microsecond-timescale hopping processes. Therefore only a few machine learning force field schemes are able to capture the time- and length scales required for accurate comparison with experimental results. By using a new class of machine learning interatomic potentials, known as ultra-fast potentials (UFPs), we are able to efficiently access timescales beyond the microsecond regime. In tandem, we have developed a machine learning model for predicting the full <small><sup>7</sup></small>Li electric field gradient (EFG) tensors in LPS. By combining the long timescale trajectories from the UFP with our model for <small><sup>7</sup></small>Li EFG tensors, we are able to extract the autocorrelation function (ACF) for <small><sup>7</sup></small>Li quadrupolar frequencies during Li diffusion. We extract the decay constants from the ACF for both crystalline β-LPS and amorphous LPS, and find that the predicted Li hopping rates are on the same order of magnitude as those predicted from the Li dynamics. This demonstrates the potential for machine learning to finally make predictions on experimentally relevant timescales and temperatures, and opens a new avenue of NMR crystallography: using machine learning dynamical NMR simulations for accessing polycrystalline and glass ceramic materials.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"28 1","pages":""},"PeriodicalIF":3.4,"publicationDate":"2024-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140833918","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hyunsoo Park, Anthony Onwuli, Keith Butler, Aron Walsh
The combination of elements from the Periodic Table defines a vast chemical space. Only a small fraction of these combinations yields materials that occur naturally or are accessible synthetically. Here, we enumerate binary, ternary, and quaternary element and species combinations to produce an extensive library of over 10^10 stoichiometric inorganic compositions. The unique combinations are vectorised using compositional embedding vectors drawn from a variety of published machine-learning models. Dimensionality reduction techniques are employed to present a two-dimensional representation of inorganic crystal-chemical space, which is labelled according to whether they pass standard chemical filters and if they appear in known materials databases.
{"title":"Mapping inorganic crystal chemical space","authors":"Hyunsoo Park, Anthony Onwuli, Keith Butler, Aron Walsh","doi":"10.1039/d4fd00063c","DOIUrl":"https://doi.org/10.1039/d4fd00063c","url":null,"abstract":"The combination of elements from the Periodic Table defines a vast chemical space. Only a small fraction of these combinations yields materials that occur naturally or are accessible synthetically. Here, we enumerate binary, ternary, and quaternary element and species combinations to produce an extensive library of over 10^10 stoichiometric inorganic compositions. The unique combinations are vectorised using compositional embedding vectors drawn from a variety of published machine-learning models. Dimensionality reduction techniques are employed to present a two-dimensional representation of inorganic crystal-chemical space, which is labelled according to whether they pass standard chemical filters and if they appear in known materials databases.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"5 1","pages":""},"PeriodicalIF":3.4,"publicationDate":"2024-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140576864","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mark Aarts, Martin Z. Bazant, Lydéric Bocquet, Fabio Cicoira, Robert A. W. Dryfe, Sanli Faez, Y. K. Catherine Fung, Ehud Haimov, Bee Hockin, Christian Holm, Tim M. Kamsma, Frédéric Kanoufi, Alexei A. Kornyshev, Serge G. Lemay, Yan Levin, Sophie Marbach, Elalyaa Mohamed, Joan Montes de Oca, Frieder Mugele, Monica Olvera de la Cruz, Susan Perkin, Jenny Pringle, Paul Robin, Benjamin Rotenberg, Alexander Schlaich, Igor Siretanu, Zuzanna S. Siwy, Derek Stein, René van Roij, Tanja Vidaković-Koch, Kislon Voïtchovsky, Gilad Yossifon and Yujia Zhang
{"title":"Iontronic dynamics: general discussion","authors":"Mark Aarts, Martin Z. Bazant, Lydéric Bocquet, Fabio Cicoira, Robert A. W. Dryfe, Sanli Faez, Y. K. Catherine Fung, Ehud Haimov, Bee Hockin, Christian Holm, Tim M. Kamsma, Frédéric Kanoufi, Alexei A. Kornyshev, Serge G. Lemay, Yan Levin, Sophie Marbach, Elalyaa Mohamed, Joan Montes de Oca, Frieder Mugele, Monica Olvera de la Cruz, Susan Perkin, Jenny Pringle, Paul Robin, Benjamin Rotenberg, Alexander Schlaich, Igor Siretanu, Zuzanna S. Siwy, Derek Stein, René van Roij, Tanja Vidaković-Koch, Kislon Voïtchovsky, Gilad Yossifon and Yujia Zhang","doi":"10.1039/D3FD90032K","DOIUrl":"10.1039/D3FD90032K","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"246 ","pages":" 322-355"},"PeriodicalIF":3.4,"publicationDate":"2023-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41090532","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sidahmed Abayzeed, Tarique Anwar, Alexander Barnaveli, Martin Z. Bazant, Lyderic Bocquet, Aleksandar Donev, Robert A. W. Dryfe, Sanli Faez, Amritha Janardanan, Felipe Jiménez-Ángeles, Tim M. Kamsma, Frédéric Kanoufi, Alexei A. Kornyshev, Serge G. Lemay, Yan Levin, Sophie Marbach, Joan Montes de Oca, Paul Robin, Zuzanna S. Siwy, Derek Stein, Rene van Roij, Tanja Vidaković-Koch, Gilad Yossifon and Yujia Zhang
{"title":"Iontronic coupling: general discussion","authors":"Sidahmed Abayzeed, Tarique Anwar, Alexander Barnaveli, Martin Z. Bazant, Lyderic Bocquet, Aleksandar Donev, Robert A. W. Dryfe, Sanli Faez, Amritha Janardanan, Felipe Jiménez-Ángeles, Tim M. Kamsma, Frédéric Kanoufi, Alexei A. Kornyshev, Serge G. Lemay, Yan Levin, Sophie Marbach, Joan Montes de Oca, Paul Robin, Zuzanna S. Siwy, Derek Stein, Rene van Roij, Tanja Vidaković-Koch, Gilad Yossifon and Yujia Zhang","doi":"10.1039/D3FD90031B","DOIUrl":"10.1039/D3FD90031B","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"246 ","pages":" 157-178"},"PeriodicalIF":3.4,"publicationDate":"2023-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41090783","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nadia Balucani, Michelle Brann, Sandra Brünken, Cecilia Ceccarelli, Martin Cordiner, Eric M. Crump, Kevin M. Douglas, Adam J. Fleisher, Athena Flint, Jack Fulker, Robin T. Garrod, Murthy S. Gudipati, Divita Gupta, Joshua Halpern, Dwayne E. Heard, Eric Herbst, Emily K. Hockey, Ko-Yun Huang, Ugo Jacovella, Inga Kamp, Alexander K. Lemmens, Nikku Madhusudhan, Martin R. S. McCoustra, Brett McGuire, Anthony Meijer, Cristina Puzzarini, Daniël B. Rap, Ian R. Sims, Mark H. Stockett, Ardjan Sturm, Arthur G. Suits, Ewine F. van Dishoeck, Serena Viti, Nicholas Walker, Susanna Widicus Weaver, Laurent Wiesenfeld and Olivia H. Wilkins
{"title":"Laboratory astrochemistry of the gas phase: general discussion","authors":"Nadia Balucani, Michelle Brann, Sandra Brünken, Cecilia Ceccarelli, Martin Cordiner, Eric M. Crump, Kevin M. Douglas, Adam J. Fleisher, Athena Flint, Jack Fulker, Robin T. Garrod, Murthy S. Gudipati, Divita Gupta, Joshua Halpern, Dwayne E. Heard, Eric Herbst, Emily K. Hockey, Ko-Yun Huang, Ugo Jacovella, Inga Kamp, Alexander K. Lemmens, Nikku Madhusudhan, Martin R. S. McCoustra, Brett McGuire, Anthony Meijer, Cristina Puzzarini, Daniël B. Rap, Ian R. Sims, Mark H. Stockett, Ardjan Sturm, Arthur G. Suits, Ewine F. van Dishoeck, Serena Viti, Nicholas Walker, Susanna Widicus Weaver, Laurent Wiesenfeld and Olivia H. Wilkins","doi":"10.1039/D3FD90025H","DOIUrl":"https://doi.org/10.1039/D3FD90025H","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"245 ","pages":" 391-445"},"PeriodicalIF":3.4,"publicationDate":"2023-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"24849612","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Stefan T. Bromley, Sandra Brünken, Cecilia Ceccarelli, Martin Cordiner, Kristen Darnell, Gwenaëlle Dufour, Athena Flint, Robin T. Garrod, Murthy S. Gudipati, Joshua Halpern, Eric Herbst, Ko-Yun Huang, Inga Kamp, Nikku Madhusudhan, Martin R. S. McCoustra, Arthur G. Suits, Marie Van de Sande, Ewine F. van Dishoeck, Serena Viti and Laurent Wiesenfeld
{"title":"Computational astrochemistry: general discussion","authors":"Stefan T. Bromley, Sandra Brünken, Cecilia Ceccarelli, Martin Cordiner, Kristen Darnell, Gwenaëlle Dufour, Athena Flint, Robin T. Garrod, Murthy S. Gudipati, Joshua Halpern, Eric Herbst, Ko-Yun Huang, Inga Kamp, Nikku Madhusudhan, Martin R. S. McCoustra, Arthur G. Suits, Marie Van de Sande, Ewine F. van Dishoeck, Serena Viti and Laurent Wiesenfeld","doi":"10.1039/D3FD90027D","DOIUrl":"https://doi.org/10.1039/D3FD90027D","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"245 ","pages":" 620-637"},"PeriodicalIF":3.4,"publicationDate":"2023-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"24849656","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nadia Balucani, Mathieu Bertin, Michelle Brann, Wendy A. Brown, Cecilia Ceccarelli, Rafael Martín-Doménech, Jack Fulker, Robin T. Garrod, Joel Green, Murthy S. Gudipati, Dwayne E. Heard, Eric Herbst, Ugo Jacovella, Inga Kamp, Martin R. S. McCoustra, W. M. C. Sameera, Ian Sims, Ardjan Sturm, Serena Viti, Susanna Widicus Weaver, Laurent Wiesenfeld and Olivia H. Wilkins
{"title":"Laboratory astrochemistry of and on dust and ices: general discussion","authors":"Nadia Balucani, Mathieu Bertin, Michelle Brann, Wendy A. Brown, Cecilia Ceccarelli, Rafael Martín-Doménech, Jack Fulker, Robin T. Garrod, Joel Green, Murthy S. Gudipati, Dwayne E. Heard, Eric Herbst, Ugo Jacovella, Inga Kamp, Martin R. S. McCoustra, W. M. C. Sameera, Ian Sims, Ardjan Sturm, Serena Viti, Susanna Widicus Weaver, Laurent Wiesenfeld and Olivia H. Wilkins","doi":"10.1039/D3FD90026F","DOIUrl":"https://doi.org/10.1039/D3FD90026F","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"245 ","pages":" 519-540"},"PeriodicalIF":3.4,"publicationDate":"2023-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"24849631","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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