Faraday Discussions最新文献

{"title":"Novel perturbative and variational methods for stronger correlations: general discussion.","authors":"Vibin Abraham, Kemal Atalar, Kenneth O Berard, George H Booth, Hugh G A Burton, Garnet K-L Chan, Francesco A Evangelista, Maria-Andreea Filip, Emmanuel Giner, Alexander Gunasekera, Peter J Knowles, Marie-Bernadette Lepetit, Ke Liao, Pierre-François Loos, Erika Magnusson, Nicholas J Mayhall, Carlos Mejuto-Zaera, Frank Neese, Verena A Neufeld, Pinkie Ntola, Felix Plasser, Visagan Ravindran, Christian Schilling, Gustavo Scuseria, James Shee, Benjamin X Shi, David P Tew, Alex J W Thom, Zikuan Wang, Dominika Zgid","doi":"10.1039/d4fd90041c","DOIUrl":"https://doi.org/10.1039/d4fd90041c","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142386448","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}

{"title":"Structure and dynamics in dense ionic fluids: general discussion.","authors":"Andrew P Abbott, Rob Atkin, Muhammad Dabai Bala, Stuart J Brown, Duncan W Bruce, Paola Carbone, Franca Castiglione, Margarida Costa Gomes, Jean-François Dufrêche, Karen J Edler, Andrew Feeney, Kateryna Goloviznina, Juan Luis Gómez-Estévez, Timothy S Groves, Benworth Hansen, Rachel Hendrikse, Christian Holm, Pierre Illien, Roland Kjellander, Alexei Kornyshev, Claudio J Margulis, Joshua Maurer, Shurui Miao, Susan Perkin, Elixabete Rezabal, Beatriz Rocha de Moraes, Bernhard Roling, Benjamin Rotenberg, Joshua Sangoro, Nicolas Schaeffer, Monika Schönhoff, Karina Shimizu, John M Slattery, Neave Taylor, Yasuhiro Umebayashi, Adriaan van den Bruinhorst, Masayoshi Watanabe, Fabian Zills","doi":"10.1039/d4fd90034k","DOIUrl":"https://doi.org/10.1039/d4fd90034k","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142379532","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}

{"title":"Ionic fluids out of equilibrium: electrodeposition, dissolution, electron transfer, driving forces: general discussion.","authors":"Andrew P Abbott, Rob Atkin, Margarida Costa Gomes, Jean-François Dufrêche, Christopher E Elgar, Y K Catherine Fung, Kateryna Goloviznina, Alexis Grimaud, Benworth Hansen, Jennifer M Hartley, Christian Holm, Alexei Kornyshev, Kevin R J Lovelock, Daniel M Markiewitz, Joshua Maurer, Shurui Miao, Susan Perkin, Frederik Philippi, Bernhard Roling, Nicolas Schaeffer, Monika Schönhoff, David J Sconyers, Neave Taylor, Kazuhide Ueno, Adriaan van den Bruinhorst, Masayoshi Watanabe, Yuki Yamada","doi":"10.1039/d4fd90036g","DOIUrl":"https://doi.org/10.1039/d4fd90036g","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370275","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}

{"title":"New directions in experiment and theory, interfaces, and interactions: general discussion.","authors":"Rob Atkin, Duncan W Bruce, Robert A W Dryfe, Emmanuelle Dubois, Karen J Edler, Christopher E Elgar, Andrew Feeney, Kateryna Goloviznina, Timothy S Groves, Benworth Hansen, John D Holbrey, Christian Holm, Alexei Kornyshev, Claudio J Margulis, Daniel M Markiewitz, Richard P Matthews, Joshua Maurer, Shurui Miao, Frederik Philippi, Elixabete Rezabal, Bernhard Roling, Benjamin Rotenberg, Joshua Sangoro, Monika Schönhoff, John M Slattery, Małgorzata Swadźba-Kwaśny, Neave Taylor, Masayoshi Watanabe, Jake Yang","doi":"10.1039/d4fd90037e","DOIUrl":"https://doi.org/10.1039/d4fd90037e","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142363527","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}

{"title":"Ionic fluids at equilibrium: thermodynamics, nanostructure, phase behaviour, activity: general discussion.","authors":"Andrew P Abbott, Rob Atkin, Duncan W Bruce, Paola Carbone, Giacomo Damilano, Robert A W Dryfe, Jean-Francois Dufrêche, Karen J Edler, Y K Catherine Fung, Kateryna Goloviznina, Margarida Costa Gomes, Alexis Grimaud, Timothy S Groves, Jennifer M Hartley, John D Holbrey, Christian Holm, Pierre Illien, Roland Kjellander, Alexei Kornyshev, Kevin R J Lovelock, Daniel M Markiewitz, Joshua Maurer, Shurui Miao, Naoya Nishi, Beatriz Rocha de Moraes, Bernhard Roling, Benjamin Rotenberg, Joshua Sangoro, Nicolas Schaeffer, Monika Schönhoff, David J Sconyers, John M Slattery, Małgorzata Swadźba-Kwaśny, Adriaan van den Bruinhorst, Tom Welton","doi":"10.1039/d4fd90035a","DOIUrl":"https://doi.org/10.1039/d4fd90035a","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142363526","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}

{"title":"Multi-reference coupled cluster theory using the normal ordered exponential ansatz.","authors":"Alexander D Gunasekera, Nicholas Lee, David P Tew","doi":"10.1039/d4fd00044g","DOIUrl":"https://doi.org/10.1039/d4fd00044g","url":null,"abstract":"<p><p>Properly spin-adapted coupled-cluster theory for general open-shell configurations remains an active area of research in electronic structure theory. In this contribution we examine Lindgren's normal-ordered exponential ansatz to correlate specific spin states using spin-free excitation operators, with the aid of automatic equation generation software. We present an intermediately normalised and size-extensive reformulation of the unlinked working equations, and analyse the performance of the method with single and double excitations for simple molecular systems in terms of accuracy and size-consistency.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142337477","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}

{"title":"Analysis of uncertainty of neural fingerprint-based models.","authors":"Christian W Feldmann, Jochen Sieg, Miriam Mathea","doi":"10.1039/d4fd00095a","DOIUrl":"https://doi.org/10.1039/d4fd00095a","url":null,"abstract":"<p><p>Machine learning has gained popularity for predicting molecular properties based on molecular structure. This study explores the uncertainty estimates of neural fingerprint-based models by comparing pure graph neural networks (GNN) to classical machine learning algorithms combined with neural fingerprints. We investigate the advantage of extracting the neural fingerprint from the GNN and integrating it into a method known for producing better-calibrated probability estimates. Comparisons are made using three classical machine learning methods and the Chemprop model, considering different molecular representations and calibration techniques. We utilize 19 datasets from Toxcast, reflecting real-world scenarios with balanced accuracies ranging from 0.6 to 0.8. Results demonstrate that neural fingerprints combined with classical machine learning methods exhibit a slight decrease in prediction performance compared to the native Chemprop model. However, these models provide significantly improved uncertainty estimates. Notably, uncertainty estimates of neural fingerprint-based methods remain relatively robust for molecules dissimilar to the training set. This suggests that methods like random forest with neural fingerprints can deliver strong prediction performance and reliable uncertainty estimates. When considering both performance and uncertainty, the calibrated Chemprop model and the combination of neural fingerprints with random forest or support vector classifier (SVC) yield comparable results. Surprisingly, the SVC method shows promising performance when combined with neural or count fingerprints. These findings are particularly relevant in real-world industrial projects where accurate predictions and reliable uncertainty estimates are crucial.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142337476","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}

{"title":"Metastable layered lithium-rich niobium and tantalum oxides <i>via</i> nearly instantaneous cation exchange.","authors":"Sarah L Ko, Jordan A Dorrell, Andrew J Morris, Kent J Griffith","doi":"10.1039/d4fd00103f","DOIUrl":"https://doi.org/10.1039/d4fd00103f","url":null,"abstract":"<p><p>Lithium-rich early transition metal oxides are the source of excess removeable lithium that affords high energy density to lithium-rich battery cathodes. They are also candidates for solid electrolytes in all-solid-state batteries. These highly ionic compounds are sparse on phase diagrams of thermodynamically stable oxides, but soft chemical routes offer an alternative to explore new alkali-rich crystal chemistries. In this work, a new layered polymorph of Li₃NbO₄ with coplanar [Nb₄O₁₆]^12- clusters is discovered through ion exchange chemistry. A more detailed study of the ion exchange reaction reveals that it takes place almost instantaneously, changing the crystal volume by more than 22% within seconds. The transformation of coplanar [Nb₄O₁₆]^12- in L-Li₃NbO₄ into the supertetrahedral [Nb₄O₁₆]^12- clusters found in the stable cubic c-Li₃NbO₄ is also explored. Furthermore, this synthetic pathway is extended to access a new layered polymorph of Li₃TaO₄. NMR crystallography with ^6,7Li, ²³Na, and ⁹³Nb NMR, X-ray diffraction, neutron diffraction, and first-principles calculations is applied to A₃MO₄ (A = Li, Na; M = Nb, Ta) to identify local and long-range atomic structure, to monitor the unusually rapid reaction progression, and to track the phase transitions from the metastable layered phases to the known compounds found using high-temperature synthesis. A mechanism is proposed whereby some sodium is retained at short reaction times, which then undergoes proton exchange during water washing, forming a phase with hydrogen bonds bridging the coplanar [Nb₄O₁₆]^12- clusters. This study has implications for lithium-rich transition metal oxides and associated battery materials and for ion exchange chemistry in non-framework structures. The role of techniques that can detect light elements, local structure, and subtle structural changes in soft-chemical synthesis is emphasized.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142277402","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}

{"title":"Preface.","authors":"George H Booth, Ali Alavi","doi":"10.1039/d4fd90033b","DOIUrl":"https://doi.org/10.1039/d4fd90033b","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142277403","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}

{"title":"How to do impactful research in artificial intelligence for chemistry and materials science.","authors":"Alan Aspuru-Guzik, Austin Cheng, Marta Skreta, Cher Tian Ser, Andres Guzman-Cordero, Luca Thiede, Andreas Burger, Sergio Pablo-García, Abdulrahman Aldossary, Shi Xuan Leong, Felix Strieth-Kalthoff","doi":"10.1039/d4fd00153b","DOIUrl":"https://doi.org/10.1039/d4fd00153b","url":null,"abstract":"Machine learning has been pervasively touching many fields of science. Chemistry and materials science are no exception. While machine learning has been making a great impact, it is still not reaching its full potential or maturity. In this perspective, we first outline the pervasive current applications. Then, we discuss how machine learning researchers view and approach problems in the field. Finally, we provide our considerations for maximizing impact when researching machine learning for chemistry.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":null,"pages":null},"PeriodicalIF":3.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142262638","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}