Faraday Discussions最新文献_第9页

Knowledge distillation of neural network potential for molecular crystals† 分子晶体神经网络潜能的知识提炼

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-18 DOI: 10.1039/D4FD00090K

Takuya Taniguchi

{"title":"Knowledge distillation of neural network potential for molecular crystals†","authors":"Takuya Taniguchi","doi":"10.1039/D4FD00090K","DOIUrl":"10.1039/D4FD00090K","url":null,"abstract":"Organic molecular crystals exhibit various functions due to their diverse molecular structures and arrangements. Computational approaches are necessary to explore novel molecular crystals from the material space, but quantum chemical calculations are costly and time-consuming. Neural network potentials (NNPs), trained on vast amounts of data, have recently gained attention for their ability to perform energy calculations with accuracy comparable to quantum chemical methods at high speed. However, NNPs trained on datasets primarily consisting of inorganic crystals, such as the Materials Project, may introduce bias when applied to organic molecular crystals. This study investigates the strategies to improve the accuracy of a pre-trained NNP for organic molecular crystals by distilling knowledge from a teacher model. The most effective knowledge transfer was achieved when fine-tuning using only soft targets, i.e., the teacher model's inference values. As the ratio of hard target loss increased, the efficiency of knowledge transfer decreased, leading to overfitting. As a proof of concept, the NNP created through knowledge distillation was used to predict elastic properties, resulting in improved accuracy compared to the pre-trained model.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"256 ","pages":" 139-155"},"PeriodicalIF":3.4,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00090k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141737507","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Crystal structure validation of verinurad via proton-detected ultra-fast MAS NMR and machine learning† 通过质子检测超快 MAS NMR 和机器学习确定 Verinurad 的晶体结构

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-17 DOI: 10.1039/D4FD00076E

Daria Torodii, Jacob B. Holmes, Pinelopi Moutzouri, Sten O. Nilsson Lill, Manuel Cordova, Arthur C. Pinon, Kristof Grohe, Sebastian Wegner, Okky Dwichandra Putra, Stefan Norberg, Anette Welinder, Staffan Schantz and Lyndon Emsley

引用次数: 0

Atomic-level structure of the amorphous drug atuliflapon via NMR crystallography† 通过核磁共振晶体学研究无定形药物阿托利夫拉朋的原子级结构

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-17 DOI: 10.1039/D4FD00078A

Jacob B. Holmes, Daria Torodii, Martins Balodis, Manuel Cordova, Albert Hofstetter, Federico Paruzzo, Sten O. Nilsson Lill, Emma Eriksson, Pierrick Berruyer, Bruno Simões de Almeida, Mike Quayle, Stefan Norberg, Anna Svensk Ankarberg, Staffan Schantz and Lyndon Emsley

引用次数: 0

Nanoscale visualization of the anti-tumor effect of a plasma-activated Ringer's lactate solution† 等离子激活的林格乳酸盐溶液抗肿瘤效果的纳米级可视化

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-16 DOI: 10.1039/D4FD00116H

Junichi Usuda, Kenshin Yagyu, Hiromasa Tanaka, Masaru Hori, Kenji Ishikawa and Yasufumi Takahashi

{"title":"Nanoscale visualization of the anti-tumor effect of a plasma-activated Ringer's lactate solution†","authors":"Junichi Usuda, Kenshin Yagyu, Hiromasa Tanaka, Masaru Hori, Kenji Ishikawa and Yasufumi Takahashi","doi":"10.1039/D4FD00116H","DOIUrl":"10.1039/D4FD00116H","url":null,"abstract":"Plasma-activated Ringer's lactate solutions (PALs), which are Ringer's lactate solutions treated with non-thermal atmospheric-pressure plasma, have an anti-tumor effect and can be used for chemotherapy. As the anti-tumor effect of the PAL is influenced by the cell-treatment time, it is necessary to monitor the structural changes of the cell surface with non-invasive, nanoscale, and time-lapse imaging to understand the anti-tumor effect. In this study, to characterize the anti-tumor effect of the PAL, we used scanning ion conductance microscopy (SICM), using glass nanopipettes as probes, to visualize the structural changes of the cell surface. SICM time-lapse topographic imaging visualized a decrease in the movement of lamellipodia in normal cells and cancer cells after the PAL treatment. Furthermore, in normal cells, protrusive structures were observed on the cell surface. Time-lapse imaging using SICM allowed us to characterize the differences in the morphological changes between the normal and cancer cells upon exposure to the PAL.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 212-223"},"PeriodicalIF":3.4,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00116h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141719551","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Embedding human knowledge in material screening pipeline as filters to identify novel synthesizable inorganic materials 将人类知识嵌入材料筛选管道，作为识别新型可合成无机材料的过滤器

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-16 DOI: 10.1039/D4FD00120F

Basita Das, Kangyu Ji, Fang Sheng, Kyle M. McCall and Tonio Buonassisi

{"title":"Embedding human knowledge in material screening pipeline as filters to identify novel synthesizable inorganic materials","authors":"Basita Das, Kangyu Ji, Fang Sheng, Kyle M. McCall and Tonio Buonassisi","doi":"10.1039/D4FD00120F","DOIUrl":"10.1039/D4FD00120F","url":null,"abstract":"How might one embed a chemist's knowledge into an automated materials-discovery pipeline? In generative design for inorganic crystalline materials, generating candidate compounds is no longer a bottleneck – there are now synthetic datasets of millions of compounds. However, weeding out unsynthesizable or difficult to synthesize compounds remains an outstanding challenge. Post-generation “filters” have been proposed as a means of embedding human domain knowledge, either in the form of scientific laws or rules of thumb. Examples include charge neutrality, electronegativity balance, and energy above hull. Some filters are “hard” and some are “soft” — for example, it is difficult to envision creating a stable compound while violating the rule of charge neutrality; however, several compounds break the Hume-Rothery rules. It is therefore natural to wonder: can one compile a comprehensive list of “filters” that embed domain knowledge, adopt a principled approach to classifying them as either non-conditional or conditional “filters,” and envision a software environment to implement combinations of these in a systematic manner? In this commentary we explore such questions, “filters” for screening of novel inorganic compounds for synthesizability.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"256 ","pages":" 587-600"},"PeriodicalIF":3.4,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00120f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141719553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Exploring the crystallisation of aspirin in a confined porous material using solid-state nuclear magnetic resonance† 利用固态核磁共振探索阿司匹林在密闭多孔材料中的结晶过程

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-16 DOI: 10.1039/D4FD00123K

Marie Juramy, Eric Besson, Stéphane Gastaldi, Fabio Ziarelli, Stéphane Viel, Giulia Mollica and Pierre Thureau

引用次数: 0

Scanning electrochemical probe microscopy: towards the characterization of micro- and nanostructured photocatalytic materials† 扫描电化学探针显微镜：表征微纳米结构的光催化材料

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-15 DOI: 10.1039/D4FD00136B

Giada Caniglia, Sarah Horn and Christine Kranz

{"title":"Scanning electrochemical probe microscopy: towards the characterization of micro- and nanostructured photocatalytic materials†","authors":"Giada Caniglia, Sarah Horn and Christine Kranz","doi":"10.1039/D4FD00136B","DOIUrl":"10.1039/D4FD00136B","url":null,"abstract":"Platinum-black (Pt-B) has been demonstrated to be an excellent electrocatalytic material for the electrochemical oxidation of hydrogen peroxide (H2O2). As Pt-B films can be deposited electrochemically, micro- and nano-sized conductive transducers can be modified with Pt-B. Here, we present the potential of Pt-B micro- and sub-micro-sized sensors for the detection and quantification of hydrogen (H2) in solution. Using these microsensors, no sampling step for H2 determination is required and e.g., in photocatalysis, the onset of H2 evolution can be monitored in situ. We present Pt-B-based H2 micro- and sub-micro-sized sensors based on different electrochemical transducers such as microelectrodes and atomic force microscopy (AFM)-scanning electrochemical microscopy (SECM) probes, which enable local measurements e.g., at heterogenized photocatalytically active samples. The microsensors are characterized in terms of limits of detection (LOD), which ranges from 4.0 μM to 30 μM depending on the size of the sensors and the experimental conditions such as type of electrolyte and pH. The sensors were tested for the in situ H2 evolution by light-driven water-splitting, i.e., using ascorbic acid or triethanolamine solutions, showing a wide linear concentration range, good reproducibility, and high sensitivity. Proof-of-principle experiments using Pt-B-modified cantilever-based sensors were performed using a model sample platinum substrate to map the electrochemical H2 evolution along with the topography using AFM-SECM.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 224-239"},"PeriodicalIF":3.4,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00136b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141719554","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Indigo production identifies hotspots in cytochrome P450 BM3 for diversifying aromatic hydroxylation† 靛蓝生产确定了细胞色素 P450 BM3 中芳香烃羟化多样化的热点。

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-12 DOI: 10.1039/D4FD00017J

Douglas J. Fansher, Jonathan N. Besna and Joelle N. Pelletier

{"title":"Indigo production identifies hotspots in cytochrome P450 BM3 for diversifying aromatic hydroxylation†","authors":"Douglas J. Fansher, Jonathan N. Besna and Joelle N. Pelletier","doi":"10.1039/D4FD00017J","DOIUrl":"10.1039/D4FD00017J","url":null,"abstract":"Evolution of P450 BM3 is a topic of extensive research, but screening the various substrate/reaction combinations remains a time-consuming process. Indigo production has the potential to serve as a simple high-throughput method for reaction screening, as bacterial colonies expressing indigo (+) variants can be visually identified via their blue phenotype. Indigo (+) single variants, indigo (−) single variants and a combinatorial library, containing mutations that enable the blue phenotype, were screened for their ability to hydroxylate a panel of 12 aromatic compounds using the 4-aminoantipyrine colorimetric assay. Recombination of indigo (+) single variants to create a multiple-variant library is a particularly useful strategy, as all top performing P450 BM3 variants with high hydroxylation activity were either indigo (+) single variants or contained multiple substitutions. Furthermore, active variants, as determined using the 4-AAP assay, were further characterized and several variants were identified that gave more than 90% conversion with 1,3-dichlorobenzene and predominantly formed 2,6-dichlorophenol; other variants showed significant substrate selectivity. This supports the hypothesis that substitution at positions that enable the indigo (+) phenotype, or hotspot residues, is a general mechanism for increasing aromatic hydroxylation activity. Overall, this research demonstrates that indigo (+) single variants, identified via colorimetric colony-based screening, may be recombined to generate a multiply-substituted variant library containing many variants with high aromatic hydroxylation activity. The combination of colony-based screening and other screening assays greatly accelerates enzyme engineering, as readily-identified indigo (+) single variants can be recombined to create a library of active multiple variants without extensive screening of single variants.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"252 ","pages":" 29-51"},"PeriodicalIF":3.4,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141588953","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}

引用次数: 0

Spiers Memorial Lecture: Quantum chemistry, classical heuristics, and quantum advantage 量子化学、经典启发法和量子优势

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-11 DOI: 10.1039/D4FD00141A

Garnet Kin-Lic Chan

引用次数: 0

Concluding remarks: Reflections on the Faraday Discussion on New Directions in Molecular Scattering 结束语：对法拉第分子散射新方向讨论的思考

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-11 DOI: 10.1039/D4FD00118D

Mark Brouard

引用次数: 0