Pub Date : 2025-02-25DOI: 10.1016/j.cplett.2025.142004
Qiang Guo, Jianhong Liu, Cunqin Lv
Hydrogen generation via ammonia decomposition is a highly promising method. Density functional theory (DFT) calculations were performed to explore the adsorption and decomposition of NH3 on various sub layer Ru doped Ni(100) surfaces. It was found that the doping of Ru atoms reduces the total potential energy of the ammonia decomposition process and improves the catalytic activity. In terms of the energy barrier, the doping of Ru atoms is more conducive to the activation of the N−H bond in NH₂. Moreover, we investigated the effect of specific surface area and surface coverage on catalytic activity. It was found that reasonable specific surface area and modulation of N coverage both optimize the activity of the catalysts.
{"title":"Theoretical study of ammonia decomposition mechanism on RuNi bimetallic catalysts using density functional theory","authors":"Qiang Guo, Jianhong Liu, Cunqin Lv","doi":"10.1016/j.cplett.2025.142004","DOIUrl":"10.1016/j.cplett.2025.142004","url":null,"abstract":"<div><div>Hydrogen generation via ammonia decomposition is a highly promising method. Density functional theory (DFT) calculations were performed to explore the adsorption and decomposition of NH<sub>3</sub> on various sub layer Ru doped Ni(100) surfaces. It was found that the doping of Ru atoms reduces the total potential energy of the ammonia decomposition process and improves the catalytic activity. In terms of the energy barrier, the doping of Ru atoms is more conducive to the activation of the N−H bond in NH₂. Moreover, we investigated the effect of specific surface area and surface coverage on catalytic activity. It was found that reasonable specific surface area and modulation of N coverage both optimize the activity of the catalysts.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 142004"},"PeriodicalIF":2.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143534150","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}
Pub Date : 2025-02-24DOI: 10.1016/j.cplett.2025.141991
Xinyu Jiang , Yishu Wang , Bohan Wang , Meiheng Lv , Huaxin Liu , Yinhua Ma , Fangjian Shang , Wenze Li
In this study, the density functional theory (DFT) and time-dependent density functional theory (TDDFT) methods were used to theoretically study the recognition and fluorescence mechanism of a newly reported efficient H2S probe. The recognition mechanism was determined to be between the probe DTHP and HS−. According to the results of FMO and LIIC analyses, the activation of fluorescence is attributed to the inhibition of TICT process, and its rationality is further confirmed from the fluorescence properties of the recognized products.
{"title":"A theoretical perspective on the sensing mechanism of a 7-hydroxy-4-methylcoumarin based fluorescence probe for H2S detection","authors":"Xinyu Jiang , Yishu Wang , Bohan Wang , Meiheng Lv , Huaxin Liu , Yinhua Ma , Fangjian Shang , Wenze Li","doi":"10.1016/j.cplett.2025.141991","DOIUrl":"10.1016/j.cplett.2025.141991","url":null,"abstract":"<div><div>In this study, the density functional theory (DFT) and time-dependent density functional theory (TDDFT) methods were used to theoretically study the recognition and fluorescence mechanism of a newly reported efficient H<sub>2</sub>S probe. The recognition mechanism was determined to be between the probe DTHP and HS<sup>−</sup>. According to the results of FMO and LIIC analyses, the activation of fluorescence is attributed to the inhibition of TICT process, and its rationality is further confirmed from the fluorescence properties of the recognized products.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141991"},"PeriodicalIF":2.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143534135","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}
Pub Date : 2025-02-23DOI: 10.1016/j.cplett.2025.141990
Li Zhao, Renchao Che
Nitrous acid (HONO) is a crucial atmospheric precursor to hydroxyl radicals, originating from the photolysis of o-nitrophenol. Understanding the photochemistry of o-nitrophenol is essential due to its significant role in atmospheric chemistry and its impact on air quality and climate. This study investigates the excited-state dynamics of photoexcited o-nitrophenol using high-level electronic structure calculations and on-the-fly surface hopping simulations. We identified three minimum energy conical intersections (MECIs) that facilitate the internal conversion (IC) process from the first excited singlet state (S1) to the ground state (S0). The surface hopping simulations reveal three distinct decay pathways: two involve significant excited-state intramolecular proton transfer (ESIPT) processes occurring on a timescale of 52 fs, consistent with experimental observations, and the third one involves rotational motion around the C5-N1 bond.
{"title":"Internal conversion pathways in the deactivation of o-Nitrophenol in the gas phase","authors":"Li Zhao, Renchao Che","doi":"10.1016/j.cplett.2025.141990","DOIUrl":"10.1016/j.cplett.2025.141990","url":null,"abstract":"<div><div>Nitrous acid (HONO) is a crucial atmospheric precursor to hydroxyl radicals, originating from the photolysis of o-nitrophenol. Understanding the photochemistry of o-nitrophenol is essential due to its significant role in atmospheric chemistry and its impact on air quality and climate. This study investigates the excited-state dynamics of photoexcited o-nitrophenol using high-level electronic structure calculations and on-the-fly surface hopping simulations. We identified three minimum energy conical intersections (MECIs) that facilitate the internal conversion (IC) process from the first excited singlet state (S<sub>1</sub>) to the ground state (S<sub>0</sub>). The surface hopping simulations reveal three distinct decay pathways: two involve significant excited-state intramolecular proton transfer (ESIPT) processes occurring on a timescale of 52 fs, consistent with experimental observations, and the third one involves rotational motion around the C5-N1 bond.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141990"},"PeriodicalIF":2.8,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143519215","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}
Nanofluids exhibit enhanced thermal conductivity over conventional fluids. Modification of nanoparticle surfaces with distinct chemical properties (Janus particles) can improve thermal conductivity. Using molecular dynamics, we examined how wetting balances of Janus particles impact thermal conductivity. Our results demonstrate that Janus particles can enhance thermal conductivity more than homogeneous nanoparticles. Interestingly, the excess wetting surface area decreases the enhancement. Structural analysis reveals this change in thermal conductivity correlates with the density of solvents in the interfacial layer around the nanoparticle. Moreover, the dynamics of the nanoparticle do not enhance the thermal conductivity under homogeneous temperature fields.
{"title":"Effect of Janus balance on the thermal conductivity of nanofluid","authors":"Takahiro Ikeda , Yusei Kobayashi , Masashi Yamakawa","doi":"10.1016/j.cplett.2025.141969","DOIUrl":"10.1016/j.cplett.2025.141969","url":null,"abstract":"<div><div>Nanofluids exhibit enhanced thermal conductivity over conventional fluids. Modification of nanoparticle surfaces with distinct chemical properties (Janus particles) can improve thermal conductivity. Using molecular dynamics, we examined how wetting balances of Janus particles impact thermal conductivity. Our results demonstrate that Janus particles can enhance thermal conductivity more than homogeneous nanoparticles. Interestingly, the excess wetting surface area decreases the enhancement. Structural analysis reveals this change in thermal conductivity correlates with the density of solvents in the interfacial layer around the nanoparticle. Moreover, the dynamics of the nanoparticle do not enhance the thermal conductivity under homogeneous temperature fields.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141969"},"PeriodicalIF":2.8,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143478822","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}
Pub Date : 2025-02-22DOI: 10.1016/j.cplett.2025.141989
Jiacheng Ding , Yandong Che , Meixia Zhang , Lingru Kong , Tõnu Pullerits , Yanqiu Yang , Peng Song
Surface-enhanced Raman scattering (SERS) technology can detect molecular information; Because of its high sensitivity, it is widely used in chemical analysis. In this study discussed the experimental detection of 1,4-diethynylbenzene molecule based on SERS technology. The SERS spectra of 1,4-diethynylbenzene molecule were calculated by Density Functional Theory (DFT) simulation, and the results showed that SERS could efficiently detect 1,4-diethynylbenzene molecule. In addition, the frontal molecular orbitals and electrostatic potential distributions of 1,4-diethynylbenzene and Ag3–1,4-diethynylbenzene molecules were simulated and calculated by DFT, respectively, and the dock mode of Ag3 cluster and 1,4-diethynylbenzene molecules was discussed.
{"title":"Revealing the 1,4-diethynylbenzene SERS activity and docking studies by DFT","authors":"Jiacheng Ding , Yandong Che , Meixia Zhang , Lingru Kong , Tõnu Pullerits , Yanqiu Yang , Peng Song","doi":"10.1016/j.cplett.2025.141989","DOIUrl":"10.1016/j.cplett.2025.141989","url":null,"abstract":"<div><div>Surface-enhanced Raman scattering (SERS) technology can detect molecular information; Because of its high sensitivity, it is widely used in chemical analysis. In this study discussed the experimental detection of 1,4-diethynylbenzene molecule based on SERS technology. The SERS spectra of 1,4-diethynylbenzene molecule were calculated by Density Functional Theory (DFT) simulation, and the results showed that SERS could efficiently detect 1,4-diethynylbenzene molecule. In addition, the frontal molecular orbitals and electrostatic potential distributions of 1,4-diethynylbenzene and Ag3–1,4-diethynylbenzene molecules were simulated and calculated by DFT, respectively, and the dock mode of Ag3 cluster and 1,4-diethynylbenzene molecules was discussed.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141989"},"PeriodicalIF":2.8,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510524","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}
Pub Date : 2025-02-22DOI: 10.1016/j.cplett.2025.141992
Sai Zhang, Yutong Han, Yuning Wang, Suochen Lu, Xingzhu Tang, Chaofan Sun
By adopting the density functional theory (DFT) and time-dependent density functional theory (TD-DFT) methods, the excited state intramolecular charge transfer (ESIPT) processes and photophysical properties of 3-OHPht-Pyr and 3-OHPht-Iquin with different substituents (pyridine and isoquinoline) are studied. The results indicate that 3-OHPht-Pyr is more prone to the ESIPT process accompanied by molecular twisting compared to 3-OHPht-Iquin. Moreover, the differences in twisting angles and trends result in the differences of the fluorescence peaks of the two molecules. It is worth noting that the Stokes shifts of the two molecules can reach 170 nm and 220 nm, respectively.
{"title":"Photophysical properties of 3-hydroxyphthalimide fluorophores based on the ESIPT mechanism: A theoretical study","authors":"Sai Zhang, Yutong Han, Yuning Wang, Suochen Lu, Xingzhu Tang, Chaofan Sun","doi":"10.1016/j.cplett.2025.141992","DOIUrl":"10.1016/j.cplett.2025.141992","url":null,"abstract":"<div><div>By adopting the density functional theory (DFT) and time-dependent density functional theory (TD-DFT) methods, the excited state intramolecular charge transfer (ESIPT) processes and photophysical properties of 3-OHPht-Pyr and 3-OHPht-Iquin with different substituents (pyridine and isoquinoline) are studied. The results indicate that 3-OHPht-Pyr is more prone to the ESIPT process accompanied by molecular twisting compared to 3-OHPht-Iquin. Moreover, the differences in twisting angles and trends result in the differences of the fluorescence peaks of the two molecules. It is worth noting that the Stokes shifts of the two molecules can reach 170 nm and 220 nm, respectively.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141992"},"PeriodicalIF":2.8,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143478823","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}
Iodates are key in laser technology due to their optical properties. Using first-principles calculations, we studied the electronic structures and optical properties of orthorhombic and triclinic Pb(IO3)2. Both phases show moderate birefringence (0.094 and 0.124@1064 nm). Analysis reveals that birefringence originates from IO3 groups with stereochemically active lone pairs. Furthermore, spin-orbit coupling (SOC) from Pb and I atoms alters electronic structures, reducing birefringence to 0.073 and 0.107@1064 nm. Using the “downshifting of conduction band” and “screening SOC with special atoms” strategies, this study reveals that SOC induced changes in band splitting by lead atoms are crucial in reducing birefringence.
{"title":"The birefringence in orthorhombic and triclinic lead-iodates and the functional basic units' contribution: A first-principles investigation","authors":"Jialong Wang, Enshen Wang, Xiuhua Cui, Peng Li, Qun Jing, Zhaohui Chen","doi":"10.1016/j.cplett.2025.141987","DOIUrl":"10.1016/j.cplett.2025.141987","url":null,"abstract":"<div><div>Iodates are key in laser technology due to their optical properties. Using first-principles calculations, we studied the electronic structures and optical properties of orthorhombic and triclinic Pb(IO<sub>3</sub>)<sub>2</sub>. Both phases show moderate birefringence (0.094 and 0.124@1064 nm). Analysis reveals that birefringence originates from IO<sub>3</sub> groups with stereochemically active lone pairs. Furthermore, spin-orbit coupling (SOC) from Pb and I atoms alters electronic structures, reducing birefringence to 0.073 and 0.107@1064 nm. Using the <em>“downshifting of conduction band”</em> and “screening SOC with special atoms” strategies, this study reveals that SOC induced changes in band splitting by lead atoms are crucial in reducing birefringence.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141987"},"PeriodicalIF":2.8,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143511758","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}
The mechanisms and origins of ligand-controlled Rh(I)-catalyzed CC activation of benzocyclobutenones and their coupling with pendant dienamides were investigated using DFT. This study specifically examined the pathways and factors influencing product formation, with particular emphasis on the role of phosphine ligands. Triphenylphosphine (PPh3) facilitates the formation of the type-II [4 + 4] product, anti-Bredt benzofused aza-bicyclo[5.3.1] bridged compound. Conversely, the bidentate diphosphate ligand 1,3-bis(diphenylphosphino)propane (dppp) introduces significant steric hindrance, which promotes the formation of alternative fused tricycle product.
{"title":"Theoretical investigation of the CC bond activation mechanism of benzocyclobutenones and dienamides catalyzed by Rh(I): The ligand-controlled products selectivity","authors":"Xin Xiang, Wei Wei, Zeng-Xia Zhao, Hong-Xing Zhang","doi":"10.1016/j.cplett.2025.141979","DOIUrl":"10.1016/j.cplett.2025.141979","url":null,"abstract":"<div><div>The mechanisms and origins of ligand-controlled Rh(I)-catalyzed C<img>C activation of benzocyclobutenones and their coupling with pendant dienamides were investigated using DFT. This study specifically examined the pathways and factors influencing product formation, with particular emphasis on the role of phosphine ligands. Triphenylphosphine (<strong>PPh</strong><sub><strong>3</strong></sub>) facilitates the formation of the type-II [4 + 4] product, anti-Bredt benzofused aza-bicyclo[5.3.1] bridged compound. Conversely, the bidentate diphosphate ligand 1,3-bis(diphenylphosphino)propane (<strong>dppp</strong>) introduces significant steric hindrance, which promotes the formation of alternative fused tricycle product.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"866 ","pages":"Article 141979"},"PeriodicalIF":2.8,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143480329","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}
Pub Date : 2025-02-19DOI: 10.1016/j.cplett.2025.141984
Ziqi Zhong , Borui Du , Guowu Zhan , Jingran Xiao
Herein, the 3D printing technology is harnessed as a new and flexible strategy to fabricate a structural-parameter adjustable 3D-structured Ti-Fe2O3 photoanode. The Ti alloy was discovered to be practicable during the synthesis of Ti-Fe2O3 and enlisted as a substrate material for crafting a conical-array patterned Ti-Fe2O3 photoanode. The conical array fashions an angle between the incident light (longitudinal side) and the photogenerated charge transport (transverse side), along with a considerably augmented light-receiving area. Significantly, the charge separation efficiency progressively escalates as the cone height augments. This undertaking accentuates the importance of modulating the parameter of a 3D-structured Fe2O3 photoanode.
{"title":"3D-printed Ti-Fe2O3 photoanode with conical array for enhanced photoelectrochemical water splitting","authors":"Ziqi Zhong , Borui Du , Guowu Zhan , Jingran Xiao","doi":"10.1016/j.cplett.2025.141984","DOIUrl":"10.1016/j.cplett.2025.141984","url":null,"abstract":"<div><div>Herein, the 3D printing technology is harnessed as a new and flexible strategy to fabricate a structural-parameter adjustable 3D-structured Ti-Fe<sub>2</sub>O<sub>3</sub> photoanode. The Ti alloy was discovered to be practicable during the synthesis of Ti-Fe<sub>2</sub>O<sub>3</sub> and enlisted as a substrate material for crafting a conical-array patterned Ti-Fe<sub>2</sub>O<sub>3</sub> photoanode. The conical array fashions an angle between the incident light (longitudinal side) and the photogenerated charge transport (transverse side), along with a considerably augmented light-receiving area. Significantly, the charge separation efficiency progressively escalates as the cone height augments. This undertaking accentuates the importance of modulating the parameter of a 3D-structured Fe<sub>2</sub>O<sub>3</sub> photoanode.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141984"},"PeriodicalIF":2.8,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463676","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}
Pub Date : 2025-02-18DOI: 10.1016/j.cplett.2025.141964
Oz Y. Mendelsohn , Michal Hartstein , Stefan Chmiela , Alexandre Tkatchenko , Leeor Kronik
Halide perovskites (HaPs) have emerged as promising new materials for a wide range of optoelectronic applications, notably solar energy conversion. These materials are well known to exhibit significant dynamical effects even at room temperature, which affect both their electronic properties and their long-term stability. Molecular dynamics (MD) simulations can provide significant insights into such effects. However, long time scale simulations require both accuracy and scalability. The latter is an issue for first principles methods and the former is challenging for classical force fields. Machine-learned force fields (MLFF) are a promising avenue for bridging across this seeming contradiction. Here, we apply the gradient-domain machine learning approach, using CsPbBr as an example. We find that training based on room temperature density functional theory (DFT) data fails to generate an MLFF that provides long-term stable MD, owing to an insufficient sampling of rare events in the training set. We show that this problem is resolved by using a temperature ensemble (TE) method, which can be generated in parallel and yields a combined data set based on MD trajectories from a variety of temperatures. The MLFF model based on the TE method yields high accuracy for long-term simulations, showing remaining errors of the same magnitude of inherent errors in the DFT calculation.
{"title":"Stable molecular dynamics simulations of halide perovskites from a temperature-ensemble gradient-domain machine learning approach","authors":"Oz Y. Mendelsohn , Michal Hartstein , Stefan Chmiela , Alexandre Tkatchenko , Leeor Kronik","doi":"10.1016/j.cplett.2025.141964","DOIUrl":"10.1016/j.cplett.2025.141964","url":null,"abstract":"<div><div>Halide perovskites (HaPs) have emerged as promising new materials for a wide range of optoelectronic applications, notably solar energy conversion. These materials are well known to exhibit significant dynamical effects even at room temperature, which affect both their electronic properties and their long-term stability. Molecular dynamics (MD) simulations can provide significant insights into such effects. However, long time scale simulations require both accuracy and scalability. The latter is an issue for first principles methods and the former is challenging for classical force fields. Machine-learned force fields (MLFF) are a promising avenue for bridging across this seeming contradiction. Here, we apply the gradient-domain machine learning approach, using CsPbBr<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span> as an example. We find that training based on room temperature density functional theory (DFT) data fails to generate an MLFF that provides long-term stable MD, owing to an insufficient sampling of rare events in the training set. We show that this problem is resolved by using a temperature ensemble (TE) method, which can be generated in parallel and yields a combined data set based on MD trajectories from a variety of temperatures. The MLFF model based on the TE method yields high accuracy for long-term simulations, showing remaining errors of the same magnitude of inherent errors in the DFT calculation.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"867 ","pages":"Article 141964"},"PeriodicalIF":2.8,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510396","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}
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