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Ligand field exciton annihilation in bulk CrCl3 块状 CrCl3 中的配体场激子湮灭
The Journal of Chemical Physics Pub Date : 2024-09-18 DOI: 10.1063/5.0223772
Samanvitha Sridhar, Ario Khansari, Shaun O’Donnell, Alexandra T. Barth, Evgeny O. Danilov, Felix N. Castellano, Paul A. Maggard, Daniel B. Dougherty
{"title":"Ligand field exciton annihilation in bulk CrCl3","authors":"Samanvitha Sridhar, Ario Khansari, Shaun O’Donnell, Alexandra T. Barth, Evgeny O. Danilov, Felix N. Castellano, Paul A. Maggard, Daniel B. Dougherty","doi":"10.1063/5.0223772","DOIUrl":"https://doi.org/10.1063/5.0223772","url":null,"abstract":"The layered van der Waals material CrCl3 exhibits very strongly bound ligand field excitons that control optoelectronic applications and are connected with magnetic ordering by virtue of their d-orbital origin. Time-resolved photoluminescence of these exciton populations at room temperature shows that their relaxation is dominated by exciton–exciton annihilation and that the spontaneous decay lifetime is very long. These observations allow the rough quantification of the exciton annihilation rate constant and contextualization in light of a recent theory of universal scaling behavior of the annihilation process.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"17 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cluster intercalation of aluminum tetrachloride in AlN cathode: Exploration and analysis of aluminum ion batteries 氮化铝阴极中的四氯化铝簇插层：铝离子电池的探索与分析
The Journal of Chemical Physics Pub Date : 2024-09-18 DOI: 10.1063/5.0219080
Shanshan He, Leilei Li, Yijin Wu, Shan He, Donghui Guo
{"title":"Cluster intercalation of aluminum tetrachloride in AlN cathode: Exploration and analysis of aluminum ion batteries","authors":"Shanshan He, Leilei Li, Yijin Wu, Shan He, Donghui Guo","doi":"10.1063/5.0219080","DOIUrl":"https://doi.org/10.1063/5.0219080","url":null,"abstract":"When chloroaluminate (AlCl4−) serves as the electrolyte, aluminum nitride (AlN) has shown promise as a cathode material in aluminum ion batteries. However, there is currently a lack of research on the mechanisms of charge transfer and cluster intercalation between AlCl4 and AlN cathode materials. Herein, first-principles calculations are employed to investigate the intercalation mechanism of AlCl4 within the AlN cathode. By calculating the formation energies of stage-1–5 AlN–AlCl4 intercalation compounds with the insertion of individual AlCl4 cluster, we found that the structure of the stage-4 intercalation compounds exhibits the highest stability, suggesting that when the clusters begin to intercalate, it is important to start with the formation of the stage-4 intercalation compounds. In the subsequent phases of the charging process (stages 1 and 2), the stabilized structure with four inserted clusters demonstrates two characteristics: the coexistence of standing and lying clusters and the insertion of two standing clusters in an upside-down doubly stacked configuration, which further improve the spatial utilization while maintaining the structural stability. In addition, we infer that a phenomenon of coexisting intercalation compounds with mixed stages will occur in the course of the charging and discharging processes. More importantly, the diffusion barrier of AlCl4 in AlN–AlCl4 intercalation compounds decreases with the reduction of stage number, ensuring the rate performance of batteries. Therefore, we expect that our work will contribute to comprehend the intercalation mechanism of AlCl4 into the AlN cathode materials of aluminum ion batteries, providing guidance for related experimental work.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"86 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
From disorder to order: A dynamic approach to mesophase formation in soft sphere model 从无序到有序：软球模型中介相形成的动态方法
The Journal of Chemical Physics Pub Date : 2024-09-17 DOI: 10.1063/5.0224154
María Victoria Uranga Wassermann, Ezequiel R. Soulé, Cristian Balbuena
{"title":"From disorder to order: A dynamic approach to mesophase formation in soft sphere model","authors":"María Victoria Uranga Wassermann, Ezequiel R. Soulé, Cristian Balbuena","doi":"10.1063/5.0224154","DOIUrl":"https://doi.org/10.1063/5.0224154","url":null,"abstract":"This study explores the dynamics of self-assembly and mesophase formation through molecular dynamics simulations of hexagonal and lamellar systems using a simplified coarse-grained model. We focus on characterizing the order–disorder transitions driven by temperature variations and emphasize the often overlooked disordered regime, which serves as a precursor to periodic mesoscale ordering. Our findings not only underscore the morphological richness of the disordered regime, comparable to that of its periodic counterparts, but also reveal the presence of clustering regimes within isotropic phases, thus corroborating prior experimental and theoretical observations. By employing the dynamic correlation coefficient, this work introduces a novel approach to understanding the fundamental mechanisms of mesophase formation, providing new insights into the complex dynamics of self-assembly.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"43 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260504","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling hidden dynamic correlations in CASSCF correlation energies by Hartree–Fock nodes 通过哈特里-福克节点揭示 CASSCF 相关能中隐藏的动态相关性
The Journal of Chemical Physics Pub Date : 2024-09-17 DOI: 10.1063/5.0223733
Martin Šulka, Katarína Šulková, Matúš Dubecký
{"title":"Unveiling hidden dynamic correlations in CASSCF correlation energies by Hartree–Fock nodes","authors":"Martin Šulka, Katarína Šulková, Matúš Dubecký","doi":"10.1063/5.0223733","DOIUrl":"https://doi.org/10.1063/5.0223733","url":null,"abstract":"We have recently introduced an original method for sharply partitioning the correlation energy into dynamic and non-dynamic contributions. This method is based on the node of the Hartree–Fock (HF) Slater determinant and the stochastic projector fixed-node diffusion Monte Carlo (FNDMC) method [Šulka et al., J. Chem. Theory Comput. 19, 8147 (2023)]. This approach addresses the challenge of dissecting correlation energy in quantum chemistry. Here, we present the first application of this technique to explore CASSCF correlation energy contributions in selected molecular systems such as BH, FH, F2, and H2–H2. The results show that correlation energies derived from the full-valence active space CASSCF method, often believed to describe mostly non-dynamic correlation effects, contain an extraneous, unwanted, system-dependent component that belongs to the dynamic correlation energy. The findings suggest that the new HF-node/FNDMC-based electron correlation energy decomposition method provides a useful complementary tool, enabling the detection of inherent challenges in distinguishing between dynamic and non-dynamic contributions to correlation energies within methods where precise dissection of these effects is not possible.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"3 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260507","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Kohn–Sham fragment energy decomposition analysis Kohn-Sham 碎片能量分解分析
The Journal of Chemical Physics Pub Date : 2024-09-13 DOI: 10.1063/5.0216596
Tommaso Giovannini
{"title":"Kohn–Sham fragment energy decomposition analysis","authors":"Tommaso Giovannini","doi":"10.1063/5.0216596","DOIUrl":"https://doi.org/10.1063/5.0216596","url":null,"abstract":"We introduce the concept of Kohn–Sham fragment localized molecular orbitals (KS-FLMOs), which are Kohn–Sham molecular orbitals (MOs) localized in specific fragments constituting a generic molecular system. In detail, we minimize the local electronic energies of various fragments, while maximizing the repulsion between them, resulting in the effective localization of the MOs. We use the developed KS-FLMOs to propose a novel energy decomposition analysis, which we name Kohn–Sham fragment energy decomposition analysis, which allows for rationalizing the main non-covalent interactions occurring in interacting systems both in vacuo and in solution, providing physical insights into non-covalent interactions. The method is validated against state-of-the-art energy decomposition analysis techniques and with high-level calculations.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"43 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260510","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Active string fluids and gels formed by dipolar active Brownian particles in 3D 三维双极活性布朗粒子形成的活性弦流体和凝胶体
The Journal of Chemical Physics Pub Date : 2024-09-13 DOI: 10.1063/5.0215545
Maria Kelidou, Mohammad Fazelzadeh, Baptiste Parage, Marinde van Dijk, Twan Hooijschuur, Sara Jabbari-Farouji
{"title":"Active string fluids and gels formed by dipolar active Brownian particles in 3D","authors":"Maria Kelidou, Mohammad Fazelzadeh, Baptiste Parage, Marinde van Dijk, Twan Hooijschuur, Sara Jabbari-Farouji","doi":"10.1063/5.0215545","DOIUrl":"https://doi.org/10.1063/5.0215545","url":null,"abstract":"Self-propelled particles possessing permanent magnetic dipole moments occur naturally in magnetotactic bacteria and can be built into man-made systems such as active colloids or micro-robots. Yet, the interplay between self-propulsion and anisotropic dipole–dipole interactions on dynamic self-assembly in three dimensions (3D) remains poorly understood. We conduct Brownian dynamics simulations of active dipolar particles in 3D, focusing on the low-density regime, where dipolar hard spheres tend to form chain-like aggregates and percolated networks with increasing dipolar coupling strength. We find that strong active forces override dipolar attractions, effectively inhibiting chain-like aggregation and network formation. Conversely, activating particles with low to moderate forces results in a fluid composed of active chains and rings. At strong dipolar coupling strengths, this active fluid transitions into an active gel, consisting of a percolated network of active chains. Although the overall structure of the active gel remains interconnected, the network experiences more frequent configurational rearrangements due to the reduced bond lifetime of active dipolar particles. Consequently, particles exhibit enhanced translational and rotational diffusion within the active fluid of strings and active gels compared to their passive counterparts. We quantify the influence of activity on aggregate topology as they transition from branched structures to unconnected chains and rings. Our findings are summarized in a state diagram, delineating the impact of dipolar coupling strength and active force magnitude on the system.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"207 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260512","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Non-equilibrium rate theory for polariton relaxation dynamics 极化子弛豫动力学的非平衡速率理论
The Journal of Chemical Physics Pub Date : 2024-09-13 DOI: 10.1063/5.0231396
Yifan Lai, Wenxiang Ying, Pengfei Huo
{"title":"Non-equilibrium rate theory for polariton relaxation dynamics","authors":"Yifan Lai, Wenxiang Ying, Pengfei Huo","doi":"10.1063/5.0231396","DOIUrl":"https://doi.org/10.1063/5.0231396","url":null,"abstract":"We derive an analytic expression of the non-equilibrium Fermi’s golden rule (NE-FGR) expression for a Holstein–Tavis–Cumming Hamiltonian, a universal model for many molecules collectively coupled to the optical cavity. These NE-FGR expressions capture the full-time-dependent behavior of the rate constant for transitions from polariton states to dark states. The rate is shown to be reduced to the well-known frequency domain-based equilibrium Fermi’s golden rule (E-FGR) expression in the equilibrium and collective limit and is shown to retain the same scaling with the number of sites in non-equilibrium and non-collective cases. We use these NE-FGR to perform population dynamics with a time-non-local and time-local quantum master equation and obtain accurate population dynamics from the initially occupied upper or lower polariton states. Furthermore, NE-FGR significantly improves the accuracy of the population dynamics when starting from the lower polariton compared to the E-FGR theory, highlighting the importance of the non-Markovian behavior and the short-time transient behavior in the transition rate constant.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"86 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260514","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Designing a hollow MoSe2/CuS nanospheres type-II heterojunction photocatalyst with superior UV–vis-NIR absorption for photocatalytic degradation of organic pollutants 设计具有优异紫外-可见-近红外吸收能力的中空 MoSe2/CuS 纳米球 II 型异质结光催化剂，用于光催化降解有机污染物
The Journal of Chemical Physics Pub Date : 2024-09-13 DOI: 10.1063/5.0209430
Zhilong Zhang, Rong Wu, Jianyong Yue, YaLi Zhu, JiaLei Hui
{"title":"Designing a hollow MoSe2/CuS nanospheres type-II heterojunction photocatalyst with superior UV–vis-NIR absorption for photocatalytic degradation of organic pollutants","authors":"Zhilong Zhang, Rong Wu, Jianyong Yue, YaLi Zhu, JiaLei Hui","doi":"10.1063/5.0209430","DOIUrl":"https://doi.org/10.1063/5.0209430","url":null,"abstract":"In this work, a hollow MoSe2/CuS type-II heterojunction was fabricated using hollow MoSe2 nanospheres as the basis for structural design. UV–Vis–NIR diffuse absorption tests show that MoSe2/CuS has a broad spectral absorption to extend the optical response range from UV–Vis to NIR. The light source utilization rate and interfacial area are increased by the hollow MoSe2/CuS core–shell structure. The broad absorption ability of MoSe2/CuS can facilitate the photocatalysis process. As the electrochemical impedance of MoSe2/CuS is lower than that of the MoSe2, MoSe2/CuS has a good photogenerated carrier separation efficiency. Benefiting from the synergistic facilitation effect of the multi-level 3D hollow nanosphere and the significant space charge region in type-II heterojunction, the RhB degradation efficiency of MoSe2/CuS reached 96.0% in 120.0 min under Xe (350 W) broadband spectrum light irradiation. The photocatalysis mechanism of the hollow MoSe2/CuS core–shell structure was investigated. This work provides an insight into the application of broad spectrum semiconductor heterojunctions to solve environmental problems.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"29 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260508","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Limitations of the rate-distribution formalism in describing luminescence quenching in the presence of diffusion 速率分布形式主义在描述存在扩散的发光淬灭时的局限性
The Journal of Chemical Physics Pub Date : 2024-09-13 DOI: 10.1063/5.0223438
Jakub Jędrak, Gonzalo Angulo
{"title":"Limitations of the rate-distribution formalism in describing luminescence quenching in the presence of diffusion","authors":"Jakub Jędrak, Gonzalo Angulo","doi":"10.1063/5.0223438","DOIUrl":"https://doi.org/10.1063/5.0223438","url":null,"abstract":"When encountering complex fluorescence decays that deviate from exponentiality, a very appealing approach is to use lifetime or rate constant distributions. These are related by Laplace transform to the sum of exponential functions, stretched exponentials, Becquerel’s decay function, and others. However, the limitations of this approach have not been sufficiently discussed in the literature. In particular, the time-independent probability distributions of the rate constants or decay times are occasionally used to describe bimolecular quenching. We show that in such a case, this mathematical formalism has a clear physical interpretation only when the fluorophore and quencher molecules are immobile, as in the solid state. However, such an interpretation is no longer possible once we consider the motion of fluorophores with respect to quenchers. Therefore, for systems in which the relative motion of fluorophores and quenchers cannot be neglected, it is not appropriate to use the time-independent rate or decay time distributions to describe, fit, or rationalize experimental results on fluorescence decay.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"26 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260511","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Correlation functions from tensor network influence functionals: The case of the spin-boson model 张量网络影响函数的相关函数：自旋玻色子模型案例
The Journal of Chemical Physics Pub Date : 2024-09-13 DOI: 10.1063/5.0224880
Haimi Nguyen, Nathan Ng, Lachlan P. Lindoy, Gunhee Park, Andrew J. Millis, Garnet Kin-Lic Chan, David R. Reichman
{"title":"Correlation functions from tensor network influence functionals: The case of the spin-boson model","authors":"Haimi Nguyen, Nathan Ng, Lachlan P. Lindoy, Gunhee Park, Andrew J. Millis, Garnet Kin-Lic Chan, David R. Reichman","doi":"10.1063/5.0224880","DOIUrl":"https://doi.org/10.1063/5.0224880","url":null,"abstract":"We investigate the application of matrix product state (MPS) representations of the influence functionals (IFs) for the calculation of real-time equilibrium correlation functions in open quantum systems. Focusing specifically on the unbiased spin-boson model, we explore the use of IF-MPSs for complex time propagation, as well as IF-MPSs for constructing correlation functions in the steady state. We examine three different IF approaches: one based on the Kadanoff–Baym contour targeting correlation functions at all times, one based on a complex contour targeting the correlation function at a single time, and a steady state formulation, which avoids imaginary or complex times, while providing access to correlation functions at all times. We show that within the IF language, the steady state formulation provides a powerful approach to evaluate equilibrium correlation functions.","PeriodicalId":501648,"journal":{"name":"The Journal of Chemical Physics","volume":"8 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260509","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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