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Ab initio calculations of through-space and through-bond charge-transfer properties of interacting Janus-like PbSe and CdSe quantum dot heterostructures 相互作用的Janus-like PbSe和CdSe量子点异质结构的穿越空间和穿越键电荷转移性质的从头计算
4区 化学
Molecular Physics Pub Date : 2023-10-26 DOI: 10.1080/00268976.2023.2273415
Hadassah B. Griffin, Andrei B. Kryjevski, Dmitri S. Kilin
{"title":"<i>Ab initio</i> calculations of through-space and through-bond charge-transfer properties of interacting Janus-like PbSe and CdSe quantum dot heterostructures","authors":"Hadassah B. Griffin, Andrei B. Kryjevski, Dmitri S. Kilin","doi":"10.1080/00268976.2023.2273415","DOIUrl":"https://doi.org/10.1080/00268976.2023.2273415","url":null,"abstract":"AbstractHeterostructure quantum dots (QDs) are composed of two QD nanocrystals (NCs) conjoined at an interface. They are useful in applications such as photovoltaic solar cells. The properties of the interface between the NCs determine the efficiency of electron–hole recombination rates and charge transfer. Therefore, a fundamental understanding of how this interface works between the two materials is useful. To contribute to this understanding, we simulated two isolated heterostructure QD models with Janus-like geometry composed of Cd33Se33 + Pb68Se68 NCs. The first Janus-like model has a bond connection between the two NCs and is approximately 16 × 17 × 29 Å3 in size. The second model has a through-space connection between the NCs and is approximately 16 × 17 × 31 Å3. We use density functional theory to simulate the ground state properties of these models. Nonadiabatic on-the-fly couplings calculations were then used to construct the Redfield Tensor, which described the excited state dynamics due to nonradiative relaxation. From our results, we identified a qualitative trend which shows that having a bond connecting the two NCs reduces hole relaxation time. We also identified for a sample of electron–hole excitations pairs that the through-bond model allows for a net positive or negative numerical net charge transfer, depending on the excitation pair.KEYWORDS: Nonadiabatic couplingsRedfield tensorheterostructure quantum dotssolar cellsnonradiative relaxation AcknowledgementsWe also acknowledge that this research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231, allocation ‘Computational Modeling of Photo-catalysis and Photo-induced Charge Transfer Dynamics on Surfaces'. DSK acknowledges the support of NSF CHE-1944921. DSK thanks David Micha, Sergei Tretiak, Oleg Prezhdo, and Svetlana Kilina for inspiring discussions. HG thanks David Graupner, Landon Johnson, Dr. Yulun Han, Dr. Dinesh Thapa, Kamrun Nahar Keya, Patricia Adeoye, Adam Flesche, William Tupa, Joseph Granlie, Amara Arshad, Meade Erickson, Sarah Ghazanfari, and other collaborators for editorial suggestions.Disclosure statementNo potential conflict of interest was reported by the author(s).FundingWe gratefully acknowledge the support of the National Science foundation via NSF CHE-2004197 for this study. This work was supported by Chemical Sciences, Geosciences, and Biosciences Division [grant number DE-AC02-05CH11231, allocation Computational Modeling of Photocatalysis and Photo-induced Charge Transfer Dynamics on Surfaces]; National Science Foundation [grant number 1944921].","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"34 2","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136381106","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Sweetness and light: computation of the rotational spectra of proto-saccharides 甜与光:原糖旋转光谱的计算
4区 化学
Molecular Physics Pub Date : 2023-10-26 DOI: 10.1080/00268976.2023.2273976
Mengqi Sang, Terri E. Field-Theodore, Peter R. Taylor
{"title":"Sweetness and light: computation of the rotational spectra of proto-saccharides","authors":"Mengqi Sang, Terri E. Field-Theodore, Peter R. Taylor","doi":"10.1080/00268976.2023.2273976","DOIUrl":"https://doi.org/10.1080/00268976.2023.2273976","url":null,"abstract":"","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"30 4","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134908715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
The heavy Carbene analogues and . Convergent quantum mechanical studies* 重卡宾类似物和。收敛量子力学研究*
4区 化学
Molecular Physics Pub Date : 2023-10-24 DOI: 10.1080/00268976.2023.2271579
Jincan Jin, Henry F. Mull, Justin M. Turney, Henry F. Schaefer III
{"title":"The heavy Carbene analogues and . Convergent quantum mechanical studies*","authors":"Jincan Jin, Henry F. Mull, Justin M. Turney, Henry F. Schaefer III","doi":"10.1080/00268976.2023.2271579","DOIUrl":"https://doi.org/10.1080/00268976.2023.2271579","url":null,"abstract":"AbstractIn 2021 Olaru, Mebs, and Beckmann reported the synthesis of remakrable cationic carbene analogues PR2+ and AsR2+. This work followed the same group's synthesis of SbR2+ and BiR2+. To better understand these important systems, SbH2+ and BiH2+ have been studied with high level ab initio quantum mechanical methods. Geometries were optimised with the CCSDT(Q) method with the cc-pwCVTZ-PP basis set using small core pseudopotentials. Fundamental vibrational frequencies were computed to provide theoretical predictions for future synthetic studies. Relative energies with respect to Pn+ + H2 (Pn = Sb, Bi) were determined at the CCSDT/CBS level of theory via the Focal Point Analysis method, and anharmonic zero-point vibrational energy and higher order contributions were also computed. For SbH2+, we obtained R = 1.697 Å and θ=90.8∘ with Sb++H2→SbH2+ reaction enthalpy of ΔH=−18.71kcalmol−1. For BiH2+, the analogous results were R = 1.774 Å, θ=89.7∘, and ΔH=−7.64kcalmol−1 for Bi++H2→BiH2+.Keywords: Pnictogenium cationsantimonybismuthab initioCCSDT(Q) Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingWe acknowledge support from the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) under Contract No. DE-SC0018412.","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"1 6","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135316084","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
A computational and spectroscopic study of MgCCH (X 2 Σ + ): towards characterizing MgCCH + MgCCH (x2 Σ +)的计算和光谱研究:对MgCCH +的表征
4区 化学
Molecular Physics Pub Date : 2023-10-24 DOI: 10.1080/00268976.2023.2267135
Joseph E. Burns, Qianyi Cheng, Ryan C. Fortenberry, Ming Sun, Lindsay N. Zack, Trishal Zaveri, Nathan J. DeYonker, Lucy M. Ziurys
{"title":"A computational and spectroscopic study of MgCCH (X <sup>2</sup> Σ <sup>+</sup> ): towards characterizing MgCCH <sup>+</sup>","authors":"Joseph E. Burns, Qianyi Cheng, Ryan C. Fortenberry, Ming Sun, Lindsay N. Zack, Trishal Zaveri, Nathan J. DeYonker, Lucy M. Ziurys","doi":"10.1080/00268976.2023.2267135","DOIUrl":"https://doi.org/10.1080/00268976.2023.2267135","url":null,"abstract":"","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"31 5","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135321855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Predicting the physicochemical properties of drugs for the treatment of Parkinson's disease using topological indices and MATLAB programming 利用拓扑指数和MATLAB编程预测帕金森病治疗药物的理化性质
4区 化学
Molecular Physics Pub Date : 2023-10-24 DOI: 10.1080/00268976.2023.2270082
Mehri Hasani, Masoud Ghods
{"title":"Predicting the physicochemical properties of drugs for the treatment of Parkinson's disease using topological indices and MATLAB programming","authors":"Mehri Hasani, Masoud Ghods","doi":"10.1080/00268976.2023.2270082","DOIUrl":"https://doi.org/10.1080/00268976.2023.2270082","url":null,"abstract":"","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"61 2","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135322029","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Molecular spectra for molecular Mobius square potential 分子莫比乌斯平方势的分子光谱
4区 化学
Molecular Physics Pub Date : 2023-10-24 DOI: 10.1080/00268976.2023.2271094
C.A. Onate, I.B. Okon, E. Omugbe, M. C. Onyeaju, E.S. Eyube, K.O. Emeje, U.E. Vincent, J.P. Araujo, K.J. Oyewumi
{"title":"Molecular spectra for molecular Mobius square potential","authors":"C.A. Onate, I.B. Okon, E. Omugbe, M. C. Onyeaju, E.S. Eyube, K.O. Emeje, U.E. Vincent, J.P. Araujo, K.J. Oyewumi","doi":"10.1080/00268976.2023.2271094","DOIUrl":"https://doi.org/10.1080/00268976.2023.2271094","url":null,"abstract":"AbstractThe solutions of the Schrὅdinger equation for a molecular Mobius square potential are obtained using two elegant traditional methods. In each case, the energy equation is obtained. The pure vibrational energies for seven different molecules are studied using their respective spectroscopic constants and the obtained energy equation. The present results are compared with the standard results and the results of other potential models. The present study shows that the molecular Mobius square potential produces better results compared to some potential models.KEYWORDS: Bound stateeigensolutionsspectroscopywave equationpotential model Disclosure statementNo potential conflict of interest was reported by the author(s).","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"BME-21 3","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135315685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Practical guide to the statistical mechanics of molecular polaritons 分子极化的统计力学实用指南
4区 化学
Molecular Physics Pub Date : 2023-10-24 DOI: 10.1080/00268976.2023.2272691
Csaba Fábri
{"title":"Practical guide to the statistical mechanics of molecular polaritons","authors":"Csaba Fábri","doi":"10.1080/00268976.2023.2272691","DOIUrl":"https://doi.org/10.1080/00268976.2023.2272691","url":null,"abstract":"AbstractA theoretical approach aimed at the quantum statistical mechanics of a molecular ensemble coupled to a lossless cavity mode is presented. A canonical ensemble is considered and an approximate formula is devised for the Helmholtz free energy correction due to cavity-molecule coupling, which enables the derivation of experimentally measurable thermodynamic quantities. The frequency of the cavity mode is assumed to lie in the infrared range. Therefore, the cavity couples to molecular vibrations and our treatment is restricted to the electronic ground state of the molecule. The method is tested for an analytically solvable model system of one-dimensional harmonic oscillators coupled to the cavity. The performance of the approximation and its range of validity are discussed in detail. It is shown that the leading-order correction to the Helmholtz free energy is proportional to the square of the collective coupling strength. We also demonstrate that the cavity mode does not have a significant impact on the thermodynamic properties of the system in the collective ultrastrong coupling regime (the collective coupling strength is comparable to the frequency of the cavity mode).Keywords: Polaritonic chemistrymolecular polaritonsstatistical mechanicscanonical ensemble Disclosure statementNo potential conflict of interest was reported by the author(s).","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"11 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135316082","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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: 1
Second virial coefficient, Boyle temperature and equation of state of van Hove fluids with a downward concavity attractive parabolic-well 二阶维里系数、波义耳温度和下凹吸引抛物井van Hove流体的状态方程
4区 化学
Molecular Physics Pub Date : 2023-10-20 DOI: 10.1080/00268976.2023.2270721
Mariano López de Haro, Álvaro Rodríguez Rivas
{"title":"Second virial coefficient, Boyle temperature and equation of state of van Hove fluids with a downward concavity attractive parabolic-well","authors":"Mariano López de Haro, Álvaro Rodríguez Rivas","doi":"10.1080/00268976.2023.2270721","DOIUrl":"https://doi.org/10.1080/00268976.2023.2270721","url":null,"abstract":"AbstractThe second virial coefficient, the Boyle temperature and the equation of state of van Hove fluids with a relatively short ranged attractive parabolic-well of downward concavity are considered. The analytic second virial coefficient for this fluid is obtained explicitly and it is used to compute the Boyle temperature of the fluid as a function of the range of the potential. Further, an equation of state is derived using the second-order thermodynamic perturbation theory of Barker and Henderson in the macroscopic compressibility approximation, with the hard-sphere fluid being the reference fluid. For this latter we profit from the fully analytical expression of the radial distribution function, consistent with the Carnahan-Starling equation state, derived within the so-called rational function approximation method up to a range twice the size of the hard-core diameter. The results for the reduced pressure of the fluid as a function of the packing fraction and two values of the range of the potential well at different temperatures are compared with Monte Carlo simulation data. Estimates of the values of the critical temperature are also provided.KEYWORDS: Van Hove potentialparabolic-well fluidthermodynamic perturbation theoryequation of state Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingOne of us (A.R.R.) acknowledges financial support from Consejería de Transformación Económica, Industria, Conocimiento y Universidades de la Junta de Andalucía through post-doctoral grant no. DC 00316 (PAIDI 2020), co-funded by the EU Fondo Social Europeo (FSE). A.R.-R. also acknowledges support by Ministerio de Ciencias e Innovación (Spain) grant no. PID2021-126348NB-I00.","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"29 11","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135567633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
First principles studies of adsorption of H 2 S on vacancy defected and transition metal-doped phosphorene-graphene heterostructures 空位缺陷和掺杂过渡金属的磷烯-石墨烯异质结构对h2 - S吸附的第一性原理研究
4区 化学
Molecular Physics Pub Date : 2023-10-17 DOI: 10.1080/00268976.2023.2270075
Pengcheng Li, Qingxiao Zhou, Juncheng Zhu, Zenghui Zhao, Weiwei Ju, Dongtao Su
{"title":"First principles studies of adsorption of H <sub>2</sub> S on vacancy defected and transition metal-doped phosphorene-graphene heterostructures","authors":"Pengcheng Li, Qingxiao Zhou, Juncheng Zhu, Zenghui Zhao, Weiwei Ju, Dongtao Su","doi":"10.1080/00268976.2023.2270075","DOIUrl":"https://doi.org/10.1080/00268976.2023.2270075","url":null,"abstract":"AbstractThe adsorption stability, geometry, and electronic and magnetic properties of H2S adsorbed on pristine, vacancy defected, and transition metal (TM)-doped phosphorene-graphene (PG) heterostructures were calculated using density functional theory. In pristine and vacancy defected PG systems, the interaction between H2S and the heterostructure was weak, and the mechanism was physical adsorption. After TM-doping (Ti, V, Cr, Mn, Co, and Ni), the strong orbital hybridisation between the dopant and H2S significantly enhanced the interaction between H2S and the doped heterostructures, and the physisorption mechanism of H2S changed to chemical adsorption. The adsorption energy and desorption time of H2S molecules on Mn-doped PG heterostructures was suitable, which can be applied as sensors to detect H2S gas. The density of states of Cr- and Mn-doped PG heterostructures exhibited asymmetric electron spin states, indicating the existence of magnetic moments. Thus, introducing defects and TM dopants on PG heterostructures can improve H2S sensitivity, providing a theoretical basis for developing gas detection sensors.KEYWORDS: Phosphorene-graphene heterostructuresensorDFTtransition-metal dopant Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingThis work is supported by National Natural Science Foundation of China (NSFC, Grant Nos. 61874160 and 11604080), Key Science Foundation of Higher Education of Henan (22A140005), Natural Science Foundation of Henan (grant number 202300410125), Program for Innovative Research Team (in Science and Technology) in University of Henan Province (22IRTSTHN012), and the Student Research Training Program of School of Physics and Engineering (grant number WLSRTP202201).","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"26 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135994500","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Sparse adaptive basis set methods for solution of the time dependent Schrodinger equation 时变薛定谔方程解的稀疏自适应基集方法
4区 化学
Molecular Physics Pub Date : 2023-10-16 DOI: 10.1080/00268976.2023.2268221
Keiran C. Thompson, Todd J. Martinez
{"title":"Sparse adaptive basis set methods for solution of the time dependent Schrodinger equation","authors":"Keiran C. Thompson, Todd J. Martinez","doi":"10.1080/00268976.2023.2268221","DOIUrl":"https://doi.org/10.1080/00268976.2023.2268221","url":null,"abstract":"AbstractScalable numerical solutions to the time dependent Schrodinger equation remain an outstanding goal in theoretical chemistry. Here we present a method which utilises recent breakthroughs in signal processing to consistently adapt a dictionary of basis functions to the dynamics of the system. We show that for two low-dimensional model problems the size of the basis set does not grow quickly with time and appears only weakly dependent on dimensionality. The generality of this finding remains to be seen. The method primarily uses energies and gradients of the potential, opening the possibility for its use in on-the-fly ab initio quantum wavepacket dynamics.KEYWORDS: Wavepacket propagationtime-dependent Schrodinger equationcompressed sensing AcknowledgementsThis material is based upon work supported by the U.S. Department of Energy Office of Science National Quantum Information Science Research Centers as part of the Q-NEXT centre. Partial support was also provided by the AMOS programme of the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division.Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingThis work was supported by Basic Energy Sciences [Q-Next Centre and AMOS Programme].","PeriodicalId":18817,"journal":{"name":"Molecular Physics","volume":"2 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136114211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
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