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Article: Time-Dependent Density Functional Theory for Open Systems and Its Applications

TitleTime-Dependent Density Functional Theory for Open Systems and Its Applications
Authors
Issue Date2018
PublisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journals/achre4/about.html
Citation
Accounts of Chemical Research, 2018, v. 51, p. 385-393 How to Cite?
AbstractPhotovoltaic devices, electrochemical cells, catalysis processes, light emitting diodes, scanning tunneling microscopes, molecular electronics, and related devices have one thing in common: open quantum systems where energy and matter are not conserved. Traditionally quantum chemistry is confined to isolated and closed systems, while quantum dissipation theory studies open quantum systems. The key quantity in quantum dissipation theory is the reduced system density matrix. As the reduced system density matrix is an O(M! × M!) matrix, where M is the number of the particles of the system of interest, quantum dissipation theory can only be employed to simulate systems of a few particles or degrees of freedom. It is thus important to combine quantum chemistry and quantum dissipation theory so that realistic open quantum systems can be simulated from first-principles. We have developed a first-principles method to simulate the dynamics of open electronic systems, the time-dependent density functional theory for open systems (TDDFT-OS). Instead of the reduced system density matrix, the key quantity is the reduced single-electron density matrix, which is an N × N matrix where N is the number of the atomic bases of the system of interest. As the dimension of the key quantity is drastically reduced, the TDDFT-OS can thus be used to simulate the dynamics of realistic open electronic systems and efficient numerical algorithms have been developed. As an application, we apply the method to study how quantum interference develops in a molecular transistor in time domain. We include electron−phonon interaction in our simulation and show that quantum interference in the given system is robust against nuclear vibration not only in the steady state but also in the transient dynamics. As another application, by combining TDDFT-OS with Ehrenfest dynamics, we study current-induced dissociation of water molecules under scanning tunneling microscopy and follow its time dependent dynamics. Given the rapid development in ultrafast experiments with atomic resolution in recent years, time dependent simulation of open electronic systems will be useful to gain insight and understanding of such experiments. This Account will mainly focus on the practical aspects of the TDDFT-OS method, describing the numerical implementation and demonstrating the method with applications.
Persistent Identifierhttp://hdl.handle.net/10722/259172
ISSN
2019 Impact Factor: 20.832
2015 SCImago Journal Rankings: 11.465
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorChen, S-
dc.contributor.authorKwok, YH-
dc.contributor.authorChen, G-
dc.date.accessioned2018-09-03T04:02:40Z-
dc.date.available2018-09-03T04:02:40Z-
dc.date.issued2018-
dc.identifier.citationAccounts of Chemical Research, 2018, v. 51, p. 385-393-
dc.identifier.issn0001-4842-
dc.identifier.urihttp://hdl.handle.net/10722/259172-
dc.description.abstractPhotovoltaic devices, electrochemical cells, catalysis processes, light emitting diodes, scanning tunneling microscopes, molecular electronics, and related devices have one thing in common: open quantum systems where energy and matter are not conserved. Traditionally quantum chemistry is confined to isolated and closed systems, while quantum dissipation theory studies open quantum systems. The key quantity in quantum dissipation theory is the reduced system density matrix. As the reduced system density matrix is an O(M! × M!) matrix, where M is the number of the particles of the system of interest, quantum dissipation theory can only be employed to simulate systems of a few particles or degrees of freedom. It is thus important to combine quantum chemistry and quantum dissipation theory so that realistic open quantum systems can be simulated from first-principles. We have developed a first-principles method to simulate the dynamics of open electronic systems, the time-dependent density functional theory for open systems (TDDFT-OS). Instead of the reduced system density matrix, the key quantity is the reduced single-electron density matrix, which is an N × N matrix where N is the number of the atomic bases of the system of interest. As the dimension of the key quantity is drastically reduced, the TDDFT-OS can thus be used to simulate the dynamics of realistic open electronic systems and efficient numerical algorithms have been developed. As an application, we apply the method to study how quantum interference develops in a molecular transistor in time domain. We include electron−phonon interaction in our simulation and show that quantum interference in the given system is robust against nuclear vibration not only in the steady state but also in the transient dynamics. As another application, by combining TDDFT-OS with Ehrenfest dynamics, we study current-induced dissociation of water molecules under scanning tunneling microscopy and follow its time dependent dynamics. Given the rapid development in ultrafast experiments with atomic resolution in recent years, time dependent simulation of open electronic systems will be useful to gain insight and understanding of such experiments. This Account will mainly focus on the practical aspects of the TDDFT-OS method, describing the numerical implementation and demonstrating the method with applications.-
dc.languageeng-
dc.publisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journals/achre4/about.html-
dc.relation.ispartofAccounts of Chemical Research-
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in [JournalTitle], copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see [insert ACS Articles on Request author-directed link to Published Work, see http://pubs.acs.org/page/policy/articlesonrequest/index.html].-
dc.titleTime-Dependent Density Functional Theory for Open Systems and Its Applications-
dc.typeArticle-
dc.identifier.emailChen, S: h0992048@hku.hk-
dc.identifier.emailKwok, YH: balloonr@hku.hk-
dc.identifier.emailChen, G: ghchen@hku.hk-
dc.identifier.authorityChen, G=rp00671-
dc.identifier.doi10.1021/acs.accounts.7b00382-
dc.identifier.scopuseid_2-s2.0-85042305558-
dc.identifier.hkuros288594-
dc.identifier.volume51-
dc.identifier.spage385-
dc.identifier.epage393-
dc.identifier.isiWOS:000426014500020-
dc.publisher.placeUnited States-

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