Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory
The implementation of local control theory using nonadiabatic molecular dynamics within the framework of linear-response time-dependent density functional theory is discussed. The method is applied to study the photoexcitation of lithium fluoride, for which we demonstrate that this approac...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | deu |
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Swiss Chemical Society
2013-04-01
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| Series: | CHIMIA |
| Subjects: | |
| Online Access: | https://www.chimia.ch/chimia/article/view/5368 |
| _version_ | 1824044579132801024 |
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| author | Basile F. E. Curchod Thomas J. Penfold Ursula Rothlisberger Ivano Tavernelli |
| author_facet | Basile F. E. Curchod Thomas J. Penfold Ursula Rothlisberger Ivano Tavernelli |
| author_sort | Basile F. E. Curchod |
| collection | DOAJ |
| description |
The implementation of local control theory using nonadiabatic molecular dynamics within the framework of linear-response time-dependent density functional theory is discussed. The method is applied to study the photoexcitation of lithium fluoride, for which we demonstrate that this
approach can efficiently generate a pulse, on-the-fly, able to control the population transfer between two selected electronic states. Analysis of the computed control pulse yields insights into the photophysics of the process identifying the relevant frequencies associated to the curvature
of the initial and final state potential energy curves and their energy differences. The limitations inherent to the use of the trajectory surface hopping approach are also discussed.
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| first_indexed | 2024-12-23T00:13:32Z |
| format | Article |
| id | doaj.art-556b3939640d43329f0d35cd6f6cb59c |
| institution | Directory Open Access Journal |
| issn | 0009-4293 2673-2424 |
| language | deu |
| last_indexed | 2024-12-23T00:13:32Z |
| publishDate | 2013-04-01 |
| publisher | Swiss Chemical Society |
| record_format | Article |
| series | CHIMIA |
| spelling | doaj.art-556b3939640d43329f0d35cd6f6cb59c2022-12-21T18:07:28ZdeuSwiss Chemical SocietyCHIMIA0009-42932673-24242013-04-0167410.2533/chimia.2013.218Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional TheoryBasile F. E. Curchod0Thomas J. Penfold1Ursula Rothlisberger2Ivano Tavernelli3Laboratory of Computational Chemistry and Biochemistry Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, SwitzerlandLaboratory of Computational Chemistry and Biochemistry Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland; Laboratory of Ultrafast Spectroscopy Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland; SwissFEL Paul Scherrer Institute, SwitzerlandLaboratory of Computational Chemistry and Biochemistry Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, SwitzerlandLaboratory of Computational Chemistry and Biochemistry Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland. ivano.tavernelli@epfl.ch The implementation of local control theory using nonadiabatic molecular dynamics within the framework of linear-response time-dependent density functional theory is discussed. The method is applied to study the photoexcitation of lithium fluoride, for which we demonstrate that this approach can efficiently generate a pulse, on-the-fly, able to control the population transfer between two selected electronic states. Analysis of the computed control pulse yields insights into the photophysics of the process identifying the relevant frequencies associated to the curvature of the initial and final state potential energy curves and their energy differences. The limitations inherent to the use of the trajectory surface hopping approach are also discussed. https://www.chimia.ch/chimia/article/view/5368Born-oppenheimer approximationLinear-response time-dependent density functional theoryLocal control theoryNonadiabatic dynamics |
| spellingShingle | Basile F. E. Curchod Thomas J. Penfold Ursula Rothlisberger Ivano Tavernelli Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory CHIMIA Born-oppenheimer approximation Linear-response time-dependent density functional theory Local control theory Nonadiabatic dynamics |
| title | Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory |
| title_full | Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory |
| title_fullStr | Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory |
| title_full_unstemmed | Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory |
| title_short | Local Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory |
| title_sort | local control theory using trajectory surface hopping and linear response time dependent density functional theory |
| topic | Born-oppenheimer approximation Linear-response time-dependent density functional theory Local control theory Nonadiabatic dynamics |
| url | https://www.chimia.ch/chimia/article/view/5368 |
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