Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems
The restricted excitation subspace approximation is explored as a basis to reduce the memory storage required in linear response time-dependent density functional theory (TDDFT) calculations within the Tamm-Dancoff approximation. It is shown that excluding the core orbitals and up to 70% of the virt...
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Taylor & Francis
2018
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| Online Access: | http://eprints.nottingham.ac.uk/49206/ http://eprints.nottingham.ac.uk/49206/ http://eprints.nottingham.ac.uk/49206/ http://eprints.nottingham.ac.uk/49206/8/Assessment%20of%20time%20dependent%20density%20functional%20theory%20with%20the%20restricted%20excitation%20space%20approximation%20for%20excited%20state%20calculations%20of%20large.pdf |
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nottingham-492062018-05-01T15:48:32Z http://eprints.nottingham.ac.uk/49206/ Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems Hanson-Heine, Magnus W.D. George, Michael W. Besley, Nicholas A. The restricted excitation subspace approximation is explored as a basis to reduce the memory storage required in linear response time-dependent density functional theory (TDDFT) calculations within the Tamm-Dancoff approximation. It is shown that excluding the core orbitals and up to 70% of the virtual orbitals in the construction of the excitation subspace does not result in significant changes in computed UV/vis spectra for large molecules. The reduced size of the excitation subspace greatly reduces the size of the subspace vectors that need to be stored when using the Davidson procedure to determine the eigenvalues of the TDDFT equations. Furthermore, additional screening of the two-electron integrals in combination with a reduction in the size of the numerical integration grid used in the TDDFT calculation leads to significant computational savings. The use of these approximations represents a simple approach to extend TDDFT to the study of large systems and make the calculations increasingly tractable using modest computing resources. Taylor & Francis 2018-02-06 Article PeerReviewed application/pdf en cc_by http://eprints.nottingham.ac.uk/49206/8/Assessment%20of%20time%20dependent%20density%20functional%20theory%20with%20the%20restricted%20excitation%20space%20approximation%20for%20excited%20state%20calculations%20of%20large.pdf Hanson-Heine, Magnus W.D. and George, Michael W. and Besley, Nicholas A. (2018) Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems. Molecular Physics, 116 (11). pp. 1452-1459. ISSN 1362-3028 http://www.tandfonline.com/doi/full/10.1080/00268976.2018.1430388 doi:10.1080/00268976.2018.1430388 doi:10.1080/00268976.2018.1430388 |
| repository_type |
Digital Repository |
| institution_category |
Local University |
| institution |
University of Nottingham Malaysia Campus |
| building |
Nottingham Research Data Repository |
| collection |
Online Access |
| language |
English |
| description |
The restricted excitation subspace approximation is explored as a basis to reduce the memory storage required in linear response time-dependent density functional theory (TDDFT) calculations within the Tamm-Dancoff approximation. It is shown that excluding the core orbitals and up to 70% of the virtual orbitals in the construction of the excitation subspace does not result in significant changes in computed UV/vis spectra for large molecules. The reduced size of the excitation subspace greatly reduces the size of the subspace vectors that need to be stored when using the Davidson procedure to determine the eigenvalues of the TDDFT equations. Furthermore, additional screening of the two-electron integrals in combination with a reduction in the size of the numerical integration grid used in the TDDFT calculation leads to significant computational savings. The use of these approximations represents a simple approach to extend TDDFT to the study of large systems and make the calculations increasingly tractable using modest computing resources. |
| format |
Article |
| author |
Hanson-Heine, Magnus W.D. George, Michael W. Besley, Nicholas A. |
| spellingShingle |
Hanson-Heine, Magnus W.D. George, Michael W. Besley, Nicholas A. Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems |
| author_facet |
Hanson-Heine, Magnus W.D. George, Michael W. Besley, Nicholas A. |
| author_sort |
Hanson-Heine, Magnus W.D. |
| title |
Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems |
| title_short |
Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems |
| title_full |
Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems |
| title_fullStr |
Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems |
| title_full_unstemmed |
Assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems |
| title_sort |
assessment of time-dependent density functional theory with the restricted excitation space approximation for excited state calculations of large systems |
| publisher |
Taylor & Francis |
| publishDate |
2018 |
| url |
http://eprints.nottingham.ac.uk/49206/ http://eprints.nottingham.ac.uk/49206/ http://eprints.nottingham.ac.uk/49206/ http://eprints.nottingham.ac.uk/49206/8/Assessment%20of%20time%20dependent%20density%20functional%20theory%20with%20the%20restricted%20excitation%20space%20approximation%20for%20excited%20state%20calculations%20of%20large.pdf |
| first_indexed |
2018-09-06T14:05:01Z |
| last_indexed |
2018-09-06T14:05:01Z |
| _version_ |
1610867227095990272 |