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231224s2016 xx |||||o 00| ||eng c |
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|a 10.1002/jcc.24357
|2 doi
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|a pubmed24n0862.xml
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|a DE-627
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|e rakwb
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| 041 |
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|a eng
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| 100 |
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|a Tsuneda, Takao
|e verfasserin
|4 aut
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|a Relationship between orbital energy gaps and excitation energies for long-chain systems
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|c 2016
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
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|a ƒa Online-Ressource
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|a Date Completed 19.07.2018
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|a Date Revised 19.07.2018
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2016 Wiley Periodicals, Inc.
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|a The difference between the excitation energies and corresponding orbital energy gaps, the exciton binding energy, is investigated based on time-dependent (TD) density functional theory (DFT) for long-chain systems: all-trans polyacetylenes and linear oligoacenes. The optimized geometries of these systems indicate that bond length alternations significantly depend on long-range exchange interactions. In TDDFT formalism, the exciton binding energy comes from the two-electron interactions between occupied and unoccupied orbitals through the Coulomb-exchange-correlation integral kernels. TDDFT calculations show that the exciton binding energy is significant when long-range exchange interactions are involved. Spin-flip (SF) TDDFT calculations are then carried out to clarify double-excitation effects in these excitation energies. The calculated SF-TDDFT results indicate that double-excitation effects significantly contribute to the excitations of long-chain systems. The discrepancies between the vertical ionization potential minus electron affinity (IP-EA) values and the HOMO-LUMO excitation energies are also evaluated for the infinitely long polyacetylene and oligoacene using the least-square fits to estimate the exciton binding energy of infinitely long systems. It is found that long-range exchange interactions are required to give the exciton binding energy of the infinitely long systems. Consequently, it is concluded that long-range exchange interactions neglected in many DFT calculations play a crucial role in the exciton binding energies of long-chain systems, while double-excitation correlation effects are also significant to hold the energy balance of the excitations. © 2016 Wiley Periodicals, Inc
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|a Journal Article
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|a Research Support, Non-U.S. Gov't
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|a HOMO-LUMO gap
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|a band gap
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|a double-excitation effect
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|a exciton binding energy
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|a long-range exchange effect
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|a Singh, Raman K
|e verfasserin
|4 aut
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| 700 |
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|a Nakata, Ayako
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Journal of computational chemistry
|d 1984
|g 37(2016), 16 vom: 15. Juni, Seite 1451-62
|w (DE-627)NLM098138448
|x 1096-987X
|7 nnns
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| 773 |
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|g volume:37
|g year:2016
|g number:16
|g day:15
|g month:06
|g pages:1451-62
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|u http://dx.doi.org/10.1002/jcc.24357
|3 Volltext
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