Molecular excitation energies to high-lying bound states from timedependent density-functional response thesoty:Characterization and correction of the time-dependent local density approximation ionization threshold

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	Molecular excitation energies to high-lying bound states from timedependent density-functional response thesoty:Characterization and correction of the time-dependent local density approximation ionization threshold
	Mark E. Casida ; Christine Jamorski ; Kim C. Casida ; and Dennis R. Salahub
发表期刊	Journal of the Chemical ohysics
	1998
卷号	108 期号:11 页码:4439-4450
通讯作者	Mark E. Casida
英文摘要	This paper presents an evaluation of the performance of time-dependent density-functional response theory (TD-DFRT) for the calculation of high-lying bound electronic excitation energies of molecules. TD-DFRT excitation energies are reported for a large number of states for each of four molecules: N2, CO, CH2O, and C2H4. In contrast to the good results obtained for low-lying states within the time-dependent local density approximation (TDLDA), there is a marked deterioration of the results for high-lying bound states. This is manifested as a collapse of the states above the TDLDA ionization threshold, which is at ??HOMOLDA (the negative of the highest occupied molecular orbital energy in the LDA). The ??HOMOLDA is much lower than the true ionization potential because the LDA exchange-correlation potential has the wrong asymptotic behavior. For this reason, the excitation energies were also calculated using the asymptotically correct potential of van Leeuwen and Baerends (LB94) in the self-consistent field step. This was found to correct the collapse of the high-lying states that was observed with the LDA. Nevertheless, further improvement of the functional is desirable. For low-lying states the asymptotic behavior of the exchange-correlation potential is not critical and the LDA potential does remarkably well. We propose criteria delineating for which states the TDLDA can be expected to be used without serious impact from the incorrect asymptotic behavior of the LDA potential
文献类型	期刊论文
条目标识符	http://ir.yic.ac.cn/handle/133337/4571
专题	科研共享资源
推荐引用方式 GB/T 7714	Mark E. Casida,Christine Jamorski,Kim C. Casida,et al. Molecular excitation energies to high-lying bound states from timedependent density-functional response thesoty:Characterization and correction of the time-dependent local density approximation ionization threshold[J]. Journal of the Chemical ohysics,1998,108(11):4439-4450.
APA	Mark E. Casida,Christine Jamorski,Kim C. Casida,&and Dennis R. Salahub.(1998).Molecular excitation energies to high-lying bound states from timedependent density-functional response thesoty:Characterization and correction of the time-dependent local density approximation ionization threshold.Journal of the Chemical ohysics,108(11),4439-4450.
MLA	Mark E. Casida,et al."Molecular excitation energies to high-lying bound states from timedependent density-functional response thesoty:Characterization and correction of the time-dependent local density approximation ionization threshold".Journal of the Chemical ohysics 108.11(1998):4439-4450.

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