Perspectives on double-excitations in TDDFT

被引：165

作者：

Elliott, Peter ^{[1
]}

Goldson, Sharma ^{[1
]}

Canahui, Chris ^{[1
]}

Maitra, Neepa T. ^{[1
]}

机构：

[1] CUNY Hunter Coll, Dept Phys & Astron, New York, NY 10065 USA

来源：

CHEMICAL PHYSICS | 2011年 / 391卷 / 01期

基金：

美国国家科学基金会;

关键词：

TDDFT; DFT; Kohn-Sham; Double excitations; Linear-response; Quadratic response; Second-order response; Autoionization; Semiclassical; Frozen Gaussian; Density matrix; Density functional; Adiabatic approximation; DENSITY-FUNCTIONAL THEORY; EXCITED-STATES; MOLECULAR PHOTOIONIZATION; DRESSED TDDFT; RANGE; ENERGIES; EXCHANGE; SPECTROSCOPY; PERFORMANCE; RESONANCES;

D O I：

10.1016/j.chemphys.2011.03.020

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The adiabatic approximation in time-dependent density functional theory (TDDFT) yields reliable excitation spectra with great efficiency in many cases, but fundamentally fails for states of double-excitation character. We discuss how double-excitations are at the root of some of the most challenging problems for TDDFT today. We then present new results for (i) the calculation of autoionizing resonances in the helium atom, (ii) understanding the nature of the double excitations appearing in the quadratic response function, and (iii) retrieving double-excitations through a real-time semiclassical approach to correlation in a model quantum dot. (C) 2011 Published by Elsevier B. V.

引用

页码：110 / 119

页数：10

共 77 条

[1]

[Anonymous], 1996, RECENT DEV APPL DENS

[2] Excitations in time-dependent density-functional theory [J].

Appel, H ;

Gross, EKU ;

Burke, K .

PHYSICAL REVIEW LETTERS, 2003, 90 (04) :4

[3] Time-dependent natural orbitals and occupation numbers [J].

Appel, H. ;

Gross, E. K. U. .

EPL, 2010, 92 (02)

[4] Charge-Transfer Excitations and Time-Dependent Density Functional Theory: Problems and Some Proposed Solutions [J].

Autschbach, Jochen .

CHEMPHYSCHEM, 2009, 10 (11) :1757-1760

[5] Gaussian Type Orbitals basis sets for the calculation of continuum properties in molecules: the differential photoionization cross section of acetylene [J].

Cacelli, I ;

Moccia, R ;

Rizzo, A .

CHEMICAL PHYSICS, 2000, 252 (1-2) :67-81

[6] Propagator corrections to adiabatic time-dependent density-functional theory linear response theory [J].

Casida, ME .

JOURNAL OF CHEMICAL PHYSICS, 2005, 122 (05)

[7] A dressed TDDFT treatment of the 2Ag states of butadiene and hexatriene [J].

Cave, RJ ;

Zhang, F ;

Maitra, NT ;

Burke, K .

CHEMICAL PHYSICS LETTERS, 2004, 389 (1-3) :39-42

[8] Long-range charge-transfer excited states in time-dependent density functional theory require non-local exchange [J].

Dreuw, A ;

Weisman, JL ;

Head-Gordon, M .

JOURNAL OF CHEMICAL PHYSICS, 2003, 119 (06) :2943-2946

[9]

ELLIOTT P, UNPUB

[10] Excited States from Time-Dependent Density Functional Theory [J].

Elliott, Peter ;

Furche, Filipp ;

Burke, Kieron .

REVIEWS IN COMPUTATIONAL CHEMISTRY, VOL 26, 2009, 26 :91-165

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