Perspectives on double-excitations in TDDFT

Peter Elliott; Sharma Goldson; Chris Canahui; Neepa T. Maitra

doi:10.1016/j.chemphys.2011.03.020

Perspectives on double-excitations in TDDFT

Peter Elliott, Sharma Goldson, Chris Canahui, Neepa T. Maitra

Research output: Contribution to journal › Article › peer-review

171 Scopus citations

Abstract

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.

Original language	English (US)
Pages (from-to)	110-119
Number of pages	10
Journal	Chemical Physics
Volume	391
Issue number	1
DOIs	https://doi.org/10.1016/j.chemphys.2011.03.020
State	Published - Nov 24 2011
Externally published	Yes

All Science Journal Classification (ASJC) codes

General Physics and Astronomy
Physical and Theoretical Chemistry

Keywords

Adiabatic approximation
Autoionization
DFT
Density functional
Density matrix
Double excitations
Frozen Gaussian
Kohn-Sham
Linear-response
Quadratic response
Second-order response
Semiclassical
TDDFT

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10.1016/j.chemphys.2011.03.020

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title = "Perspectives on double-excitations in TDDFT",

abstract = "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.",

keywords = "Adiabatic approximation, Autoionization, DFT, Density functional, Density matrix, Double excitations, Frozen Gaussian, Kohn-Sham, Linear-response, Quadratic response, Second-order response, Semiclassical, TDDFT",

author = "Peter Elliott and Sharma Goldson and Chris Canahui and Maitra, {Neepa T.}",

note = "Funding Information: We acknowledge support from the National Science Foundation ( CHE-0647913 ), the Cottrell Scholar Program of Research Corporation and the NIH-funded MARC program (SG and CC), grant GM007823-30 .",

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doi = "10.1016/j.chemphys.2011.03.020",

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AU - Elliott, Peter

AU - Goldson, Sharma

AU - Canahui, Chris

AU - Maitra, Neepa T.

N1 - Funding Information: We acknowledge support from the National Science Foundation ( CHE-0647913 ), the Cottrell Scholar Program of Research Corporation and the NIH-funded MARC program (SG and CC), grant GM007823-30 .

PY - 2011/11/24

Y1 - 2011/11/24

N2 - 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.

AB - 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.

KW - Adiabatic approximation

KW - Autoionization

KW - DFT

KW - Density functional

KW - Density matrix

KW - Double excitations

KW - Frozen Gaussian

KW - Kohn-Sham

KW - Linear-response

KW - Quadratic response

KW - Second-order response

KW - Semiclassical

KW - TDDFT

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DO - 10.1016/j.chemphys.2011.03.020

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VL - 391

SP - 110

EP - 119

JO - Chemical Physics

JF - Chemical Physics

IS - 1

ER -

Perspectives on double-excitations in TDDFT

Abstract

All Science Journal Classification (ASJC) codes

Keywords

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