### Abstract

We present an implementation for considering finite lifetime of the electronic excited states into linear-response theory within time-dependent density-functional theory. The lifetime of the excited states is introduced by a common phenomenological damping factor. The real and imaginary frequency-dependent polarizabilities can thus be calculated over a broad range of frequencies. This allows for the study of linear-response properties both in the resonance and nonresonance cases. The method is complementary to the standard approach of calculating the excitation energies from the poles of the polarizability. The real and imaginary polarizabilities can then be calculated in any specific energy range of interest, in contrast to the excitation energies which are usually solved only for the lowest electronic states. We have verified the method by investigating the photoabsorption properties of small alkali clusters. For these systems, we have calculated the real and imaginary polarizabilities in the energy range of 1-4 eV and compared these with excitation energy calculations. The results showed good agreement with both previous theoretical and experimental results.

Original language | English (US) |
---|---|

Article number | 224115 |

Journal | Journal of Chemical Physics |

Volume | 122 |

Issue number | 22 |

DOIs | |

State | Published - Jun 8 2005 |

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### All Science Journal Classification (ASJC) codes

- Physics and Astronomy(all)
- Physical and Theoretical Chemistry

### Cite this

*Journal of Chemical Physics*,

*122*(22), [224115]. https://doi.org/10.1063/1.1929740

}

*Journal of Chemical Physics*, vol. 122, no. 22, 224115. https://doi.org/10.1063/1.1929740

**Finite lifetime effects on the polarizability within time-dependent density-functional theory.** / Jensen, L.; Autschbach, J.; Schatz, G. C.

Research output: Contribution to journal › Article

TY - JOUR

T1 - Finite lifetime effects on the polarizability within time-dependent density-functional theory

AU - Jensen, L.

AU - Autschbach, J.

AU - Schatz, G. C.

PY - 2005/6/8

Y1 - 2005/6/8

N2 - We present an implementation for considering finite lifetime of the electronic excited states into linear-response theory within time-dependent density-functional theory. The lifetime of the excited states is introduced by a common phenomenological damping factor. The real and imaginary frequency-dependent polarizabilities can thus be calculated over a broad range of frequencies. This allows for the study of linear-response properties both in the resonance and nonresonance cases. The method is complementary to the standard approach of calculating the excitation energies from the poles of the polarizability. The real and imaginary polarizabilities can then be calculated in any specific energy range of interest, in contrast to the excitation energies which are usually solved only for the lowest electronic states. We have verified the method by investigating the photoabsorption properties of small alkali clusters. For these systems, we have calculated the real and imaginary polarizabilities in the energy range of 1-4 eV and compared these with excitation energy calculations. The results showed good agreement with both previous theoretical and experimental results.

AB - We present an implementation for considering finite lifetime of the electronic excited states into linear-response theory within time-dependent density-functional theory. The lifetime of the excited states is introduced by a common phenomenological damping factor. The real and imaginary frequency-dependent polarizabilities can thus be calculated over a broad range of frequencies. This allows for the study of linear-response properties both in the resonance and nonresonance cases. The method is complementary to the standard approach of calculating the excitation energies from the poles of the polarizability. The real and imaginary polarizabilities can then be calculated in any specific energy range of interest, in contrast to the excitation energies which are usually solved only for the lowest electronic states. We have verified the method by investigating the photoabsorption properties of small alkali clusters. For these systems, we have calculated the real and imaginary polarizabilities in the energy range of 1-4 eV and compared these with excitation energy calculations. The results showed good agreement with both previous theoretical and experimental results.

UR - http://www.scopus.com/inward/record.url?scp=20544466926&partnerID=8YFLogxK

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U2 - 10.1063/1.1929740

DO - 10.1063/1.1929740

M3 - Article

C2 - 15974659

AN - SCOPUS:20544466926

VL - 122

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 22

M1 - 224115

ER -