Title

Time-dependent density-functional theory of exciton-exciton correlations in the nonlinear optical response

Authors

Authors

V. Turkowski;M. N. Leuenberger

Comments

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Abbreviated Journal Title

Phys. Rev. B

Keywords

EXCITATIONS; SYSTEMS; REGIME; Physics, Condensed Matter

Abstract

We analyze possible nonlinear exciton-exciton correlation effects in the optical response of semiconductors by using a time-dependent density-functional theory (TDDFT) approach. For this purpose we derive the nonlinear (third-order) TDDFT equation for the excitonic polarization. In this equation the nonlinear time-dependent effects are described by the time-dependent (nonadiabatic) part of the effective exciton-exciton interaction, which depends on the exchange-correlation (XC) kernel. We apply the approach to study the nonlinear optical response of a GaAs quantum well. In particular, we calculate the two-dimensional Fourier spectrum (2DFS) of the system and compare it with experimental data. We find that the memory effects play a crucial role in this response, and in particular that it is necessary to use a nonadiabatic XC kernel to describe excitonic bound states, biexcitons, which are formed due to the retarded TDDFT exciton-exciton interaction.

Journal Title

Physical Review B

Volume

89

Issue/Number

7

Publication Date

1-1-2014

Document Type

Article

Language

English

First Page

5

WOS Identifier

WOS:000332397300006

ISSN

1098-0121

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