Two-Dimensional Terahertz Correlation Spectra of Electronic Excitations in Semiconductor Quantum Wells

We discuss a novel approach for nonlinear two-dimensional (2D) spectroscopy in the terahertz (THz) frequency range which is based on a collinear interaction geometry of a sequence of THz pulses with the sample. The nonlinear polarization is determined by a phase-resolved measurement of the electric...

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Bibliographic Details
Published in:The journal of physical chemistry. B 2011-05, Vol.115 (18), p.5448-5455
Main Authors: Kuehn, W, Reimann, K, Woerner, M, Elsaesser, T, Hey, R
Format: Article
Language:English
Subjects:
Electrons
Quantum Theory
Semiconductors
Terahertz Spectroscopy - instrumentation
Terahertz Spectroscopy - methods
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Summary:We discuss a novel approach for nonlinear two-dimensional (2D) spectroscopy in the terahertz (THz) frequency range which is based on a collinear interaction geometry of a sequence of THz pulses with the sample. The nonlinear polarization is determined by a phase-resolved measurement of the electric field transmitted through the sample as a function of the delay τ between two phase-locked pulses and the “real” time t. The information provided by a single 2D scan along the τ and t axes is equivalent to that from a noncollinear photon-echo setup equipped with four local oscillators, each interacting with a different diffracted order. We address basic concepts of collinear 2D THz spectroscopy, in particular data analysis and phasing issues. Different rephasing and nonrephasing contributions to the third-order response are separated and 2D correlation spectra derived. As a prototype application, 2D correlation spectra of intersubband excitations of electrons in semiconductor quantum wells are presented.
ISSN:1520-6106
1520-5207
DOI:10.1021/jp1099046