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 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.