Isolating excitonic Raman coherence in semiconductors using two-dimensional correlation spectroscopy

Abstract

We present the experimental and simulation results of two-dimensional optical coherent correlation spectroscopy signals along the phase-matching direction k(I) = -k(1) + k(2) + k(3) projected on the two-dimensional (2D) (Omega(3),Omega(2)) plane corresponding to the second and third delay periods. Overlapping Raman coherences in the conventional (Omega(3),Omega(1)) 2D projection may now be clearly resolved. The linewidths of the heavy-hole (HH) and light-hole (LH) excitonic Raman coherence peaks are obtained. Further insights on the higher-order (beyond time-dependent Hartree-Fock) correlation effects among mixed (HH and LH) two excitons can be gained by using a cocircular pulse polarization configuration.