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.

Nonlinear optical signals and spectroscopy with quantum light

“…We now present a different multidimensional time-domain signal that involves higher electronic states manifold, but does not require excited populations. This is known as doublequantum-coherence (DQC) (Kim et al, 2009;Mukamel et al, 2007;Palmieri et al, 2009;Yang and Mukamel, 2008) where the system evolves in the coherence between ground and doubly excited state |f g| rather than in a population |f f |. This technique reveals the energies of single and doubly excited state energies as well as the correlations between single and doubly excited states .…”

“…Time domain two dimensional (2D) spectroscopic techniques (Mukamel, 2000), provide a versatile tool for exploring the properties of molecular systems, such as photosynthetic aggregates (Abramavicius et al, 2008;Engel et al, 2007) or coupled (Hybrid-)nanostructures to semiconductor quantum wells (Pasenow et al, 2008;Vogel et al, 2009;Yang et al, 2008;Zhang et al, 2007). These techniques use sequences of coherent pulses that are shorter than the dephasing times of the system.…”

Correlation and dephasing effects on the non-radiative coherence between bright excitons in an InAs QD ensemble measured with 2D spectroscopy

“…In this work, we demonstrate that δ 1 can be measured for all QDs in the inhomogeneously broadened ensemble simultaneously by monitoring the temporal evolution of the coherence [15] between |H and |V using two-dimensional Fouriertransform spectroscopy (2DFTS), which is based on three-pulse transient FWM [16]. The non-radiative |H -|V coherence, which has no optical dipole moment, can be probed optically by coherently exciting the |0 -|H and |0 -|V transitions using either two orthogonal linearly-polarized pulses or a single circularly-polarized pulse.…”

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

“…When T is stepped instead of τ , a Fourier transform provides a zeroquantum 2D spectrum, plotted as a function of ω T and ω t for a fixed delay τ [12]. In such a spectrum, population terms contribute to a zero-energy peak, whose linewidth is characteristic of population decay rates.…”