Identifying incoherent mixing effects in the coherent two-dimensional photocurrent excitation spectra of semiconductors

Abstract

We have previously demonstrated that in the context of two-dimensional (2D) coherent electronic spectroscopy measured by phase modulation and phase-sensitive detection, an \emph{incoherent} nonlinear response, due to pairs of photoexcitations produced via linear excitation pathways, contribute to the measured signal as unexpected background [Gr\'egoire et al., J.\ Chem.\ Phys. \textbf{147}, 114201 (2017)]. Here, we simulate the effect of such incoherent population mixing in the photocurrent signal collected from a GaAs solar cell by acting externally on the transimpedance amplifier circuit used for phase-sensitive detection, and we identify an effective strategy to recognize the presence of incoherent population mixing in 2D data. While we find that incoherent mixing is reflected by cross-talk between the linear amplitude at the two time-delay variables in the four-pulse excitation sequence, we do not observe any strict phase correlations between the coherent and incoherent contributions, as expected from modelling of a simple system.