Multidimensional coherent photocurrent spectroscopy of a semiconductor nanostructure

Abstract

Multidimensional Coherent Optical Photocurrent Spectroscopy (MD-COPS) is implemented using unstabilized interferometers. Photocurrent from a semiconductor sample is generated using a sequence of four excitation pulses in a collinear geometry. Each pulse is frequency shifted by a unique radio frequency through acousto-optical modulation; the Four-Wave Mixing (FWM) signal is then selected in the frequency domain. The interference of an auxiliary continuous wave laser, which is sent through the same interferometers as the excitation pulses, is used to synthesize reference frequencies for lock-in detection of the photocurrent FWM signal. This scheme enables the partial compensation of mechanical fluctuations in the setup, achieving sufficient phase stability without the need for active stabilization. The method intrinsically provides both the real and imaginary parts of the FWM signal as a function of inter-pulse delays. This signal is subsequently Fourier transformed to create a multi-dimensional spectrum. Measurements made on the excitonic resonance in a double InGaAs quantum well embedded in a p-i-n diode demonstrate the technique.

Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy

“…There are many different spectrometer designs for collecting 2D spectra 18,[34][35][36][37][38][39][40][41][42] . Our spectrometer design, shown in Supplementary Fig.…”

Nonlinear optical signals and spectroscopy with quantum light

“…Information similar to coherent spectroscopy can be extracted from the parametric dependence on various pulse sequences applied prior to the incoherent detection (Mukamel and Richter, 2011a;Rahav and Mukamel, 2010). Possible incoherent detection modes include fluorescence (Barkai, 2008;Elf et al, 2007), photoaccoustic (Patel and Tam, 1981), AFM (Mamin et al, 2005;Poggio et al, 2009;Rajapaksa and Kumar Wickramasinghe, 2011;Rajapaksa et al, 2010) or photocurrent detection (Cheng and Xie, 2012;Nardin et al, 2013). …”

Optimizing sparse sampling for 2D electronic spectroscopy

“…Coherent two-dimensional (2D) electronic spectroscopy [1][2][3][4][5] has become an established method to study, among others, energy transfer in light harvesting complexes, [6][7][8] electronic dynamics in semiconductors, [9][10][11][12][13] plasmonic coherences, 14 and photochemical reactions. 15 Most of the experimental realizations rely on the non-collinear box geometry and heterodyned detection of a coherent optical signal.…”

“…15 Most of the experimental realizations rely on the non-collinear box geometry and heterodyned detection of a coherent optical signal. Another option that has been developed is action-based 2D spectroscopy using a train of four (often collinear) laser pulses and a phase-modulation, 10,16 or phase-cycling scheme. 17,18 The action-based ansatz employs the detection of incoherent signals, e.g., fluorescence 16,17 (see also Fig.…”