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arXiv:2601.05753

Spectral Tailoring of Inhomogeneous Optical Response Using Two-Dimensional Coherent Spectroscopy

Pradeep Kumar, Rohan Singh

Published Jan 9, 2026• 0 citations
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Abstract

Controlling the coherent optical response of inhomogeneous ensembles is a key challenge in advancing light-matter interaction engineering. We present a comparative study of two spectral tailoring approaches using two-dimensional coherent spectroscopy (2DCS): the prepulse and double-pulse (DP) methods. In the prepulse scheme, a high-intensity pulse induces Rabi oscillations, modulating the 2D spectral amplitude and lineshape when its spectral bandwidth matches the ensemble full width at half maximum (FWHM). To overcome this limitation, the DP method employs variable inter-pulse delay to generate predetermined periodic spectral modulation without bandwidth constraints. Moreover, tuning the relative phase between DP pulses allows selective switching of frequency components, enabling controlled enhancement or suppression of distinct spectral features. These observations highlight that, while the prepulse approach is constrained by spectral bandwidth, the DP method provides a more versatile and reliable route to manipulate the coherent optical response of inhomogeneous ensembles. We are hoping these findings might stimulate further research in optical switching and coherent storage for quantum memory devices using inhomogeneous ensembles.

DOI
10.48550/arxiv.2601.05753

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Controlling the coherent optical response of inhomogeneous ensembles is a key challenge in advancing light-matter interaction engineering. We present a comparative study of two spectral tailoring approaches using two-dimensional coherent spectroscopy (2DCS): the prepulse and double-pulse (DP) methods. In the prepulse scheme, a high-intensity pulse induces Rabi oscillations, modulating the 2D spectral amplitude and lineshape when its spectral bandwidth matches the ensemble full width at half maximum (FWHM). To overcome this limitation, the DP method employs variable inter-pulse delay to generate predetermined periodic spectral modulation without bandwidth constraints. Moreover, tuning the relative phase between DP pulses allows selective switching of frequency components, enabling controlled enhancement or suppression of distinct spectral features. These observations highlight that, while the prepulse approach is constrained by spectral bandwidth, the DP method provides a more versatile and reliable route to manipulate the coherent optical response of inhomogeneous ensembles. We are hoping these findings might stimulate further research in optical switching and coherent storage for quantum memory devices using inhomogeneous ensembles.
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Coherent control of a strongly inhomogeneously broadened system, namely, InAs self-assembled quantum dots, is demonstrated. To circumvent the deleterious effects of the inhomogeneous broadening, which usually masks the results of coherent manipulation, we use prepulse two-dimensional coherent spectroscopy to provide a size-selective readout of the ground, exciton, and biexciton states. The dependence on the timing of the prepulse is due to the dynamics of the coherently generated populations. To further validate the results, we performed prepulse polarization dependent measurements and confirmed the behavior expected from selection rules. All measured spectra can be excellently reproduced by solving the optical Bloch equations for a 4-level system.
Inhomogeneous broadening in ensembles of semiconductor quantum dots (QDs) has hindered coherent operations due to the detuning effects, caused by the large fluctuation in the QD transition energy due to size dispersion. This difficulty is especially evident when using femtosecond laser pulses for excitation. Here, the authors successfully measure detuning-dependent coherent evolution for a QD ensemble by employing prepulse two-dimensional coherent spectroscopy. The dephasing mechanism is found to be significantly different from that observed using picosecond lasers. This work presents a novel method to explore collective phenomena, such as superfluorescence, as well as motivating future studies of coherent interactions in the femtosecond regime.
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We propose to employ multi-color narrow-bandwidth pulses to dissect the quantum pathways in two-dimensional correlation spectroscopy (2DCS) optical signals generated along the phase-matching directions k I = − k 1 + k 2 + k 3 (photon echo) and k III = k 1 + k 2 − k 3 (double quantum coherence). Simulations demonstrate how the resolution of 2DCS signals in GaAs quantum wells may be enhanced by spectrally selecting desired Liouville-space pathways. Pulse-shaping techniques may be used to further enhance the resolution.
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