[1] Coherent nonlinear optical response for high-intensity excitation, R. Tripathi, K. K. Maurya, P. Kumar, B. De, and R. Singh, J. Chem. Phys. 162, 114111 (2025). DOI Special Collection: David Jonas Festschrift
The coherent optical response of materials plays a crucial role in advancing quantum information applications. Two-dimensional coherent spectroscopy (2DCS) serves as a powerful tool for investigating these properties across a wide range of systems. Traditionally, such experiments are conducted in the low-excitation regime, mainly due to theoretical challenges in interpreting data at high excitation intensities. In this work, we present a technique that enables exact calculations of 2D spectra even in the high-intensity regime. Our simulations are used to model experiments on semiconductor nanostructures, including both our own measurements and previously reported results from other research groups. These findings are highly relevant for researchers conducting spectroscopy with intense light fields.
[2] Quantitative Line shape Analysis for Arbitrary Inhomogeneity in 2D Coherent Spectroscopy, B. De, P. Kumar, K. K. Maurya, R. Tripathi, and R. Singh, Opt. Lett. 50, 4502 (2025). DOI
This work presents a novel framework for analyzing two-dimensional coherent spectroscopy (2DCS) data beyond the conventional assumption of Gaussian inhomogeneity. By introducing a bivariate spectral distribution function (BSDF), we demonstrate the extraction of homogeneous and arbitrary inhomogeneous linewidths from experimental 2D spectra. This method was applied to GaAs quantum dot samples, revealing non-Gaussian inhomogeneous broadening and enabling accurate spectral diffusion analysis.
Coherent Control through High-Intensity Excitation: A Simulation of Two-Dimensional Coherent Spectroscopy, R. Tripathi, K. K. Maurya, and R. Singh, Conference on Lasers and Electro-Optics/Pacific Rim, Optica Publishing Group, 2024.