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Conference on Lasers and Electro-Optics

Correlation effects in double-quantum multidimensional coherent spectroscopy

Bachana Lomsadze, Steven T. Cundiff

Published Jan 1, 2021• 0 citations
Publisher

Abstract

We investigate the correlation effects in double-quantum 2D spectroscopy by solving the optical Bloch equations. We also explain the discrepancies between the experimental results reported by multiple groups.
DOI
10.1364/cleo_at.2021.jtu3a.158

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Optical multidimensional coherent spectroscopy is a powerful tool for studying structure and dynamics in complex systems, such as semiconductors. In optical two-dimensional coherent spectroscopy (2DCS), where the spectrum is presented in a two-dimensional (2D) plane with two frequency axes, an important advantage is the ability to isolate quantum pathways by unfolding a one-dimensional spectrum onto a 2D plane. For many systems, however, the quantum pathways are only partially separated in a 2D spectrum. In order to completely isolate the quantum pathways, we extend 2DCS into a third dimension to generate three-dimensional (3D) spectra in which the spectrum is further unfolded. A 3D spectrum provides complete and well-isolated information of the third-order optical response of the system. The information can be used to fully characterize the quantum pathways and to determine the system’s Hamiltonian. Quantitative knowledge of the Hamiltonian enables prediction and control of quantum processes. For instance, such information is essential for deterministic control and improved performance of coherent control schemes.