Revealing a full quantum ladder by nonlinear spectroscopy

Abstract

Coherent two-dimensional spectroscopy in IR or visible region is very effective for studying correlations, energy relaxation/transfer pathways in complex multi-chromophore or multi-mode systems. However it is usually restricted up to two-quanta excitations and their properties. In this paper an arbitrary level of excitation is suggested as the utility to scan nonlinear potential surfaces of quantum systems up to a desired excitation degree. This can be achieved by a simple three-pulse laser spectroscopy approach. Accurate evaluation of high-level anharmonicities as well as transition amplitudes can be directly obtained. Additionally, questions regarding the quantum nature of the probed system can be addressed by studying absolute peak positions.

arXiv comment11 pages, 4 figures, original manuscript

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