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.
@article{arxiv.2006.13559,
title = {Revealing a full quantum ladder by nonlinear spectroscopy},
author = {Darius Abramavicius},
journal= {arXiv preprint arXiv:2006.13559},
year = {2020}
}