Coherent multidimensional spectroscopy of dilute gas-phase nanosystems.

Bruder, Lukas; Bangert, Ulrich; Binz, Marcel; Uhl, Daniel; Vexiau, Romain; Bouloufa-Maafa, Nadia; Dulieu, Olivier; Stienkemeier, Frank · Nat Commun · 2018

basic_science · Level V

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Abstract

Two-dimensional electronic spectroscopy (2DES) is one of the most powerful spectroscopic techniques with unique sensitivity to couplings, coherence properties and real-time dynamics of a quantum system. While successfully applied to a variety of condensed phase samples, high precision experiments on isolated systems in the gas phase have been so far precluded by insufficient sensitivity. However, such experiments are essential for a precise understanding of fundamental mechanisms and to avoid misinterpretations. Here, we solve this issue by extending 2DES to isolated nanosystems in the gas phase prepared by helium nanodroplet isolation in a molecular beam-type experiment. This approach uniquely provides high flexibility in synthesizing tailored, quantum state-selected model systems of single and many-body character. In a model study of weakly-bound Rb<sub>2</sub> and Rb<sub>3</sub> molecules we demonstrate the method's unique capacity to elucidate interactions and dynamics in tailored quantum systems, thereby also bridging the gap to experiments in ultracold quantum science.