Coherent multidimensional spectroscopy of dilute gas-phase nanosystems

Lukas Bruder (), Ulrich Bangert, Marcel Binz, Daniel Uhl, Romain Vexiau, Nadia Bouloufa-Maafa, Olivier Dulieu and Frank Stienkemeier
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Lukas Bruder: University of Freiburg
Ulrich Bangert: University of Freiburg
Marcel Binz: University of Freiburg
Daniel Uhl: University of Freiburg
Romain Vexiau: CNRS, Université Paris-Sud, ENS Cachan, Université Paris-Saclay
Nadia Bouloufa-Maafa: CNRS, Université Paris-Sud, ENS Cachan, Université Paris-Saclay
Olivier Dulieu: CNRS, Université Paris-Sud, ENS Cachan, Université Paris-Saclay
Frank Stienkemeier: University of Freiburg

Nature Communications, 2018, vol. 9, issue 1, 1-7

Abstract: 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 Rb2 and Rb3 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.

Date: 2018
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DOI: 10.1038/s41467-018-07292-w

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