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      Coherent multidimensional spectroscopy of dilute gas-phase nanosystems

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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 2 and Rb 3 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.

          Abstract

          Coherent multidimensional spectroscopy has greatly advanced our understanding of molecular dynamics but was so far broadly limited to complex condensed phase probes. Bruder et al. extend the method to isolated nanosystems in the gas phase and study cold molecules in a superfluid helium environment.

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          Most cited references38

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          Two-dimensional femtosecond spectroscopy.

          The simplest two-dimensional (2D) spectra show how excitation with one (variable) frequency affects the spectrum at all other frequencies, thus revealing the molecular connections between transitions. Femtosecond 2D Fourier transform (2D FT) spectra are more flexible and share some of the remarkable properties of their conceptual parent, 2D FT nuclear magnetic resonance. When 2D FT spectra are experimentally separated into real absorptive and imaginary refractive parts, the time resolution and frequency resolution can both reach the uncertainty limit set for each resonance by the sample itself. Coherent four-level contributions to the signal provide new molecular phase information, such as relative signs of transition dipoles. The nonlinear response can be picked apart by selecting a single coherence pathway (e.g., specifying the relative signs of energy level difference frequencies during different time intervals as in the photon echo). Because molecules are frozen on the femtosecond timescale, femtosecond 2D FT experiments can separate a distribution of instantaneous molecular environments and intramolecular geometries as inhomogeneous broadening. This review provides an introduction to two-dimensional Fourier transform experiments exploiting second- and third-order vibrational and electronic nonlinearities.
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            Superfluid Helium Droplets: A Uniquely Cold Nanomatrix for Molecules and Molecular Complexes

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              Coherent two-dimensional optical spectroscopy.

              M. Cho (2008)
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                Author and article information

                Contributors
                lukas.bruder@physik.uni-freiburg.de
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                16 November 2018
                16 November 2018
                2018
                : 9
                : 4823
                Affiliations
                [1 ]GRID grid.5963.9, Institute of Physics, , University of Freiburg, ; 79104 Freiburg, Germany
                [2 ]Laboratoire Aimé Cotton, CNRS, Université Paris-Sud, ENS Cachan, Université Paris-Saclay, 91405 Orsay Cedex, France
                [3 ]GRID grid.5963.9, Freiburg Institute of Advanced Studies (FRIAS), , University of Freiburg, ; Albertstr. 19 79194 Freiburg, Germany
                Author information
                http://orcid.org/0000-0001-9992-9925
                http://orcid.org/0000-0001-6014-8013
                Article
                7292
                10.1038/s41467-018-07292-w
                6240067
                30446649
                344eb82c-bd83-4ebd-b017-f68f5a8edf39
                © The Author(s) 2018

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 27 June 2018
                : 25 October 2018
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