Coherent multidimensional spectroscopy of dilute gas-phase nanosystems

Abstract

Two-dimensional electronic spectroscopy (2DES) is one of the most powerful spectroscopic techniques, capable of attaining a nearly complete picture of a quantum system including its couplings, quantum coherence properties and its real-time dynamics. While successfully applied to a variety of condensed phase samples, high precision experiments on isolated quantum 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, e.g. as for the nature of quantum coherences in energy trans-port. 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 properties. For demonstration, we deduce a precise and conclusive picture of the ultrafast coherent dynamics in isolated high-spin Rb2 molecules and present for the first time a dynamics study of the system-bath interaction between a single molecule (here Rb3) and a superfluid helium environment. The results demonstrate the unique capacity to elucidate prototypical interactions and dynamics in tailored quantum systems and bridges the gap to experiments in ultracold quantum science.

References in corpus (10)

• Origin of Long Lived Coherences in Light-Harvesting Complexes
• Spectroscopy and dynamics in helium nanodroplets
• Density Functional Theory of doped superfluid liquid helium and nanodroplets
• Controlling a quantum gas of polar molecules in an optical lattice
• Vibronic Lineshapes of PTCDA Oligomers in Helium Nanodroplets
• Vibrational relaxation and dephasing of Rb2 attached to helium nanodroplets
• Phase-modulated electronic wave-packet interferometry reveals high resolution vibronic spectra of free Rb atoms and Rb*He molecules
• Homo- and heteronuclear alkali metal trimers formed on helium nanodroplets. II. Femtosecond spectroscopy and spectra assignments
• Polarizability of ultracold ${\text{Rb}}_2$ molecules in the rovibrational ground state of ${\mathrm{a}}^3{\Sigma }_u^{+}$
• Desorption Dynamics of Rb_2 Molecules off the Surface of Helium Nanodroplets

Cited by in corpus (17)

• Phase-Modulated Rapid-Scanning Fluorescence-Detected Two-Dimensional Electronic Spectroscopy
• Coherent multidimensional spectroscopy in the gas phase
• Long-lived nuclear coherences inside helium nanodroplets
• Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor
• A flexible and scalable, fully software-based lock-in amplifier for nonlinear spectroscopy
• High-resolution two-dimensional electronic spectroscopy reveals homogeneous line profiles in isolated nanoparticles
• Inelastic scattering of photoelectrons from He nanodroplets
• Phase cycling of extreme ultraviolet pulse sequences generated in rare gases
• Optical Two-dimensional Coherent Spectroscopy of Cold Atoms
• Revealing a full quantum ladder by nonlinear spectroscopy
• Two-dimensional electronic spectroscopy of an ultracold gas
• High-Gain Harmonic Generation with temporally overlapping seed pulses and application to ultrafast spectroscopy
• Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy
• Improved stabilization scheme for extreme ultraviolet quantum interference experiments
• Background-free measurement of exciton-exciton annihilation by two-quantum fluorescence-detected pump-probe spectroscopy
• Disentangling Single- and Biexciton Dynamics with Photoelectron-Detected Two-Dimensional Electronic Spectroscopy
• Low-dispersive phase-modulated rapid scanning interferometry