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Torsional Wave-Packet Dynamics in 2-Fluorobiphenyl Investigated by State-Selective Ionization-Detected Impulsive Stimulated Raman Spectroscopy.
J Phys Chem A
June 2023
Department of Chemistry, School of Science, Tokyo Institute of Technology, Meguro 152-8550, Japan.
We report the creation and observation of vibrational wave packets pertinent to torsional motion in a biphenyl derivative in its electronic ground-state manifold. Adiabatically cooled molecular samples of 2-fluorobiphenyl were irradiated by intense nonresonant ultrashort laser pulses to drive impulsive stimulated Raman excitation of torsional motion. Spectral change due to the nonadiabatic vibrational excitation is probed in a state-selective manner using resonance-enhanced two-photon ionization through the S ← S electronic transition.
View Article and Find Full Text PDFOptical Control of the Resonant Dipole-Dipole Interaction between Rydberg Atoms.
Phys Rev Lett
August 2017
Laboratoire Charles Fabry, UMR 8501, Institut d'Optique, CNRS, Univ Paris Sud 11, 2 Avenue Augustin Fresnel, 91127 Palaiseau cedex, France.
We report on the local control of the transition frequency of a spin 1/2 encoded in two Rydberg levels of an individual atom by applying a state-selective light shift using an addressing beam. With this tool, we first study the spectrum of an elementary system of two spins, tuning it from a nonresonant to a resonant regime, where "bright" (super-radiant) and "dark" (subradiant) states emerge. We observe the collective enhancement of the microwave coupling to the bright state.
View Article and Find Full Text PDFAtom-diatom scattering dynamics of spinning molecules.
J Chem Phys
January 2015
Institut für Theoretische Physik, Leibniz Universität Hannover, 30167 Hannover, Germany.
We present full quantum mechanical scattering calculations using spinning molecules as target states for nuclear spin selective atom-diatom scattering of reactive D+H2 and F+H2 collisions. Molecules can be forced to rotate uni-directionally by chiral trains of short, non-resonant laser pulses, with different nuclear spin isomers rotating in opposite directions. The calculations we present are based on rotational wavepackets that can be created in this manner.
View Article and Find Full Text PDFDynamics of the A-band ultraviolet photodissociation of methyl iodide and ethyl iodide via velocity-map imaging with 'universal' detection.
Phys Chem Chem Phys
February 2015
Department of Chemistry, University of Oxford, Chemistry Research Laboratory, 12 Mansfield Rd, Oxford, OX1 3TA, UK.
We report data from a comprehensive investigation into the photodissociation dynamics of methyl iodide and ethyl iodide at several wavelengths in the range 236-266 nm, within their respective A-bands. The use of non-resonant single-photon ionization at 118.2 nm allows detection and velocity-map imaging of all fragments, regardless of their vibrotational or electronic state.
View Article and Find Full Text PDFVibrationally state-selective spin-orbit transfer with strong nonresonant pulses.
J Phys Chem A
April 2007
Departamento de Química Física, Universidad Complutense, 28040 Madrid, Spain.
By dynamic Stark shift using strong nonresonant pulses, we show that it is in principle possible to prepare arbitrary superposition states of mixed multiplicity. By a proper choice of parameters, the transfer of population is shown to follow the Rabi formula, where the initial and target states are now vibrational states of two light-induced molecular potentials of different multiplicity. Starting from nonstationary wave packets, the spin transfer can proceed via parallel transfer using a single pulse or by sequential transfer using a pulse sequence.
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