Through coherent excitation of a pair of vibronically coupled eigenlevels, an oscillation of 130 kcal/mol in energy excitation between electronic and vibrational motions (on a time scale of 10 s) is created for the triatomic molecule, sulfur dioxide (SO). The reactivity of the molecule can be influenced depending upon whether the molecule is vibrationally or electronically excited with this substantial amount of energy. The effect of excitation on reactivity is demonstrated through SO photodissociation as a function of time following coherent excitation, monitored by multiphoton ionization of the SO product.
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http://dx.doi.org/10.1021/acs.jpca.1c05778 | DOI Listing |
Nanomaterials (Basel)
December 2024
Theoretical Physical Chemistry, UR MOLSYS, University of Liege, B4000 Liège, Belgium.
Dynamical symmetries, time-dependent operators that almost commute with the Hamiltonian, extend the role of ordinary symmetries. Motivated by progress in quantum technologies, we illustrate a practical algebraic approach to computing such time-dependent operators. Explicitly we expand them as a linear combination of time-independent operators with time-dependent coefficients.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Physics, Stockholm University, AlbaNova University Center, SE-10691 Stockholm, Sweden.
Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical reactivity. However, the interactions in a molecular ensemble are complex, and the exact mechanisms that lead to modifications are not fully understood yet.
View Article and Find Full Text PDFJ Magn Reson
December 2024
Univ. Lille, CNRS, Centrale Lille, Univ. Artois, UMR 8181, UCCS - Unité de Catalyse et Chimie du Solide, F-59000 Lille, France. Electronic address:
The two-dimensional (2D) refocused INADEQUATE NMR experiment, which correlates double-quantum (DQ) and single-quantum (SQ) coherences, is widely used to probe the chemical connectivities in solids. Nevertheless, the multiplets along the F dimension reduce the resolution and sensitivity of this experiment. The Composite-Refocusing (CR) technique with two excitation pulses has been proposed to suppress these multiplets in 2D INADEQUATE spectra of liquids.
View Article and Find Full Text PDFIn doped semiconductors such as monolayer transition-metal dichalcogenides (TMDs), the optical properties are predominantly determined by exciton polarons, which are coherent superpositions of excitons and electron-hole excitation pairs in the Fermi sea. Here, we theoretically study the effect of exciton polarons on thermal radiation in doped two-dimensional semiconductors. By deriving an emissivity formula in terms of the dielectric function and the thickness of two-dimensional semiconductors, we show that the emissivity spectrum exhibits a narrow peak at the energy of an exciton polaron.
View Article and Find Full Text PDFCommun Phys
December 2024
LaserLaB, Department of Physics and Astronomy, Vrije Universiteit Amsterdam, De Boelelaan 1081, 1081 HV Amsterdam, the Netherlands.
Laser spectroscopy of atomic hydrogen and hydrogen-like atoms is a powerful tool for tests of fundamental physics. The 1-2 transition of hydrogen in particular is a cornerstone for stringent Quantum Electrodynamics (QED) tests and for an accurate determination of the Rydberg constant. We report laser excitation of the 1-2 transition in singly-ionized helium (He), a hydrogen-like ion with much higher sensitivity to QED than hydrogen itself.
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