Extreme ultraviolet frequency combs are a versatile tool with applications including precision measurement, strong-field physics, and solid-state physics. Here we report on an application of extreme ultraviolet frequency combs and their driving lasers for studying strong-field effects in molecular systems. We perform field-free molecular alignment and high-order harmonic generation with aligned molecules in a gas jet at a repetition rate of 154 MHz using a high-powered optical frequency comb inside a femtosecond enhancement cavity. The cavity-enhanced system provides a means to reach suitable intensities to study field-free molecular alignment and enhance the observable effects of the molecule-field interaction. We observe modulations of the driving field, arising from the nature of impulsive stimulated Raman scattering responsible for coherent molecular rotations. We foresee the impact of this work on the study of molecule-based strong-field physics, with improved precision and a more fundamental understanding of the interaction effects on both the field and molecules.
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http://dx.doi.org/10.1103/PhysRevLett.114.153001 | DOI Listing |
J Chem Phys
January 2025
Institute of Chemistry, ELTE Eötvös Loránd University, Pázmány Péter Sétány 1/A, H-1117 Budapest, Hungary.
Accurate rovibrational molecular models are employed to gain insight in high-resolution into the collective effects and intermolecular processes arising when molecules in the gas phase interact with a resonant infrared (IR) radiation mode. An efficient theoretical approach is detailed, and numerical results are presented for the HCl, H2O, and CH4 molecules confined in an IR cavity. It is shown that by employing a rotationally resolved model for the molecules, revealing the various cavity-mediated interactions between the field-free molecular eigenstates, it is possible to obtain a detailed understanding of the physical processes governing the energy level structure, absorption spectra, and dynamic behavior of the confined systems.
View Article and Find Full Text PDFSoft Matter
December 2024
UNAM-National Nanotechnology Research Center and Institute of Materials Science & Nanotechnology, Bilkent University, Ankara 06800, Turkey.
Polyelectrolyte hydrogels can deform under electric fields due to their unique nature combining polymer elasticity and electrostatics within a single structure. While the response of hydrogels to electric fields is relatively well-characterized at the macroscale, at the mesoscale-where the behaviour of the constituent chains becomes significant-the effect of external electric potentials on the hydrogel structure is poorly understood. In this study, we explored the mechanical response of a semi-infinite polyelectrolyte hydrogel slab to transient, sinusoidal electric fields using extensive coarse-grained molecular dynamics simulations with both short and long-range electrostatics.
View Article and Find Full Text PDFHum Brain Mapp
October 2024
Queen Mary School Hainan, Beijing University of Posts and Telecommunications, Hainan, China.
Macroscale functional gradient techniques provide a continuous coordinate system that extends from unimodal regions to transmodal higher-order networks. However, the alterations of these functional gradients in AD and their correlations with cognitive terms and gene expression profiles remain to be established. In the present study, we directly studied the functional gradients with functional MRI data from seven scanners.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Department of Organic Chemistry, University of Geneva, Geneva, Switzerland.
The control over the movement of electrons during chemical reactions with oriented external electric fields (OEEFs) has been predicted to offer a general approach to catalysis. Recently, we suggested that many problems to realize electric-field catalysis in practice under scalable bulk conditions could possibly be solved on multiwalled carbon nanotubes in electromicrofluidic reactors. Here, we selected monoterpene cyclizations to assess the scope of our system in organic synthesis.
View Article and Find Full Text PDFJ Chem Phys
September 2024
Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY, Notkestrasse 85, 22607 Hamburg, Germany.
We computationally studied the effect of nuclear-quadrupole interactions on the field-free impulsive alignment of different asymmetric-top molecules. Our analysis is focused on the influence of the hyperfine- and rotational-energy-level structures. These depend on the number of nuclear spins, the rotational constants, and the symmetry of the tensors involved in the nuclear spin and external field interactions.
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