We simulate semiclassically angular momentum transfer for a molecular system subject to a circularly polarized light (CPL) field either moving along a single Born-Oppenheimer (BO) surface or moving along multiple BO surfaces. Both sets of simulations are able to conserve the total angular momentum around the propagation direction of the CPL field, the former requiring a Berry force and the latter requiring a surface parametrized by both nuclear position and momentum (a so-called phase-space approach). Our results provide new insight into the nature of semiclassical nonadiabatic dynamics methods and further demonstrate the power of such methods to capture angular momentum transfer between different media, highlighting the need for accurate algorithms that conserve the total angular momentum.
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http://dx.doi.org/10.1021/acs.jctc.4c00225 | DOI Listing |
J Chem Phys
January 2025
Department of Chemistry, University of British Columbia, Vancouver, British Columbia V6T 1Z1, Canada.
We present an algorithm that combines quantum scattering calculations with probabilistic machine-learning models to predict quantum dynamics rate coefficients for a large number of state-to-state transitions in molecule-molecule collisions much faster than with direct solutions of the Schrödinger equation. By utilizing the predictive power of Gaussian process regression with kernels, optimized to make accurate predictions outside of the input parameter space, the present strategy reduces the computational cost by about 75%, with an accuracy within 5%. Our method uses temperature dependences of rate coefficients for transitions from the isolated states of initial rotational angular momentum j, determined via explicit calculations, to predict the temperature dependences of rate coefficients for other values of j.
View Article and Find Full Text PDFNat Commun
January 2025
Department of Optics and Optical Engineering, University of Science and Technology of China, Hefei, China.
The spin angular momentum (SAM) plays a significant role in light-matter interactions. It is well known that light carrying SAM can exert optical torques on micro-objects and drive rotations, but 3D rotation around an arbitrary axis remains challenging. Here, we demonstrate full control of the 3D optical torque acting on a trapped microparticle by tailoring the vectorial SAM transfer.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
January 2025
Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012 China. Electronic address:
The line list is essential for accurately modeling various astrophysical phenomena, such as stellar photospheres and atmospheres of extrasolar planets. This paper introduces a new line database for the PS molecule spanning from the ultraviolet to the infrared regions, covering wavenumbers up to 45000 cm and containing over ten million transitions between 150,458 states with total angular momentum J < 160. Accurate line intensities for rotational, vibrational and electronic transitions are generated by using the general purpose variational code DUO.
View Article and Find Full Text PDFSensors (Basel)
December 2024
Research Center of Applied Electromagnetics, Nanjing University of Information Science and Technology, Nanjing 210044, China.
We present a novel photoreconfigurable metasurface designed for independent and efficient control of electromagnetic waves with identical incident polarization and frequency across the entire spatial domain. The proposed metasurface features a three-layer architecture: a top layer incorporating a gold circular split ring resonator (CSRR) filled with perovskite material and dual -shaped perovskite resonators; a middle layer of polyimide dielectric; and a bottom layer comprising a perovskite substrate with an oppositely oriented circular split ring resonator filled with gold. By modulating the intensity of a laser beam, we achieve autonomous manipulation of incident circularly polarized terahertz waves in both transmission and reflection modes.
View Article and Find Full Text PDFSci Adv
January 2025
Center for Nano Science and Technology, Fondazione Istituto Italiano di Tecnologia, Milano, Italy.
Achieving highly tailored control over both the spatial and temporal evolution of light's orbital angular momentum (OAM) on ultrafast timescales remains a critical challenge in photonics. Here, we introduce a method to modulate the OAM of light on a femtosecond scale by engineering a space-time coupling in ultrashort pulses. By linking azimuthal position with time, we implement an azimuthally varying Fourier transformation to dynamically alter light's spatial distribution in a fixed transverse plane.
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