We investigate the role played by electron-hole pair and phonon excitations in the interaction of reactive gas molecules and atoms with metal surfaces. We present a theoretical framework that allows us to evaluate within a full-dimensional dynamics the combined contribution of both excitation mechanisms while the gas particle-surface interaction is described by an ab initio potential energy surface. The model is applied to study energy dissipation in the scattering of N(2) on W(110) and N on Ag(111). Our results show that phonon excitation is the dominant energy loss channel, whereas electron-hole pair excitations represent a minor contribution. We substantiate that, even when the energy dissipated is quantitatively significant, important aspects of the scattering dynamics are well captured by the adiabatic approximation.
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http://dx.doi.org/10.1103/PhysRevLett.108.096101 | DOI Listing |
Phys Rev Lett
December 2024
Radboud University Nijmegen, Institute for Molecules and Materials, 6525 AJ, Nijmegen, The Netherlands.
Resonant pumping of the electronic f-f transitions in the orbital multiplet of dysprosium ions (Dy^{3+}) in a complex perovskite DyFeO_{3} is shown to impulsively launch THz lattice dynamics corresponding to the B_{2g} phonon mode, which is dominanted by the motion of Dy^{3+} ions. The findings, supported by symmetry analysis and density-functional theory calculations, not only provide a novel route for highly selective excitation of the rare-earth crystal lattices but also establish important relationships between the symmetry of the electronic and lattice excitations in complex oxides.
View Article and Find Full Text PDFPhys Rev Lett
December 2024
International Center for Quantum Materials, School of Physics, Peking University, Beijing 100871, China.
Sci Rep
January 2025
Instituto de Alta Investigación, Universidad de Tarapacá, 1000000, Arica, Chile.
CuZnSn(S,Se) (CZT(S,Se)) thin films exhibit the characteristics necessary to be effective absorbers in solar cells. In this report, the room temperature experimental Raman scattering spectra, recorded at different excitation wavelengths, are systematically analyzed theoretically using the results of DFT harmonic frequencies calculations at the Γ-point for various modifications of kesterite (KS), stannite (ST), and pre-mixed Cu-Au (PMCA) crystal structures. The specific anharmonism-induced features in the spectra of CZT(S,Se) crystals are identified, and the spectral lineshapes at varied strengths of anharmonic interaction are simulated.
View Article and Find Full Text PDFACS Appl Opt Mater
December 2024
Department of Physics, Umeå University, Linnaeus väg 24, 901 87 Umeå, Sweden.
Multilayered metal-dielectric nanostructures display both a strong plasmonic behavior and hyperbolic optical dispersion. The latter is responsible for the appearance of two separated radiative and nonradiative channels in the extinction spectrum of these structures. This unique property can open plenty of opportunities toward the development of multifunctional systems that simultaneously can behave as optimal scatterers and absorbers at different wavelengths, an important feature to achieve multiscale control of light-matter interactions in different spectral regions for different types of applications, such as optical computing or detection of thermal radiation.
View Article and Find Full Text PDFACS Nano
December 2024
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
Ultrafast thermal switches are pivotal for managing heat generated in advanced solid-state applications, including high-speed chiplets, thermo-optical modulators, and on-chip lasers. However, conventional phonon-based switches cannot meet the demand for picosecond-level response times, and existing near-field radiative thermal switches face challenges in efficiently modulating heat transfer across vacuum gaps. To overcome these limitations, we propose an ultrafast thermal switch design based on pump-driven transient polaritons in asymmetric terminals.
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