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Photons can excite collective and single-particle excitations in metals; the collective plasmonic excitations are of keen interest in physics, chemistry, optics, and nanotechnology because they enhance coupling of electromagnetic energy and can drive nonlinear processes in electronic materials, particularly where their dielectric function ϵ(ω) approaches zero. We investigate the nonlinear angle-resolved two-photon photoemission (2PP) spectroscopy of the Ag(111) surface through the ϵ(ω) near-zero region. In addition to the Einsteinian single-particle photoemission, the 2PP spectra report unequivocal signatures of nonlocal dielectric, plasmonically enhanced, excitation processes.
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http://dx.doi.org/10.1103/PhysRevLett.123.017404 | DOI Listing |
Phys Rev Lett
July 2019
Department of Physics and Astronomy and Pittsburgh Quantum Institute, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, USA.
Photons can excite collective and single-particle excitations in metals; the collective plasmonic excitations are of keen interest in physics, chemistry, optics, and nanotechnology because they enhance coupling of electromagnetic energy and can drive nonlinear processes in electronic materials, particularly where their dielectric function ϵ(ω) approaches zero. We investigate the nonlinear angle-resolved two-photon photoemission (2PP) spectroscopy of the Ag(111) surface through the ϵ(ω) near-zero region. In addition to the Einsteinian single-particle photoemission, the 2PP spectra report unequivocal signatures of nonlocal dielectric, plasmonically enhanced, excitation processes.
View Article and Find Full Text PDFACS Nano
July 2018
Department of Physics and Astronomy and Pittsburgh Quantum Institute , University of Pittsburgh, Pittsburgh , Pennsylvania 15260 , United States.
Using two-photon photoemission electron microscopy (2P-PEEM) we image the polarization dependence of coupling and propagation of surface plasmon polaritons (SPPs) launched from edges of a triangular, micrometer size, single-crystalline Ag crystal by linearly or circularly polarized light. 2P-PEEM records interferences between the optical excitation field and SPPs it creates with nanofemto space-time resolution. Both the linearly and circularly polarized femtosecond light pulses excite spatially asymmetric 2PP yield distributions, which are imaged.
View Article and Find Full Text PDFJ Am Chem Soc
May 2017
Department of Physics and Astronomy and Pittsburgh Quantum Institute, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States.
Hot electron processes at metallic heterojunctions are central to optical-to-chemical or electrical energy transduction. Ultrafast nonlinear photoexcitation of graphite (Gr) has been shown to create hot thermalized electrons at temperatures corresponding to the solar photosphere in less than 25 fs. Plasmonic resonances in metallic nanoparticles are also known to efficiently generate hot electrons.
View Article and Find Full Text PDFJ Chem Theory Comput
May 2014
Nano-Bio Spectroscopy Group and ETSF Scientific Development Center, Departamento de Física de Materiales, Centro de Física de Materiales CSIC-UPV/EHU-MPC and DIPC, Universidad del País Vasco UPV/EHU , E-20018 San Sebastián, Spain.
Electronic level alignment at the interface between an adsorbed molecular layer and a semiconducting substrate determines the activity and efficiency of many photocatalytic materials. Standard density functional theory (DFT)-based methods have proven unable to provide a quantitative description of this level alignment. This requires a proper treatment of the anisotropic screening, necessitating the use of quasiparticle (QP) techniques.
View Article and Find Full Text PDFAcc Chem Res
May 2011
Department of Physics and Astronomy, Petersen Institute of NanoScience and Engineering, University of Pittsburgh, Pennsylvania 15260, United States.
Electronic and optical properties of molecules and molecular solids are traditionally considered from the perspective of the frontier orbitals and their intermolecular interactions. How molecules condense into crystalline solids, however, is mainly attributed to the long-range polarization interaction. In this Account, we show that long-range polarization also introduces a distinctive set of diffuse molecular electronic states, which in quantum structures or solids can combine into nearly-free-electron (NFE) bands.
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