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Title: Above-threshold multiphoton photoemission from noble metal surfaces

Abstract

Exciting solids with intense femtosecond laser pulses prompts electrons of the interrogated material to respond in a highly nonlinear manner, as is evident in the emission of high-order harmonic radiation and photoelectrons with kinetic energies well above that of the driving photons. Such high-field interactions can be resolved, for example, in above-threshold multiphoton photoemission (ATP) spectroscopy. In this work, we interrogate the nonlinear photoelectric responses of the pristine copper, silver, and gold noble metal surfaces in (111) and (100) crystal orientations in the perturbative regime. Using multiphoton photoemission spectroscopy (mPP) excited by finely tuned optical fields, we characterize enhancement of the mPP and ATP yields from (111) surfaces in selected k||-momentum ranges when the occupied Shockley surface (SS) states are (near-)resonantly coupled by multiphoton transitions to image potential (IP) intermediate states in the excitation process. The ATP signal from the IP states of (111) surfaces is largely defined by their formation through polarization of SS electrons; this observation is contrasted with ATP experiments from the Ag(100) surface, for which the SS becomes an unoccupied resonance and the IP states can only be excited from bands with significantly more bulk character. In addition, based on the optical power and nonlinear order-dependentmore » mPP spectra, we provide evidence for ATP being a one-step, rather than a sequential process, as previously postulated.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2]
  1. Univ. of Pittsburgh, PA (United States). Dept. of Physics and Astronomy and Pittsburgh Quantum Institute; I. Georg-August-Universität Göttingen (Germany). Physikalisches Institut
  2. Univ. of Pittsburgh, PA (United States). Dept. of Physics and Astronomy and Pittsburgh Quantum Institute
Publication Date:
Research Org.:
Univ. of Pittsburgh, PA (United States). Condensed Phase and Interfacial Molecular Science (CPIMS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Alexander von Humboldt Foundation
OSTI Identifier:
1598264
Grant/Contract Number:  
SC0002313
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 101; Journal Issue: 7; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 74 ATOMIC AND MOLECULAR PHYSICS; nonlinear optics, Floquet engineering, above threshold photomiession

Citation Formats

Reutzel, Marcel, Li, Andi, and Petek, Hrvoje. Above-threshold multiphoton photoemission from noble metal surfaces. United States: N. p., 2020. Web. doi:10.1103/PhysRevB.101.075409.
Reutzel, Marcel, Li, Andi, & Petek, Hrvoje. Above-threshold multiphoton photoemission from noble metal surfaces. United States. doi:https://doi.org/10.1103/PhysRevB.101.075409
Reutzel, Marcel, Li, Andi, and Petek, Hrvoje. Thu . "Above-threshold multiphoton photoemission from noble metal surfaces". United States. doi:https://doi.org/10.1103/PhysRevB.101.075409. https://www.osti.gov/servlets/purl/1598264.
@article{osti_1598264,
title = {Above-threshold multiphoton photoemission from noble metal surfaces},
author = {Reutzel, Marcel and Li, Andi and Petek, Hrvoje},
abstractNote = {Exciting solids with intense femtosecond laser pulses prompts electrons of the interrogated material to respond in a highly nonlinear manner, as is evident in the emission of high-order harmonic radiation and photoelectrons with kinetic energies well above that of the driving photons. Such high-field interactions can be resolved, for example, in above-threshold multiphoton photoemission (ATP) spectroscopy. In this work, we interrogate the nonlinear photoelectric responses of the pristine copper, silver, and gold noble metal surfaces in (111) and (100) crystal orientations in the perturbative regime. Using multiphoton photoemission spectroscopy (mPP) excited by finely tuned optical fields, we characterize enhancement of the mPP and ATP yields from (111) surfaces in selected k||-momentum ranges when the occupied Shockley surface (SS) states are (near-)resonantly coupled by multiphoton transitions to image potential (IP) intermediate states in the excitation process. The ATP signal from the IP states of (111) surfaces is largely defined by their formation through polarization of SS electrons; this observation is contrasted with ATP experiments from the Ag(100) surface, for which the SS becomes an unoccupied resonance and the IP states can only be excited from bands with significantly more bulk character. In addition, based on the optical power and nonlinear order-dependent mPP spectra, we provide evidence for ATP being a one-step, rather than a sequential process, as previously postulated.},
doi = {10.1103/PhysRevB.101.075409},
journal = {Physical Review B},
number = 7,
volume = 101,
place = {United States},
year = {2020},
month = {2}
}

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