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Title: Probing periodic potential of crystals via strong-field re-scattering

Abstract

Strong-field ionization and re-scattering phenomena have been used to image angstrom-scale structures of isolated molecules in the gas phase. These methods typically make use of the anisotropic response of the participating molecular orbital. Recently, an anisotropic strong-field response has also been observed in high-order harmonic generation (HHG) from bulk crystals. In a (100) cut magnesium oxide crystal, extreme ultraviolet high-harmonics are found to depend strongly on the crystal structure and inter-atomic bonding. Here, we extend these measurements to other two important crystal orientations: (111) and (110). We find that HHG from these orientations is also strongly anisotropic. The underlying dynamics is understood using a real-space picture, where high-harmonics are produced via coherent collision of strong-field driven electrons from the atomic sites, including from the nearest neighbor atoms. We find that harmonic efficiency is enhanced when semi-classical electron trajectories connect to the concentrated valence charge distribution regions around the atomic cores. Similarly, the efficiency is suppressed when the trajectories miss the atomic cores. Furthermore, these results further support the real-space picture of HHG with implications for retrieving the periodic potential of the crystal, if not the wavefunctions in three-dimensions.

Authors:
ORCiD logo [1];  [1];  [1];  [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1460994
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. B, Atomic, Molecular and Optical Physics
Additional Journal Information:
Journal Volume: 51; Journal Issue: 11; Journal ID: ISSN 0953-4075
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; ultrafast phenomenon; high-harmonics generation; strong-field physics

Citation Formats

You, Yong Sing, Cunningham, Eric, Reis, David A., and Ghimire, Shambhu. Probing periodic potential of crystals via strong-field re-scattering. United States: N. p., 2018. Web. doi:10.1088/1361-6455/aac11d.
You, Yong Sing, Cunningham, Eric, Reis, David A., & Ghimire, Shambhu. Probing periodic potential of crystals via strong-field re-scattering. United States. doi:10.1088/1361-6455/aac11d.
You, Yong Sing, Cunningham, Eric, Reis, David A., and Ghimire, Shambhu. Tue . "Probing periodic potential of crystals via strong-field re-scattering". United States. doi:10.1088/1361-6455/aac11d. https://www.osti.gov/servlets/purl/1460994.
@article{osti_1460994,
title = {Probing periodic potential of crystals via strong-field re-scattering},
author = {You, Yong Sing and Cunningham, Eric and Reis, David A. and Ghimire, Shambhu},
abstractNote = {Strong-field ionization and re-scattering phenomena have been used to image angstrom-scale structures of isolated molecules in the gas phase. These methods typically make use of the anisotropic response of the participating molecular orbital. Recently, an anisotropic strong-field response has also been observed in high-order harmonic generation (HHG) from bulk crystals. In a (100) cut magnesium oxide crystal, extreme ultraviolet high-harmonics are found to depend strongly on the crystal structure and inter-atomic bonding. Here, we extend these measurements to other two important crystal orientations: (111) and (110). We find that HHG from these orientations is also strongly anisotropic. The underlying dynamics is understood using a real-space picture, where high-harmonics are produced via coherent collision of strong-field driven electrons from the atomic sites, including from the nearest neighbor atoms. We find that harmonic efficiency is enhanced when semi-classical electron trajectories connect to the concentrated valence charge distribution regions around the atomic cores. Similarly, the efficiency is suppressed when the trajectories miss the atomic cores. Furthermore, these results further support the real-space picture of HHG with implications for retrieving the periodic potential of the crystal, if not the wavefunctions in three-dimensions.},
doi = {10.1088/1361-6455/aac11d},
journal = {Journal of Physics. B, Atomic, Molecular and Optical Physics},
number = 11,
volume = 51,
place = {United States},
year = {2018},
month = {5}
}

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Figures / Tables:

Figure 1 Figure 1: Crystallographic orientation dependence of high-harmonics in MgO crystal. (a) Strong, near infrared laser beam is focused to the sample at normal incidence. Estimated peak intensity at the focus is ~1013 W cm-2. The central wavelength of the laser is at 1.32 µm. High­-harmonics in extreme ultraviolet wavelength rangemore » are measured in transmission, limited by the acceptance angle of the spectrometer. For orientation dependence study the crystal is rotated to various angles (θ) about its normal. (b) Harmonics spectra obtained from (100)-cut MgO with laser polarized at along Mg-0 bond (0°) and O-O bond (45°).« less

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