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Title: Disentangling interface and bulk contributions to high-harmonic emission from solids

Abstract

Due to strong absorption of above-bandgap high harmonics generated from solids, the surface should play an important role. However, surface-induced contributions have yet to be identified. In this work, we show that the presence of the interface between a Si crystal and a native SiO 2 layer is encoded in the appearance of weak even-order high harmonics. The even harmonics arise from a surface-induced static space charge that perturbs the laser-driven motion of electrons and holes in the bulk of the material. Our demonstration extends surface-induced nonlinear optical effects to the non-perturbative regime, characterized by unbound large-amplitude motion of charge carriers, and therefore paves the way for new methodologies to probe surfaces and their chemistry.

Authors:
; ORCiD logo; ;
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE; US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1508876
Alternate Identifier(s):
OSTI ID: 1532489
Grant/Contract Number:  
AC02-76SF00515; FA9550-14-1-0108
Resource Type:
Journal Article: Published Article
Journal Name:
Optica
Additional Journal Information:
Journal Name: Optica Journal Volume: 6 Journal Issue: 5; Journal ID: ISSN 2334-2536
Publisher:
Optical Society of America
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Vampa, Giulio, Liu, Hanzhe, Heinz, Tony F., and Reis, David A. Disentangling interface and bulk contributions to high-harmonic emission from solids. United States: N. p., 2019. Web. doi:10.1364/OPTICA.6.000553.
Vampa, Giulio, Liu, Hanzhe, Heinz, Tony F., & Reis, David A. Disentangling interface and bulk contributions to high-harmonic emission from solids. United States. doi:10.1364/OPTICA.6.000553.
Vampa, Giulio, Liu, Hanzhe, Heinz, Tony F., and Reis, David A. Fri . "Disentangling interface and bulk contributions to high-harmonic emission from solids". United States. doi:10.1364/OPTICA.6.000553.
@article{osti_1508876,
title = {Disentangling interface and bulk contributions to high-harmonic emission from solids},
author = {Vampa, Giulio and Liu, Hanzhe and Heinz, Tony F. and Reis, David A.},
abstractNote = {Due to strong absorption of above-bandgap high harmonics generated from solids, the surface should play an important role. However, surface-induced contributions have yet to be identified. In this work, we show that the presence of the interface between a Si crystal and a native SiO2 layer is encoded in the appearance of weak even-order high harmonics. The even harmonics arise from a surface-induced static space charge that perturbs the laser-driven motion of electrons and holes in the bulk of the material. Our demonstration extends surface-induced nonlinear optical effects to the non-perturbative regime, characterized by unbound large-amplitude motion of charge carriers, and therefore paves the way for new methodologies to probe surfaces and their chemistry.},
doi = {10.1364/OPTICA.6.000553},
journal = {Optica},
issn = {2334-2536},
number = 5,
volume = 6,
place = {United States},
year = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1364/OPTICA.6.000553

Figures / Tables:

Fig. 1 Fig. 1: Measured high-harmonic spectra from a Si film facing the incident beam in (a) transmission and (b) reflection for a p-polarized driver and for (c) the sapphire substrate facing the incident beam in transmission for a p-polarized (blue line) and s-polarized (red line) driver. Weak even harmonics are onlymore » detected for p polarization when the Si film faces the detector. The powers of the second and third harmonics are unrelated to those of the higher harmonics because they are measured with a different spectrometer with non-overlapping spectra. (d) The power of the even harmonics (colored lines) saturates with the intensity of the driver, contrary to the odd harmonics (gray lines). (e) Real-time acquisition of the seventh and eighth harmonics for alternate illumination of two adjacent regions of the Si film (one region is marked by the blue dot and the other by the red dot). The sample is laterally translated between these two regions at the times marked by the colored dots. The fundamental beam is blocked when the power is zero. The evenharmonic power shows a transient behavior developing over ∼1 sec , contrary to the odd harmonics. Data in panels (d) and (e) is acquired in the configuration of panel (c) with p-polarized light.« less

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Works referenced in this record:

Surface nonlinear optics: a historical overview
journal, March 1999


Linking high harmonics from gases and solids
journal, June 2015


Generation and propagation of high-order harmonics in crystals
journal, April 2012


Measurement of the Berry curvature of solids using high-harmonic spectroscopy
journal, March 2018


Optical-field-induced current in dielectrics
journal, December 2012

  • Schiffrin, Agustin; Paasch-Colberg, Tim; Karpowicz, Nicholas
  • Nature, Vol. 493, Issue 7430
  • DOI: 10.1038/nature11567

Observation of high-order harmonic generation in a bulk crystal
journal, December 2010

  • Ghimire, Shambhu; DiChiara, Anthony D.; Sistrunk, Emily
  • Nature Physics, Vol. 7, Issue 2
  • DOI: 10.1038/nphys1847

Extreme ultraviolet high-harmonic spectroscopy of solids
journal, May 2015

  • Luu, T. T.; Garg, M.; Kruchinin, S. Yu.
  • Nature, Vol. 521, Issue 7553
  • DOI: 10.1038/nature14456

Electron Photoinjection from Silicon to Ultrathin Si O 2 Films via Ambient Oxygen
journal, July 1996


Real-time observation of interfering crystal electrons in high-harmonic generation
journal, July 2015

  • Hohenleutner, M.; Langer, F.; Schubert, O.
  • Nature, Vol. 523, Issue 7562
  • DOI: 10.1038/nature14652

Optical Second-Harmonic Generation in Reflection from Media with Inversion Symmetry
journal, October 1968


Anisotropic high-harmonic generation in bulk crystals
journal, November 2016

  • You, Yong Sing; Reis, David A.; Ghimire, Shambhu
  • Nature Physics, Vol. 13, Issue 4
  • DOI: 10.1038/nphys3955

Time-dependent second-harmonic generation from the Si–SiO_2 interface induced by charge transfer
journal, January 1995


Semiclassical analysis of high harmonic generation in bulk crystals
journal, February 2015


Multipolar molecules and multipolar fields: probing and controlling the tensorial nature of nonlinear molecular media
journal, January 1998

  • Brasselet, S.; Zyss, J.
  • Journal of the Optical Society of America B, Vol. 15, Issue 1
  • DOI: 10.1364/JOSAB.15.000257

Charge-carrier dynamics and trap generation in native S i / S i O 2 interfaces probed by optical second-harmonic generation
journal, April 2004


Nonperturbative harmonic generation in graphene from intense midinfrared pulsed light
journal, November 2017


Measuring and controlling the birth of attosecond XUV pulses
journal, October 2006

  • Dudovich, N.; Smirnova, O.; Levesque, J.
  • Nature Physics, Vol. 2, Issue 11
  • DOI: 10.1038/nphys434

Solid-state harmonics beyond the atomic limit
journal, June 2016

  • Ndabashimiye, Georges; Ghimire, Shambhu; Wu, Mengxi
  • Nature, Vol. 534, Issue 7608
  • DOI: 10.1038/nature17660

High harmonic generation in the relativistic limit
journal, July 2006

  • Dromey, B.; Zepf, M.; Gopal, A.
  • Nature Physics, Vol. 2, Issue 7
  • DOI: 10.1038/nphys338

Plasma mirrors for ultrahigh-intensity optics
journal, April 2007

  • Thaury, C.; Quéré, F.; Geindre, J. -P.
  • Nature Physics, Vol. 3, Issue 6
  • DOI: 10.1038/nphys595

All-Optical Reconstruction of Crystal Band Structure
journal, November 2015


High-harmonic generation from an atomically thin semiconductor
journal, November 2016

  • Liu, Hanzhe; Li, Yilei; You, Yong Sing
  • Nature Physics, Vol. 13, Issue 3
  • DOI: 10.1038/nphys3946

Sub-cycle control of terahertz high-harmonic generation by dynamical Bloch oscillations
journal, January 2014


Surface properties probed by second-harmonic and sum-frequency generation
journal, February 1989


Growth of native oxide on a silicon surface
journal, August 1990

  • Morita, M.; Ohmi, T.; Hasegawa, E.
  • Journal of Applied Physics, Vol. 68, Issue 3, p. 1272-1281
  • DOI: 10.1063/1.347181

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.