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Title: Soft X-Ray Second Harmonic Generation as an Interfacial Probe

Abstract

Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (~284 eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from the first atomic layer at the open surface. This technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.

Authors:
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Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1422881
Report Number(s):
NREL/JA-5K00-70998
Journal ID: ISSN 0031-9007; PRLTAO
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 2; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; nonlinear optics; interfaces; surfaces; x-ray techniques

Citation Formats

Lam, R. K., Raj, S. L., Pascal, T. A., Pemmaraju, C. D., Foglia, L., Simoncig, A., Fabris, N., Miotti, P., Hull, C. J., Rizzuto, A. M., Smith, J. W., Mincigrucci, R., Masciovecchio, C., Gessini, A., Allaria, E., De Ninno, G., Diviacco, B., Roussel, E., Spampinati, S., Penco, G., Di Mitri, S., Trovò, M., Danailov, M., Christensen, S. T., Sokaras, D., Weng, T. -C., Coreno, M., Poletto, L., Drisdell, W. S., Prendergast, D., Giannessi, L., Principi, E., Nordlund, D., Saykally, R. J., and Schwartz, C. P. Soft X-Ray Second Harmonic Generation as an Interfacial Probe. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.023901.
Lam, R. K., Raj, S. L., Pascal, T. A., Pemmaraju, C. D., Foglia, L., Simoncig, A., Fabris, N., Miotti, P., Hull, C. J., Rizzuto, A. M., Smith, J. W., Mincigrucci, R., Masciovecchio, C., Gessini, A., Allaria, E., De Ninno, G., Diviacco, B., Roussel, E., Spampinati, S., Penco, G., Di Mitri, S., Trovò, M., Danailov, M., Christensen, S. T., Sokaras, D., Weng, T. -C., Coreno, M., Poletto, L., Drisdell, W. S., Prendergast, D., Giannessi, L., Principi, E., Nordlund, D., Saykally, R. J., & Schwartz, C. P. Soft X-Ray Second Harmonic Generation as an Interfacial Probe. United States. doi:10.1103/PhysRevLett.120.023901.
Lam, R. K., Raj, S. L., Pascal, T. A., Pemmaraju, C. D., Foglia, L., Simoncig, A., Fabris, N., Miotti, P., Hull, C. J., Rizzuto, A. M., Smith, J. W., Mincigrucci, R., Masciovecchio, C., Gessini, A., Allaria, E., De Ninno, G., Diviacco, B., Roussel, E., Spampinati, S., Penco, G., Di Mitri, S., Trovò, M., Danailov, M., Christensen, S. T., Sokaras, D., Weng, T. -C., Coreno, M., Poletto, L., Drisdell, W. S., Prendergast, D., Giannessi, L., Principi, E., Nordlund, D., Saykally, R. J., and Schwartz, C. P. Mon . "Soft X-Ray Second Harmonic Generation as an Interfacial Probe". United States. doi:10.1103/PhysRevLett.120.023901.
@article{osti_1422881,
title = {Soft X-Ray Second Harmonic Generation as an Interfacial Probe},
author = {Lam, R. K. and Raj, S. L. and Pascal, T. A. and Pemmaraju, C. D. and Foglia, L. and Simoncig, A. and Fabris, N. and Miotti, P. and Hull, C. J. and Rizzuto, A. M. and Smith, J. W. and Mincigrucci, R. and Masciovecchio, C. and Gessini, A. and Allaria, E. and De Ninno, G. and Diviacco, B. and Roussel, E. and Spampinati, S. and Penco, G. and Di Mitri, S. and Trovò, M. and Danailov, M. and Christensen, S. T. and Sokaras, D. and Weng, T. -C. and Coreno, M. and Poletto, L. and Drisdell, W. S. and Prendergast, D. and Giannessi, L. and Principi, E. and Nordlund, D. and Saykally, R. J. and Schwartz, C. P.},
abstractNote = {Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (~284 eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from the first atomic layer at the open surface. This technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.},
doi = {10.1103/PhysRevLett.120.023901},
journal = {Physical Review Letters},
issn = {0031-9007},
number = 2,
volume = 120,
place = {United States},
year = {2018},
month = {1}
}

Works referenced in this record:

Pulse Duration of Seeded Free-Electron Lasers
journal, June 2017


Relative electron inelastic mean free paths for diamond and graphite at 8keV and intrinsic contributions to the energy-loss
journal, June 2009

  • Kunz, C.; Cowie, B. C. C.; Drube, W.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 173, Issue 1
  • DOI: 10.1016/j.elspec.2009.03.022

Wakefields studies for the SXFEL user facility
journal, May 2017

  • Song, Ming-Hao; Feng, Chao; Huang, Da-Zhang
  • Nuclear Science and Techniques, Vol. 28, Issue 7
  • DOI: 10.1007/s41365-017-0242-7

EIS: the scattering beamline at FERMI
journal, April 2015

  • Masciovecchio, Claudio; Battistoni, Andrea; Giangrisostomi, Erika
  • Journal of Synchrotron Radiation, Vol. 22, Issue 3
  • DOI: 10.1107/S1600577515003380

The structure of interfacial water on gold electrodes studied by x-ray absorption spectroscopy
journal, October 2014


Four-wave mixing experiments with extreme ultraviolet transient gratings
journal, April 2015

  • Bencivenga, F.; Cucini, R.; Capotondi, F.
  • Nature, Vol. 520, Issue 7546
  • DOI: 10.1038/nature14341

A theoretical analysis of the sum frequency generation spectrum of the water surface
journal, August 2000


X-ray two-photon absorption competing against single and sequential multiphoton processes
journal, February 2014

  • Tamasaku, Kenji; Shigemasa, Eiji; Inubushi, Yuichi
  • Nature Photonics, Vol. 8, Issue 4
  • DOI: 10.1038/nphoton.2014.10

X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92
journal, July 1993

  • Henke, B. L.; Gullikson, E. M.; Davis, J. C.
  • Atomic Data and Nuclear Data Tables, Vol. 54, Issue 2, p. 181-342
  • DOI: 10.1006/adnd.1993.1013

Anomalous nonlinear X-ray Compton scattering
journal, August 2015

  • Fuchs, Matthias; Trigo, Mariano; Chen, Jian
  • Nature Physics, Vol. 11, Issue 11
  • DOI: 10.1038/nphys3452

exciting: a full-potential all-electron package implementing density-functional theory and many-body perturbation theory
journal, August 2014

  • Gulans, Andris; Kontur, Stefan; Meisenbichler, Christian
  • Journal of Physics: Condensed Matter, Vol. 26, Issue 36
  • DOI: 10.1088/0953-8984/26/36/363202

X-Ray Second Harmonic Generation
journal, April 2014


Ab initio calculations of electron inelastic mean free paths and stopping powers
journal, October 2006


Generation of Optical Harmonics
journal, August 1961


Coherence Properties of Individual Femtosecond Pulses of an X-Ray Free-Electron Laser
journal, September 2011


Inhomogeneous Electron Gas
journal, November 1964


Density functional study of graphite bulk and surface properties
journal, February 2006


Two-stage seeded soft-X-ray free-electron laser
journal, October 2013


X-Ray Parametric Down-Conversion in the Langevin Regime
journal, July 2012


Second-Harmonic Optical Response from First Principles
journal, January 2004


Broadband Deep UV Spectra of Interfacial Aqueous Iodide
journal, September 2016

  • Rizzuto, Anthony M.; Irgen-Gioro, Shawn; Eftekhari-Bafrooei, Ali
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 19
  • DOI: 10.1021/acs.jpclett.6b01931

Structure of graphite by neutron diffraction
journal, November 1975


Atomic inner-shell X-ray laser at 1.46 nanometres pumped by an X-ray free-electron laser
journal, January 2012

  • Rohringer, Nina; Ryan, Duncan; London, Richard A.
  • Nature, Vol. 481, Issue 7382
  • DOI: 10.1038/nature10721

Nonlinear optics with coherent free electron lasers
journal, March 2016


Establishing nonlinearity thresholds with ultraintense X-ray pulses
journal, September 2016

  • Szlachetko, Jakub; Hoszowska, Joanna; Dousse, Jean-Claude
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep33292

Atomic electron tomography: 3D structures without crystals
journal, September 2016


Highly coherent and stable pulses from the FERMI seeded free-electron laser in the extreme ultraviolet
journal, September 2012


Nonlinear optics in the angstrom regime: Hard-x-ray frequency doubling in perfect crystals
journal, April 2003


Quantitative spectral and orientational analysis in surface sum frequency generation vibrational spectroscopy (SFG-VS)
journal, April 2005

  • Wang *, Hong-Fei; Gan † ‡, Wei; Lu † ‡ §, Rong
  • International Reviews in Physical Chemistry, Vol. 24, Issue 2
  • DOI: 10.1080/01442350500225894

Recent results of PADReS, the Photon Analysis Delivery and REduction System, from the FERMI FEL commissioning and user operations
journal, April 2015

  • Zangrando, Marco; Cocco, Daniele; Fava, Claudio
  • Journal of Synchrotron Radiation, Vol. 22, Issue 3
  • DOI: 10.1107/S1600577515004580

X-ray and optical wave mixing
journal, August 2012

  • Glover, T. E.; Fritz, D. M.; Cammarata, M.
  • Nature, Vol. 488, Issue 7413
  • DOI: 10.1038/nature11340

Equilibrium and Dynamic Processes at Interfaces by Second Harmonic and Sum Frequency Generation
journal, October 1992


High-Gain Harmonic-Generation Free-Electron Laser
journal, August 2000


Spectrometer for X-ray emission experiments at FERMI free-electron-laser
journal, October 2014

  • Poletto, L.; Frassetto, F.; Miotti, P.
  • Review of Scientific Instruments, Vol. 85, Issue 10
  • DOI: 10.1063/1.4898315

Laser-induced electron dynamics including photoionization: A heuristic model within time-dependent configuration interaction theory
journal, September 2009

  • Klinkusch, Stefan; Saalfrank, Peter; Klamroth, Tillmann
  • The Journal of Chemical Physics, Vol. 131, Issue 11
  • DOI: 10.1063/1.3218847

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965