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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. Here, 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:
 [1];  [1];  [2];  [3];  [4];  [4];  [5];  [5];  [1];  [1];  [1];  [4];  [4];  [4];  [4];  [6];  [4];  [4];  [4];  [4] more »;  [4];  [4];  [4];  [7];  [3];  [8];  [9];  [10];  [2];  [2];  [11];  [4];  [3];  [1];  [12] « less
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Elettra-Sincrotrone Trieste S.C.p.A., Trieste (Italy)
  5. National Research Council of Italy, Padova (Italy); Univ. of Padova, Padova (Italy)
  6. Elettra-Sincrotrone Trieste S.C.p.A., Trieste (Italy); Univ. of Nova Gorica, Nova Gorica (Slovenia)
  7. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  8. Center for High Pressure Science & Technology Advanced Research, Shanghai (China)
  9. Elettra-Sincrotrone Trieste S.C.p.A., Trieste (Italy); Elettra Lab., Trieste (Italy)
  10. National Research Council of Italy, Padova (Italy)
  11. Elettra-Sincrotrone Trieste S.C.p.A., Trieste (Italy); C.R. Frascati, Frascati (Rome) (Italy)
  12. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1418311
Alternate Identifier(s):
OSTI ID: 1416070; OSTI ID: 1417659
Grant/Contract Number:  
AC02-05CH11231; AC02-76SF00515; AC36-08GO28308; SC0004993; W911NF-13-1-0483; W911NF-17-1-0163; DGE 1106400
Resource Type:
Accepted Manuscript
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:
73 NUCLEAR PHYSICS AND RADIATION PHYSICS

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.
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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. https://doi.org/10.1103/PhysRevLett.120.023901
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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. https://doi.org/10.1103/PhysRevLett.120.023901. https://www.osti.gov/servlets/purl/1418311.
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@article{osti_1418311,
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. Here, 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},
number = 2,
volume = 120,
place = {United States},
year = {2018},
month = {1}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1103/PhysRevLett.120.023901
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Cited by: 8 works
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Figures / Tables:

FIG. 1 FIG. 1: Experimental design. (a) X-ray pulses are passed through a 2 mm iris, then focused by an ellipsoidal mirror (not shown) onto the graphite sample (spot size ∼350 $µm^2$) at normal incidence. The transmitted beam and the collinear second harmonic signal (double the fundamental photon energy) are passed throughmore » a 600 nm aluminum filter and into a spectrometer, spatially separating the second harmonic signal from the fundamental. A schematic energy level diagram of the SHG process is shown in the inset. (b) The CCD image and projection of the transmitted FEL beam and the SHG signal for a single FEL pulse. (c) Linear, total electron yield (TEY) X-ray absorption spectrum of a 500 nm graphite sample. X-ray SHG measurements were made at the three discrete photon energies (ω1) shown in the dashed lines. The non-resonant (below $C$ K-edge) and resonant (above $C$ K-edge) regions are shaded in orange and green, respectively.« less
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