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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
Resource Relation:
Journal Name: Physical Review Letters; Journal Volume: 120; Journal Issue: 2
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},
number = 2,
volume = 120,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2018},
month = {Mon Jan 01 00:00:00 EST 2018}
}