Soft X-Ray Second Harmonic Generation as an Interfacial Probe

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.

doi:10.1103/PhysRevLett.120.023901

Soft X-Ray Second Harmonic Generation as an Interfacial Probe

Journal Article · 01 January 2018 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.120.023901· OSTI ID:1422881

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. more »

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.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 1422881

Report Number(s):: NREL/JA-5K00-70998; PRLTAO

Journal Information:: Physical Review Letters, Vol. 120, Issue 2; ISSN 0031-9007

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

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