Soft X-Ray Second Harmonic Generation as an Interfacial Probe: Article No. 023901

Steven Christensen; R. Lam; S. Raj; T. Pascal; C. Pemmaraju; L. Foglia; A. Simoncig; N. Fabris; P. Miotti; C. Hull; A. Rizzuto; J. Smith; R. Mincigrucci; C. Masciovecchio; A. Gessini; E. Allaria; G. Ninno; B. Diviacco; E. Roussel; S. Spampinati; G. Penco; S. Mitri; M. Trovo; M. Danailov; D. Sokaras; T.-C. Weng; M. Coreno; L. Poletto; W. Drisdell; D. Prendergast; L. Giannessi; E. Principi; D. Nordlund; R. Saykally; C. Schwartz

doi:10.1103/PhysRevLett.120.023901

Soft X-Ray Second Harmonic Generation as an Interfacial Probe: Article No. 023901

Steven Christensen, R. Lam, S. Raj, T. Pascal, C. Pemmaraju, L. Foglia, A. Simoncig, N. Fabris, P. Miotti, C. Hull, A. Rizzuto, J. Smith, R. Mincigrucci, C. Masciovecchio, A. Gessini, E. Allaria, G. Ninno, B. Diviacco, E. Roussel, S. SpampinatiG. Penco, S. Mitri, M. Trovo, M. Danailov, D. Sokaras, T.-C. Weng, M. Coreno, L. Poletto, W. Drisdell, D. Prendergast, L. Giannessi, E. Principi, D. Nordlund, R. Saykally, C. Schwartz

Materials Science

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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.

Original language	American English
Number of pages	6
Journal	Physical Review Letters
Volume	120
Issue number	2
DOIs	https://doi.org/10.1103/PhysRevLett.120.023901
State	Published - 2018

NREL Publication Number

NREL/JA-5K00-70998

Keywords

interfaces
nonlinear optics
surfaces
x-ray techniques

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10.1103/PhysRevLett.120.023901

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Christensen, S., Lam, R., Raj, S., Pascal, T., Pemmaraju, C., Foglia, L., Simoncig, A., Fabris, N., Miotti, P., Hull, C., Rizzuto, A., Smith, J., Mincigrucci, R., Masciovecchio, C., Gessini, A., Allaria, E., Ninno, G., Diviacco, B., Roussel, E., ... Schwartz, C. (2018). Soft X-Ray Second Harmonic Generation as an Interfacial Probe: Article No. 023901. Physical Review Letters, 120(2). https://doi.org/10.1103/PhysRevLett.120.023901

@article{dd75a7d1ba7c44039e592f7f30c317ab,

title = "Soft X-Ray Second Harmonic Generation as an Interfacial Probe: Article No. 023901",

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.",

keywords = "interfaces, nonlinear optics, surfaces, x-ray techniques",

author = "Steven Christensen and R. Lam and S. Raj and T. Pascal and C. Pemmaraju and L. Foglia and A. Simoncig and N. Fabris and P. Miotti and C. Hull and A. Rizzuto and J. Smith and R. Mincigrucci and C. Masciovecchio and A. Gessini and E. Allaria and G. Ninno and B. Diviacco and E. Roussel and S. Spampinati and G. Penco and S. Mitri and M. Trovo and M. Danailov and D. Sokaras and T.-C. Weng and M. Coreno and L. Poletto and W. Drisdell and D. Prendergast and L. Giannessi and E. Principi and D. Nordlund and R. Saykally and C. Schwartz",

year = "2018",

doi = "10.1103/PhysRevLett.120.023901",

language = "American English",

volume = "120",

journal = "Physical Review Letters",

issn = "0031-9007",

publisher = "American Physical Society",

number = "2",

}

Christensen, S, Lam, R, Raj, S, Pascal, T, Pemmaraju, C, Foglia, L, Simoncig, A, Fabris, N, Miotti, P, Hull, C, Rizzuto, A, Smith, J, Mincigrucci, R, Masciovecchio, C, Gessini, A, Allaria, E, Ninno, G, Diviacco, B, Roussel, E, Spampinati, S, Penco, G, Mitri, S, Trovo, M, Danailov, M, Sokaras, D, Weng, T-C, Coreno, M, Poletto, L, Drisdell, W, Prendergast, D, Giannessi, L, Principi, E, Nordlund, D, Saykally, R & Schwartz, C 2018, 'Soft X-Ray Second Harmonic Generation as an Interfacial Probe: Article No. 023901', Physical Review Letters, vol. 120, no. 2. https://doi.org/10.1103/PhysRevLett.120.023901

TY - JOUR

T1 - Soft X-Ray Second Harmonic Generation as an Interfacial Probe

T2 - Article No. 023901

AU - Christensen, Steven

AU - Lam, R.

AU - Raj, S.

AU - Pascal, T.

AU - Pemmaraju, C.

AU - Foglia, L.

AU - Simoncig, A.

AU - Fabris, N.

AU - Miotti, P.

AU - Hull, C.

AU - Rizzuto, A.

AU - Smith, J.

AU - Mincigrucci, R.

AU - Masciovecchio, C.

AU - Gessini, A.

AU - Allaria, E.

AU - Ninno, G.

AU - Diviacco, B.

AU - Roussel, E.

AU - Spampinati, S.

AU - Penco, G.

AU - Mitri, S.

AU - Trovo, M.

AU - Danailov, M.

AU - Sokaras, D.

AU - Weng, T.-C.

AU - Coreno, M.

AU - Poletto, L.

AU - Drisdell, W.

AU - Prendergast, D.

AU - Giannessi, L.

AU - Principi, E.

AU - Nordlund, D.

AU - Saykally, R.

AU - Schwartz, C.

PY - 2018

Y1 - 2018

N2 - 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.

AB - 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.

KW - interfaces

KW - nonlinear optics

KW - surfaces

KW - x-ray techniques

U2 - 10.1103/PhysRevLett.120.023901

DO - 10.1103/PhysRevLett.120.023901

M3 - Article

SN - 0031-9007

VL - 120

JO - Physical Review Letters

JF - Physical Review Letters

IS - 2

ER -

Soft X-Ray Second Harmonic Generation as an Interfacial Probe: Article No. 023901

Abstract

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Keywords

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