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Saturable Absorption of Free-Electron Laser Radiation by Graphite near the Carbon K-Edge.
Hoffmann, Lars; Jamnuch, Sasawat; Schwartz, Craig P; Helk, Tobias; Raj, Sumana L; Mizuno, Hikaru; Mincigrucci, Riccardo; Foglia, Laura; Principi, Emiliano; Saykally, Richard J; Drisdell, Walter S; Fatehi, Shervin; Pascal, Tod A; Zuerch, Michael.
Afiliación
  • Hoffmann L; Department of Chemistry, University of California, Berkeley, California 94720, United States.
  • Jamnuch S; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
  • Schwartz CP; Fritz Haber Institute of the Max Planck Society, 14195 Berlin, Germany.
  • Helk T; ATLAS Materials Science Laboratory, Department of Nano Engineering and Chemical Engineering, University of California San Diego, La Jolla, California 92023, United States.
  • Raj SL; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
  • Mizuno H; Nevada Extreme Conditions Laboratory, University of Nevada, Las Vegas, Las Vegas, Nevada 89154, United States.
  • Mincigrucci R; Institute of Optics and Quantum Electronics, Abbe Center of Photonics, Friedrich-Schiller University, 07743 Jena, Germany.
  • Foglia L; Helmholtz Institute Jena, 07743 Jena, Germany.
  • Principi E; Department of Chemistry, University of California, Berkeley, California 94720, United States.
  • Saykally RJ; Department of Chemistry, University of California, Berkeley, California 94720, United States.
  • Drisdell WS; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
  • Fatehi S; Elettra-Sincrotrone Trieste S.C.p.A., Strada Statale 14, 34149 Trieste, Italy.
  • Pascal TA; Elettra-Sincrotrone Trieste S.C.p.A., Strada Statale 14, 34149 Trieste, Italy.
  • Zuerch M; Elettra-Sincrotrone Trieste S.C.p.A., Strada Statale 14, 34149 Trieste, Italy.
J Phys Chem Lett ; 13(39): 8963-8970, 2022 Oct 06.
Article en En | MEDLINE | ID: mdl-36165491
The interaction of intense light with matter gives rise to competing nonlinear responses that can dynamically change material properties. Prominent examples are saturable absorption (SA) and two-photon absorption (TPA), which dynamically increase and decrease the transmission of a sample depending on pulse intensity, respectively. The availability of intense soft X-ray pulses from free-electron lasers (FELs) has led to observations of SA and TPA in separate experiments, leaving open questions about the possible interplay between and relative strength of the two phenomena. Here, we systematically study both phenomena in one experiment by exposing graphite films to soft X-ray FEL pulses of varying intensity. By applying real-time electronic structure calculations, we find that for lower intensities the nonlinear contribution to the absorption is dominated by SA attributed to ground-state depletion; our model suggests that TPA becomes more dominant for larger intensities (>1014 W/cm2). Our results demonstrate an approach of general utility for interpreting FEL spectroscopies.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2022 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2022 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos