title: Vibrational sum frequency generation spectroscopy using inverted visible pulses.
abstract: We present a broadband vibrational sum frequency generation (BB-VSFG) scheme using a novel ps visible pulse shape. We generate the fs IR pulse via standard procedures and simultaneously generate an 'inverted' time-asymmetric narrowband ps visible pulse via second harmonic generation in the pump depletion regime using a very long nonlinear crystal which has high group velocity mismatch (LiNbO3). The 'inverted' ps pulse shape minimally samples the instantaneous nonresonant response but maximally samples the resonant response, maintaining high spectral resolution. We experimentally demonstrate this scheme, presenting SFG spectra of canonical organic monolayer systems in the C-H stretch region (2800-3000 cm(-1)).
authors.affiliation: Steacie Institute for Molecular Sciences, National Research Council, 100 Sussex Drive, Ottawa, Ontario K1A 0R6 Canada.
authors.forename: Champika
authors.initials: C
authors.lastname: Weeraman
authors.forename: Steven A
authors.initials: SA
authors.lastname: Mitchell
authors.forename: Rune
authors.initials: R
authors.lastname: Lausten
authors.forename: Linda J
authors.initials: LJ
authors.lastname: Johnston
authors.forename: Albert
authors.initials: A
authors.lastname: Stolow
mesh_terms: D017076:Computer-Aided Design; D004867:Equipment Design; D019544:Equipment Failure Analysis; D012815:Signal Processing, Computer-Assisted / Q000295:instrumentation*; D013057:Spectrum Analysis / Q000295:instrumentation*; D014732:Vibration