Optimally shaped narrowband picosecond pulses for femtosecond stimulated Raman spectroscopy.

A comparison between a Fabry-Pérot etalon filter and a conventional grating filter for producing the picosecond (ps) Raman pump pulses for femtosecond stimulated Raman spectroscopy (FSRS) is presented. It is shown that for pulses of equal energy the etalon filter produces Raman signals twice as large as that of the grating filter while suppressing the electronically resonant background signal. The time asymmetric profile of the etalon-generated pulse is shown to be responsible for both of these observations. A theoretical discussion is presented which quantitatively supports this hypothesis. It is concluded that etalons are the ideal method for the generation of narrowband ps pulses for FSRS because of the optical simplicity, efficiency, improved FSRS intensity and reduced backgrounds.

[1]  D. Dlott,et al.  Nonresonant Background Suppression in Broadband Vibrational Sum-Frequency Generation Spectroscopy , 2007 .

[2]  R. Mathies,et al.  Photoexcited structural dynamics of an azobenzene analog 4-nitro-4'-dimethylamino-azobenzene from femtosecond stimulated Raman. , 2012, Physical chemistry chemical physics : PCCP.

[3]  Igor V. Stiopkin,et al.  Temporal effects on spectroscopic line shapes, resolution, and sensitivity of the broad-band sum frequency generation. , 2010, The Journal of chemical physics.

[4]  R. Hochstrasser,et al.  STRUCTURE OF THE AMIDE I BAND OF PEPTIDES MEASURED BY FEMTOSECOND NONLINEAR-INFRARED SPECTROSCOPY , 1998 .

[5]  Richard A. Mathies,et al.  Ultrafast excited-state isomerization in phytochrome revealed by femtosecond stimulated Raman spectroscopy , 2009, Proceedings of the National Academy of Sciences.

[6]  R Osellame,et al.  Background-free broadband CARS spectroscopy from a 1-MHz ytterbium laser. , 2011, Optics express.

[7]  R. Mathies,et al.  Electron Transfer Dynamics of Triphenylamine Dyes Bound to TiO2 Nanoparticles from Femtosecond Stimulated Raman Spectroscopy , 2013 .

[8]  R. Mathies,et al.  Theory of femtosecond stimulated Raman spectroscopy. , 2004, The Journal of chemical physics.

[9]  G. Cerullo,et al.  Femtosecond stimulated Raman spectrometer in the 320-520nm range. , 2011, Optics express.

[10]  R. Mathies,et al.  Dependence of line shapes in femtosecond broadband stimulated Raman spectroscopy on pump-probe time delay. , 2005, The Journal of chemical physics.

[11]  N. Ernsting,et al.  Excited stilbene: intramolecular vibrational redistribution and solvation studied by femtosecond stimulated Raman spectroscopy. , 2010, The journal of physical chemistry. B.

[12]  Sukesh Roy,et al.  Communication: hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering thermometry using a narrowband time-asymmetric probe pulse. , 2012, The Journal of chemical physics.

[13]  D. Jonas.  Two-dimensional femtosecond spectroscopy. , 2003, Annual review of physical chemistry.

[14]  S. Silvestri,et al.  Ultrafast optical parametric amplifiers , 2003 .

[15]  R. Mathies,et al.  Structural Observation of the Primary Isomerization in Vision with Femtosecond-Stimulated Raman , 2005, Science.

[16]  S. Mukamel,et al.  Broadband infrared and Raman probes of excited-state vibrational molecular dynamics: simulation protocols based on loop diagrams. , 2013, Physical chemistry chemical physics : PCCP.

[17]  R. Mathies,et al.  Mapping GFP structure evolution during proton transfer with femtosecond Raman spectroscopy , 2009, Nature.

[18]  T. Scopigno,et al.  Spectrally tailored narrowband pulses for femtosecond stimulated Raman spectroscopy in the range 330-750 nm. , 2012, Optics express.

[19]  Richard A Mathies,et al.  Femtosecond broadband stimulated Raman spectroscopy: Apparatus and methods. , 2004, The Review of scientific instruments.

[20]  R. Mathies,et al.  Femtosecond stimulated Raman spectroscopy. , 2007 .

[21]  A. Dobryakov,et al.  Femtosecond stimulated Raman spectroscopy of flavin after optical excitation. , 2011, The journal of physical chemistry. B.