skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.

Journal Article · · Applied Optics
DOI:https://doi.org/10.1364/AO.53.006579· OSTI ID:1182983
 [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Engineering Sciences Center

A simple spectral focusing scheme for bandwidth optimization of gas-phase rotational coherent anti-Stokes Raman scattering (CARS) spectra is presented. The method is useful when femtosecond pump/Stokes preparation of the Raman coherence is utilized. The approach is of practical utility when working with laser pulses that are not strictly transform limited, or when windows or other sources of pulse chirp may be present in the experiment. A delay between the femtosecond preparation pulses is introduced to shift the maximum Raman preparation away from zero frequency and toward the Stokes or anti-Stokes side of the spectrum with no loss in total preparation bandwidth. Shifts of 100 cm-1 or more are attainable and allow for enhanced detection of high-energy (150-300 cm-1) rotational Raman transitions at near transform-limited optimum sensitivity. A simple theoretical treatment for the case of identical pump and Stokes pulses with linear frequency chirp is presented. The approach is then demonstrated experimentally for typical levels of transform-limited laser performance obtained our laboratory with nonresonant CARS in argon and Raman-resonant spectra from a lean H2/air flat flame.

Research Organization:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Science (NA-113)
Grant/Contract Number:
AC04-94AL85000
OSTI ID:
1182983
Report Number(s):
SAND-2014-15528J; 533705
Journal Information:
Applied Optics, Vol. 53, Issue 28; ISSN 0003-6935
Publisher:
Optical Society of America (OSA)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 20 works
Citation information provided by
Web of Science

References (25)

Femtosecond laser electronic excitation tagging for quantitative velocity imaging in air journal January 2011
Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence journal December 2006
Theory of femtosecond coherent anti-Stokes Raman scattering spectroscopy of gas-phase transitions journal July 2007
Effects of N2–CO polarization beating on femtosecond coherent anti-Stokes Raman scattering spectroscopy of N2 journal April 2009
Single-beam coherent anti-Stokes Raman scattering spectroscopy of N2 using a shaped 7 fs laser pulse journal August 2009
One-dimensional single-shot thermometry in flames using femtosecond-CARS line imaging journal January 2011
Communication: Time-domain measurement of high-pressure N2 and O2 self-broadened linewidths using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering journal November 2011
Probe-pulse optimization for nonresonant suppression in hybrid fs/ps coherent anti-Stokes Raman scattering at high temperature journal January 2011
Theoretical modeling of single-laser-shot, chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering thermometry journal April 2011
Polarization suppression of the nonresonant background in femtosecond coherent anti-Stokes Raman scattering for flame thermometry at 5 kHz journal January 2012
Communication: Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering thermometry using a narrowband time-asymmetric probe pulse journal March 2012
Communication: Two-dimensional gas-phase coherent anti-Stokes Raman spectroscopy (2D-CARS): Simultaneous planar imaging and multiplex spectroscopy in a single laser shot journal June 2013
Communication: Simplified two-beam rotational CARS signal generation demonstrated in 1D journal February 2013
Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering at flame temperatures using a second-harmonic bandwidth-compressed probe journal January 2013
Time-resolved femtosecond CARS from 10 to 50 Bar: collisional sensitivity: Time-resolved femtosecond CARS journal March 2013
Diagnostic Imaging in Flames with Instantaneous Planar Coherent Raman Spectroscopy journal March 2014
Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed gas-phase thermometry journal January 2010
Experimental comparison of single-shot broadband vibrational and dual-broadband pure rotational coherent anti-Stokes Raman scattering in hot air journal January 1996
Is rotational CARS an alternative to vibrational CARS for thermometry? journal July 1990
Rotational CARS for simultaneous measurements of temperature and concentrations of N2, O2, CO, and CO2 demonstrated in a CO/air diffusion flame journal January 2009
Ultrafast nonlinear spectroscopy with chirped optical pulses journal January 1992
Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses journal July 2004
Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion journal November 2008
Tunable excitation source for coherent Raman spectroscopy based on a single fiber laser journal October 2011
Interference-free coherence dynamics of gas-phase molecules using spectral focusing journal January 2012

Cited By (6)

Simple model of coherent anti-Stokes Raman scattering signals generated by means of linearly chirped ultrashort Gaussian laser pulses journal March 2018
Impact of moderate pump–Stokes chirp on femtosecond coherent anti‐Stokes Raman scattering spectra journal October 2019
Recent advances in ultrafast-laser-based spectroscopy and imaging for reacting plasmas and flames journal September 2017
Impact of input field characteristics on vibrational femtosecond coherent anti-Stokes Raman scattering thermometry journal January 2018
Interplay of pulse bandwidth and spectral resolution in spectral-focusing CARS microscopy journal January 2018
Flexible chirp-free probe pulse amplification for kHz fs/ps rotational CARS journal January 2020

Similar Records

Hybrid fs/ps rotational CARS temperature and oxygen measurements in the product gases of canonical flat flames
Journal Article · Wed Dec 31 00:00:00 EST 2014 · Combustion and Flame · OSTI ID:1182983

Analysis of picosecond coherent anti-Stokes Raman spectra for gas-phase diagnostics
Journal Article · Wed May 24 00:00:00 EDT 2023 · Journal of the Optical Society of America. Part B, Optical Physics · OSTI ID:1182983

Pure-rotational H2 thermometry by ultrabroadband coherent anti-Stokes Raman spectroscopy
Journal Article · Mon Jun 12 00:00:00 EDT 2017 · Journal of Chemical Physics · OSTI ID:1182983