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

Abstract

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 H 2/air flat flame.

Authors:
 [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Engineering Sciences Center
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Science (NA-113)
OSTI Identifier:
1182983
Report Number(s):
SAND-2014-15528J
Journal ID: ISSN 0003-6935; 533705
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Optics
Additional Journal Information:
Journal Volume: 53; Journal Issue: 28; Journal ID: ISSN 0003-6935
Publisher:
Optical Society of America (OSA)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Kearney, Sean Patrick. Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.. United States: N. p., 2014. Web. doi:10.1364/AO.53.006579.
Kearney, Sean Patrick. Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.. United States. https://doi.org/10.1364/AO.53.006579
Kearney, Sean Patrick. Tue . "Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.". United States. https://doi.org/10.1364/AO.53.006579. https://www.osti.gov/servlets/purl/1182983.
@article{osti_1182983,
title = {Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.},
author = {Kearney, Sean Patrick},
abstractNote = {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.},
doi = {10.1364/AO.53.006579},
url = {https://www.osti.gov/biblio/1182983}, journal = {Applied Optics},
issn = {0003-6935},
number = 28,
volume = 53,
place = {United States},
year = {2014},
month = {7}
}

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Cited by: 9 works
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Works referenced in this record:

Photolytic-interference-free, femtosecond two-photon fluorescence imaging of atomic hydrogen
journal, January 2012


Femtosecond laser electronic excitation tagging for quantitative velocity imaging in air
journal, January 2011


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journal, December 2006


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Single-beam coherent anti-Stokes Raman scattering spectroscopy of N2 using a shaped 7 fs laser pulse
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One-dimensional single-shot thermometry in flames using femtosecond-CARS line imaging
journal, January 2011


Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering
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: Simplified two-beam rotational CARS signal generation demonstrated in 1D
journal, February 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


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Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion
journal, November 2008


Interference-free coherence dynamics of gas-phase molecules using spectral focusing
journal, January 2012


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    Works referencing / citing this record:

    Comparison of chirped-probe-pulse and hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for combustion thermometry
    journal, January 2017


    Recent advances in ultrafast-laser-based spectroscopy and imaging for reacting plasmas and flames
    journal, September 2017


    Impact of moderate pump–Stokes chirp on femtosecond coherent anti‐Stokes Raman scattering spectra
    journal, October 2019