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

Kearney, Sean Patrick

doi:10.1364/AO.53.006579

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

Journal Article · Tue Jul 01 00:00:00 EDT 2014 · Applied Optics

DOI:https://doi.org/10.1364/AO.53.006579· OSTI ID:1182983

Kearney, Sean Patrick ^[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.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (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, Journal Name: Applied Optics Journal Issue: 28 Vol. 53; ISSN 0003-6935

Publisher:: Optical Society of America (OSA)Copyright Statement

Country of Publication:: United States

Language:: English

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Interplay of pulse bandwidth and spectral resolution in spectral-focusing CARS microscopy Cole, R. A.; Slepkov, A. D. Journal of the Optical Society of America B, Vol. 35, Issue 4 https://doi.org/10.1364/josab.35.000842	journal	January 2018
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