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Title: Three-beam rotational coherent anti-Stokes Raman spectroscopy thermometry in scattering environments

Abstract

Three-beam rotational coherent anti-Stokes Raman scattering (CARS) measurements performed in highly scattering environments are susceptible to contamination by two-beam CARS signals generated by the pump–probe and Stokes–probe interactions at the measurement volume. If this occurs, differences in the Raman excitation bandwidth between the two-beam and three-beam CARS signals can add significant errors to the spectral analysis. This interference to the best of our knowledge has not been acknowledged in previous three-beam rotational CARS experiments, but may introduce measurement errors up to 25% depending on the temperature, amount of scattering, and differences between the two-beam and three-beam Raman excitation bandwidths. Here, the presence of two-beam CARS signal contamination was experimentally verified using a femtosecond–picosecond rotational CARS instrument in two scattering environments: (1) a fireball generated by a laboratory-scale explosion that contained particulate matter, metal fragments, and soot, and (2) a flow of air and small liquid droplets. A polarization scheme is presented to overcome this interference. By rotating the pump and Stokes polarizations +55° and –55° from the probe, respectively, the two-beam and three-beam CARS signals are orthogonally polarized and can be separated using a polarization analyzer. Using this polarization arrangement, the Raman-resonant three-beam CARS signal amplitude is reduced by amore » factor of 2.3 compared to the case where all polarizations are parallel. This method is successfully demonstrated in both scattering environments. A theoretical model is presented, and the temperature measurement error is studied for different experimental conditions. The criteria for when this interference may be present are discussed.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [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); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1667420
Report Number(s):
SAND-2020-9121J
Journal ID: ISSN 1559-128X; 690289
Grant/Contract Number:  
AC04-94AL85000; NA-0003525
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Optics
Additional Journal Information:
Journal Volume: 59; Journal Issue: 27; Journal ID: ISSN 1559-128X
Publisher:
Optical Society of America
Country of Publication:
United States
Language:
English

Citation Formats

Richardson, Daniel R., Kearney, Sean P., and Guildenbecher, Daniel R. Three-beam rotational coherent anti-Stokes Raman spectroscopy thermometry in scattering environments. United States: N. p., 2020. Web. doi:10.1364/ao.392110.
Richardson, Daniel R., Kearney, Sean P., & Guildenbecher, Daniel R. Three-beam rotational coherent anti-Stokes Raman spectroscopy thermometry in scattering environments. United States. doi:10.1364/ao.392110.
Richardson, Daniel R., Kearney, Sean P., and Guildenbecher, Daniel R. Wed . "Three-beam rotational coherent anti-Stokes Raman spectroscopy thermometry in scattering environments". United States. doi:10.1364/ao.392110.
@article{osti_1667420,
title = {Three-beam rotational coherent anti-Stokes Raman spectroscopy thermometry in scattering environments},
author = {Richardson, Daniel R. and Kearney, Sean P. and Guildenbecher, Daniel R.},
abstractNote = {Three-beam rotational coherent anti-Stokes Raman scattering (CARS) measurements performed in highly scattering environments are susceptible to contamination by two-beam CARS signals generated by the pump–probe and Stokes–probe interactions at the measurement volume. If this occurs, differences in the Raman excitation bandwidth between the two-beam and three-beam CARS signals can add significant errors to the spectral analysis. This interference to the best of our knowledge has not been acknowledged in previous three-beam rotational CARS experiments, but may introduce measurement errors up to 25% depending on the temperature, amount of scattering, and differences between the two-beam and three-beam Raman excitation bandwidths. Here, the presence of two-beam CARS signal contamination was experimentally verified using a femtosecond–picosecond rotational CARS instrument in two scattering environments: (1) a fireball generated by a laboratory-scale explosion that contained particulate matter, metal fragments, and soot, and (2) a flow of air and small liquid droplets. A polarization scheme is presented to overcome this interference. By rotating the pump and Stokes polarizations +55° and –55° from the probe, respectively, the two-beam and three-beam CARS signals are orthogonally polarized and can be separated using a polarization analyzer. Using this polarization arrangement, the Raman-resonant three-beam CARS signal amplitude is reduced by a factor of 2.3 compared to the case where all polarizations are parallel. This method is successfully demonstrated in both scattering environments. A theoretical model is presented, and the temperature measurement error is studied for different experimental conditions. The criteria for when this interference may be present are discussed.},
doi = {10.1364/ao.392110},
journal = {Applied Optics},
issn = {1559-128X},
number = 27,
volume = 59,
place = {United States},
year = {2020},
month = {9}
}

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