Rotational-level-dependent dephasing rates and nonresonant background can lead to significant uncertainties in coherent anti-Stokes Raman scattering (CARS) thermometry under high-pressure, lowtemperature conditions if the gas composition is unknown. Hybrid femtosecond/picosecond rotational CARS is employed to minimize or eliminate the influence of collisions and nonresonant background for accurate, frequency-domain thermometry at elevated pressure. The ability to ignore these interferences and achieve thermometric errors of <5% is demonstrated for N 2 and O 2 at pressures up to 15 atm. Beyond 15 atm, the effects of collisions cannot be ignored but can be minimized using a short probe delay (~6.5 ps) after Raman excitation, thereby improving thermometric accuracy with a time-and frequency-resolved theoretical model.
KeywordsFriedrich-Alexander University Erlangen, Raman scattering, Raman spectroscopy, dephasing rates, elevated pressure, femtoseconds, frequency domains, gas compositions, gasphase, low temperatures, nonresonant, Raman excitation, chemistry, computer aided design, phase transition, radiation scattering, thermography, computer-aided design, equipment design
Disciplines
Chemistry | Mechanical Engineering
CommentsThis article is from Optics Express 15 (2012): 5003, doi: 10.1364/OE.20.005003. Posted with permission.
RightsThis paper was published in Optics Express and is made available as an electronic reprint with the permission of OSA. The paper can be found at the following URL on tahe OSA website: https://www.osapublishing.org/ oe/abstract.cfm?uri=oe-20-5-5003. Systematic or multiple reproduction or distribution to multiple locations via electronic or other means is prohibited and is subject to penalties under law. Abstract: Rotational-level-dependent dephasing rates and nonresonant background can lead to significant uncertainties in coherent anti-Stokes Raman scattering (CARS) thermometry under high-pressure, lowtemperature conditions if the gas composition is unknown. Hybrid femtosecond/picosecond rotational CARS is employed to minimize or eliminate the influence of collisions and nonresonant background for accurate, frequency-domain thermometry at elevated pressure. The ability to ignore these interferences and achieve thermometric errors of <5% is demonstrated for N 2 and O 2 at pressures up to 15 atm. Beyond 15 atm, the effects of collisions cannot be ignored but can be minimized using a short probe delay (~6.5 ps) after Raman excitation, thereby improving thermometric accuracy with a time-and frequency-resolved theoretical model.
©2012 Optical Society of America