Optimizing hybrid rotational femtosecond/picosecond coherent anti-Stokes Raman spectroscopy in nitrogen at high pressures and temperatures
Nils Torge Mecker, Trevor L. Courtney, Brian D. Patterson, David Escofet‐Martin, Brian Peterson, Christopher J. Kliewer, Mark Linne
Abstract
We demonstrate the use of hybrid rotational femtosecond/picosecond (fs/ps) coherent anti-Stokes Raman spectroscopy (HR-CARS) as a technique for temperature measurements in nitrogen gas at high pressures and temperatures. A broadband pulse shaper-adjusted 42 fs pulse interacts with a narrow-bandwidth, frequency-upconverted 5.5 ps pulse in a cell containing <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:msub> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">N</mml:mi> </mml:mrow> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>2</mml:mn> </mml:mrow> </mml:mrow> </mml:msub> </mml:mrow> </mml:math> at pressures of 1–70 atm and temperatures of 300–1000 K. A computational code is used to model spectra and fit experimental results to obtain best-fit temperatures. We demonstrate good qualitative fits as well as good accuracy and precision between thermocouple measured and best-fit temperatures over the explored pressure and temperature regimes. The overall average percentage temperature difference between thermocouple measurements and best-fit temperatures is <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mo>−</mml:mo> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>0</mml:mn> </mml:mrow> </mml:mrow> <mml:mo>.</mml:mo> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>3</mml:mn> </mml:mrow> </mml:mrow> <mml:mi mathvariant="normal">%</mml:mi> </mml:math> with a standard deviation of 7.1%, showing the suitability of HR-CARS for characterizing high-pressure and -temperature environments.