Pure-rotational H2 thermometry by ultrabroadband coherent anti-Stokes Raman spectroscopy

Courtney, Trevor L.; Bohlin, Alexis; Patterson, Brian D.; Kliewer, Christopher J.

doi:10.1063/1.4984083

Pure-rotational H₂ thermometry by ultrabroadband coherent anti-Stokes Raman spectroscopy

Journal Article · Mon Jun 12 00:00:00 EDT 2017 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4984083· OSTI ID:1473952

Courtney, Trevor L. ^[1]; ^[1]; Patterson, Brian D. ^[1]; Kliewer, Christopher J. ^[1]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Coherent anti-Stokes Raman spectroscopy (CARS) is a sensitive technique for probing highly luminous flames in combustion applications to determine temperatures and species concentrations. CARS thermometry has been demonstrated for the vibrational Q-branch and pure-rotational S-branch of several small molecules. Practical advantages of pure-rotational CARS, such as multi-species detection, reduction of coherent line mixing and collisional narrowing even at high pressures, and the potential for more precise thermometry, have motivated experimental and theoretical advances in S-branch CARS of nitrogen (N₂), for example, which is a dominant species in air-fed combustion processes. Although hydrogen (H₂) is of interest given its prevalence as a reactant and product in many gas-phase reactions, laser bandwidth limitations have precluded the extension of CARS thermometry to the H₂ S-branch. We demonstrate H₂ thermometry using hybrid femtosecond/picosecond pure-rotational CARS, in which a broadband pump/Stokes pulse enables simultaneous excitation of the set of H₂ S-branch transitions populated at flame temperatures over the spectral region of 0–2200 cm^–1. We present a pure-rotational H₂ CARS spectral model for data fitting and compare extracted temperatures to those from simultaneously collected N₂ spectra in two systems of study: a heated flow and a diffusion flame on a Wolfhard-Parker slot burner. From 300 to 650 K in the heated flow, the H₂ and N₂ CARS extracted temperatures are, on average, within 2% of the set temperature. For flame measurements, the fitted H₂ and N₂ temperatures are, on average, within 5% of each other from 300 to 1600 K. In conclusion, our results confirm the viability of pure-rotational H₂ CARS thermometry for probing combustion reactions.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-CA), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1473952

Alternate ID(s):: OSTI ID: 1363700

Report Number(s):: SAND--2018-10035J; 667836

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 22 Vol. 146; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (42)

Temperature and Hydrogen Concentration Measurements by CARS in an Ethylene-Air Bunsen Flame Müller-Dethlefs, K.; Pealat, M.; Taran, J. -P. E. Berichte der Bunsengesellschaft für physikalische Chemie, Vol. 85, Issue 8 https://doi.org/10.1002/bbpc.19810850813	journal	August 1981
Herman-wallis factors for Raman transitions of 1∑-state diatomic molecules Tipping, R. H.; Ogilvie, J. F. Journal of Raman Spectroscopy, Vol. 15, Issue 1 https://doi.org/10.1002/jrs.1250150109	journal	February 1984
Comparative analysis of Herman-Wallis factors for uses in coherent anti-Stokes Raman spectra of light molecules Marrocco, Michele Journal of Raman Spectroscopy, Vol. 40, Issue 7 https://doi.org/10.1002/jrs.2201	journal	July 2009
On the sensitivity of rotational CARS N2 thermometry to the Herman-Wallis factor Bohlin, Alexis; Bengtsson, Per-Erik; Marrocco, Michele Journal of Raman Spectroscopy, Vol. 42, Issue 10 https://doi.org/10.1002/jrs.2869	journal	February 2011
Determination of collisional line broadening coefficients with femtosecond time-resolved CARS Skenderovi?, H.; Buckup, T.; Wohlleben, W. Journal of Raman Spectroscopy, Vol. 33, Issue 11-12 https://doi.org/10.1002/jrs.952	journal	January 2002
Aspects of hydrogen CARS thermometry Bombach, R.; Gerber, T.; Hemmerling, B. Applied Physics B Photophysics and Laser Chemistry, Vol. 51, Issue 1 https://doi.org/10.1007/bf00332326	journal	July 1990
Two wavelength-CARS thermometry of hydrogen Clauss, W.; Il'yukhin, A. A.; Kozlov, D. N. Applied Physics B Laser and Optics, Vol. 62, Issue 3 https://doi.org/10.1007/bf01080956	journal	March 1996
H2 CARS thermometry in a fuel-rich, premixed, laminar CH4/air flame in the pressure range between 5 and 40 bar Bergmann, V.; Stricker, W. Applied Physics B Laser and Optics, Vol. 61, Issue 1 https://doi.org/10.1007/bf01090971	journal	July 1995
Time-domain measurements of S-branch N2–N2 Raman linewidths using picosecond pure rotational coherent anti-Stokes Raman spectroscopy Kliewer, C. J.; Bohlin, A.; Nordström, E. Applied Physics B, Vol. 108, Issue 2 https://doi.org/10.1007/s00340-012-5037-2	journal	May 2012
The analysis of the precision of single shot 2λ-CARS temperature measurements in hydrogen Clauss, W.; Kozlov, D. N.; Pykhov, R. L. Applied Physics B, Vol. 65, Issue 4-5 https://doi.org/10.1007/s003400050323	journal	October 1997
Hybrid fs/ps rotational CARS temperature and oxygen measurements in the product gases of canonical flat flames Kearney, Sean P. Combustion and Flame, Vol. 162, Issue 5 https://doi.org/10.1016/j.combustflame.2014.11.036	journal	May 2015
Rotational CARS for simultaneous measurements of temperature and concentrations of N2, O2, CO, and CO2 demonstrated in a CO/air diffusion flame Vestin, Fredrik; Bengtsson, Per-Erik Proceedings of the Combustion Institute, Vol. 32, Issue 1 https://doi.org/10.1016/j.proci.2008.06.027	journal	January 2009
Picosecond time-resolved pure-rotational coherent anti-Stokes Raman spectroscopy in sooting flames Kliewer, Christopher J.; Gao, Yi; Seeger, Thomas Proceedings of the Combustion Institute, Vol. 33, Issue 1 https://doi.org/10.1016/j.proci.2010.05.067	journal	January 2011
Development of temperature evaluation of pure Rotational Coherent Anti-Stokes Raman Scattering (RCARS) spectra influenced by spatial averaging effects Gao, Yi; Seeger, Thomas; Leipertz, Alfred Proceedings of the Combustion Institute, Vol. 35, Issue 3 https://doi.org/10.1016/j.proci.2014.07.067	journal	January 2015
Femtosecond CARS on H2 Lang, T.; Kompa, K. -L; Motzkus, M. Chemical Physics Letters, Vol. 310, Issue 1-2 https://doi.org/10.1016/s0009-2614(99)00787-3	journal	August 1999
Nitrogen and hydrogen CARS temperature measurements in a hydrogen/air flame using a near-adiabatic flat-flame burner Hancock, Robert D.; Bertagnolli, Kenneth E.; Lucht, Robert P. Combustion and Flame, Vol. 109, Issue 3 https://doi.org/10.1016/s0010-2180(96)00191-5	journal	May 1997
Spatial averaging effects in CARS thermometry of a nonpremixed flame Garman, J. Combustion and Flame, Vol. 115, Issue 4 https://doi.org/10.1016/s0010-2180(98)00021-2	journal	December 1998
CARS thermometry in high pressure rocket combustors Grisch, Frédéric; Bouchardy, Paul; Clauss, Walter Aerospace Science and Technology, Vol. 7, Issue 4 https://doi.org/10.1016/s1270-9638(03)00017-8	journal	June 2003
Direct Coherent Raman Temperature Imaging and Wideband Chemical Detection in a Hydrocarbon Flat Flame Bohlin, Alexis; Kliewer, Christopher J. The Journal of Physical Chemistry Letters, Vol. 6, Issue 4 https://doi.org/10.1021/acs.jpclett.5b00014	journal	February 2015
Diagnostic Imaging in Flames with Instantaneous Planar Coherent Raman Spectroscopy Bohlin, A.; Kliewer, C. J. The Journal of Physical Chemistry Letters, Vol. 5, Issue 7 https://doi.org/10.1021/jz500384y	journal	March 2014
Line Intensities in the Raman Effect of ¹ Σ Diatomic Molecules James, Thomas C.; Klemperer, William The Journal of Chemical Physics, Vol. 31, Issue 1 https://doi.org/10.1063/1.1730279	journal	July 1959
Measurement of vibrational, gas, and rotational temperatures of H2 (X1Σg+) in radio frequency inductive discharge plasma by multiplex coherent anti-Stokes Raman scattering spectroscopy technique Shakhatov, V. A.; De Pascale, O.; Capitelli, M. Physics of Plasmas, Vol. 12, Issue 2 https://doi.org/10.1063/1.1829065	journal	February 2005
Femtosecond time resolved coherent anti-Stokes Raman spectroscopy: Experiment and modelization of speed memory effects on H2–N2 mixtures in the collision regime Tran, H.; Joubert, P.; Bonamy, L. The Journal of Chemical Physics, Vol. 122, Issue 19 https://doi.org/10.1063/1.1894020	journal	May 2005
Femtosecond time resolved coherent anti-Stokes Raman spectroscopy of H2–N2 mixtures in the Dicke regime: Experiments and modeling of velocity effects Tran, H.; Chaussard, F.; Le Cong, N. The Journal of Chemical Physics, Vol. 131, Issue 17 https://doi.org/10.1063/1.3257640	journal	November 2009
Direct measurement of rotationally resolved H2 Q-branch Raman coherence lifetimes using time-resolved picosecond coherent anti-Stokes Raman scattering Kulatilaka, Waruna D.; Hsu, Paul S.; Stauffer, Hans U. Applied Physics Letters, Vol. 97, Issue 8 https://doi.org/10.1063/1.3483871	journal	August 2010
Competitive partitioning of rotational energy in gas ensemble equilibration McCaffery, Anthony J.; Marsh, Richard J. The Journal of Chemical Physics, Vol. 136, Issue 2 https://doi.org/10.1063/1.3675638	journal	January 2012
Rotational Raman intensities and the measured change with internuclear distance of the polarizability anisotropy of H ₂ , D ₂ , N ₂ , O ₂ , and CO Asawaroengchai, Chamnong; Rosenblatt, Gerd M. The Journal of Chemical Physics, Vol. 72, Issue 4 https://doi.org/10.1063/1.439412	journal	February 1980
Direct measurement of S-branch N ₂ -H ₂ Raman linewidths using time-resolved pure rotational coherent anti-Stokes Raman spectroscopy Bohlin, A.; Nordström, E.; Patterson, B. D. The Journal of Chemical Physics, Vol. 137, Issue 7 https://doi.org/10.1063/1.4742915	journal	August 2012
Communication: Simplified two-beam rotational CARS signal generation demonstrated in 1D Bohlin, Alexis; Patterson, Brian D.; Kliewer, Christopher J. The Journal of Chemical Physics, Vol. 138, Issue 8 https://doi.org/10.1063/1.4793556	journal	February 2013
Single-shot hyperspectral coherent Raman planar imaging in the range 0–4200 cm ⁻¹ Bohlin, Alexis; Kliewer, Christopher J. Applied Physics Letters, Vol. 105, Issue 16 https://doi.org/10.1063/1.4900477	journal	October 2014
A New Technique for the Spectroscopic Examination of Flames at Normal Pressures Wolfhard, H. G.; Parker, W. G. Proceedings of the Physical Society. Section A, Vol. 62, Issue 11 https://doi.org/10.1088/0370-1298/62/11/305	journal	November 1949
Measurement of the self-broadening of the H 2 Q (0–5) Raman transitions from 295 to 1000 K Rahn, Larry A.; Farrow, R. L.; Rosasco, G. J. Physical Review A, Vol. 43, Issue 11 https://doi.org/10.1103/physreva.43.6075	journal	June 1991
The solid molecular hydrogens in the condensed phase: Fundamentals and static properties Silvera, Isaac F. Reviews of Modern Physics, Vol. 52, Issue 2 https://doi.org/10.1103/revmodphys.52.393	journal	April 1980
Multiplex H_2 coherent anti-Stokes Raman scattering thermometry with a modeless laser Kaminski, Clemens F.; Ewart, Paul Applied Optics, Vol. 36, Issue 3 https://doi.org/10.1364/ao.36.000731	journal	January 1997
Gas-phase thermometry using delayed-probe-pulse picosecond coherent anti-Stokes Raman scattering spectra of H_2 Stauffer, Hans U.; Kulatilaka, Waruna D.; Hsu, Paul S. Applied Optics, Vol. 50, Issue 4 https://doi.org/10.1364/ao.50.000a38	journal	November 2010
Optimizing Czerny–Turner Spectrographs: A Comparison between Analytic Theory and Ray Tracing Reader, Joseph Journal of the Optical Society of America, Vol. 59, Issue 9 https://doi.org/10.1364/josa.59.001189	journal	January 1969
Measurement of nonresonant third-order susceptibilities of various gases by the nonlinear interferometric technique Hahn, Jae Won; Lee, Eun Seong Journal of the Optical Society of America B, Vol. 12, Issue 6 https://doi.org/10.1364/josab.12.001021	journal	January 1995
Spectral restoration for femtosecond spectral interferometry with attosecond accuracy Yetzbacher, Michael K.; Courtney, Trevor L.; Peters, William K. Journal of the Optical Society of America B, Vol. 27, Issue 5 https://doi.org/10.1364/josab.27.001104	journal	January 2010
Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering Miller, Joseph D.; Roy, Sukesh; Slipchenko, Mikhail N. Optics Express, Vol. 19, Issue 16 https://doi.org/10.1364/oe.19.015627	journal	January 2011
Interference-free gas-phase thermometry at elevated pressure using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering Miller, Joseph D.; Dedic, Chloe E.; Roy, Sukesh Optics Express, Vol. 20, Issue 5 https://doi.org/10.1364/oe.20.005003	journal	January 2012
Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering temperature and concentration measurements using two different picosecond-duration probes Kearney, Sean P.; Scoglietti, Daniel J.; Kliewer, Christopher J. Optics Express, Vol. 21, Issue 10 https://doi.org/10.1364/oe.21.012327	journal	January 2013
Dual-pump vibrational/rotational femtosecond/picosecond coherent anti-Stokes Raman scattering temperature and species measurements Dedic, Chloe E.; Miller, Joseph D.; Meyer, Terrence R. Optics Letters, Vol. 39, Issue 23 https://doi.org/10.1364/ol.39.006608	journal	January 2014

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Rotational CARS thermometry and concentration measurements in ethane-nitrogen mixtures using Fourier analysis Hosseinnia, Ali; Nordström, Emil; Fatehi, Hesameddin Journal of Raman Spectroscopy, Vol. 49, Issue 7 https://doi.org/10.1002/jrs.5339	journal	February 2018

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