Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy

Abstract Time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of the nitrogen molecule is used for the measurement of temperature in atmospheric-pressure, near-adiabatic, hydrogen-air diffusion flames. The initial frequency-spread dephasing rate of the Raman coherence induced by the ultrafast (∼85 fs) Stokes and pump beams is used as a measure of gas-phase temperature. This initial frequency-spread dephasing rate of the Raman coherence is completely independent of collisions and depends only on the frequency spread of the Raman transitions at different temperatures. A simple theoretical model based on the assumption of impulsive excitation of Raman coherence is used to extract temperatures from time-resolved fs-CARS experimental signals. The extracted temperatures from fs-CARS signals are in excellent agreement with the theoretical temperatures calculated from an adiabatic equilibrium calculation. The estimated absolute accuracy and the precision of the measurement technique are found to be ±40 K and ±50 K, respectively, over the temperature range 1500–2500 K.

[1]  Marlan O Scully,et al.  Optimizing the Laser-Pulse Configuration for Coherent Raman Spectroscopy , 2007, Science.

[2]  Sukesh Roy,et al.  Temperature profile measurements in the near-substrate region of low-pressure diamond-forming flames , 2002 .

[3]  A. H. Zewail,et al.  Femtosecond laser observations of molecular vibration and rotation , 1990, Nature.

[4]  A. Eckbreth Laser Diagnostics for Combustion Temperature and Species , 1988 .

[5]  P. Beaud,et al.  Determination of the ortho-/para deuterium concentration ratio with femtosecond CARS , 2003 .

[6]  M. Motzkus,et al.  Single-shot femtosecond coherent anti-Stokes Raman-scattering thermometry , 2002 .

[7]  Marek Tulej,et al.  Pressure‐dependent N2 Q‐branch fs‐CARS measurements , 2002 .

[8]  Sukesh Roy,et al.  Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals , 2005 .

[9]  M. Dantus,et al.  Coherent nonlinear spectroscopy: from femtosecond dynamics to control. , 2001, Annual review of physical chemistry (Print).

[10]  R. Lucht Femtosecond Lasers for Molecular Measurements , 2007, Science.

[11]  M D Duncan,et al.  Scanning coherent anti-Stokes Raman microscope. , 1982, Optics letters.

[12]  P. Beaud,et al.  High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature , 2001 .

[13]  G. Mourou,et al.  Laser ablation and micromachining with ultrashort laser pulses , 1997 .

[14]  Robert P Lucht,et al.  Theory of femtosecond coherent anti-Stokes Raman scattering spectroscopy of gas-phase transitions. , 2007, The Journal of chemical physics.

[15]  R. Farrow,et al.  Comparison between CARS and corrected thermocouple temperature measurements in a diffusion flame. , 1982, Applied optics.

[16]  M. Blades,et al.  Background-Free Coherent Anti-Stokes Raman Scattering of Gas- and Liquid-Phase Samples in a Mesoporous Silica Aerogel Host , 2007, Applied spectroscopy.

[17]  W. R. Wiley,et al.  Three-Dimensional Vibrational Imaging by Coherent Anti-Stokes Raman Scattering , 1999 .

[18]  R. Leonhardt,et al.  Terahertz quantum beats in molecular liquids , 1987 .

[19]  R. E. Palmer,et al.  The CARSFT computer code calculating coherent anti-Stokes Raman spectra: User and programmer information , 1989 .

[20]  Broadband Coherent Anti-Stokes Raman Spectroscopy Characterization of Polymer Thin Films , 2006, Applied spectroscopy.

[21]  M. Schmitt,et al.  The Application of Femtosecond Time-Resolved Coherent Anti-Stokes Raman Scattering for the Investigation of Ground and Excited State Molecular Dynamics of Molecules in the Gas Phase , 1998 .

[22]  S. Turns An Introduction to Combustion: Concepts and Applications , 2000 .

[23]  M. Afzelius,et al.  Dual-pump dual-broadband coherent anti-Stokes Raman scattering in reacting flows. , 2004, Optics letters.

[24]  A. Zewail,et al.  Femtosecond Photofragment Spectroscopy: The Reaction ICN → CN + I , 1985 .

[25]  K. Kompa,et al.  Femtosecond CARS on H2 , 1999 .

[26]  Robert P. Lucht,et al.  Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence , 2006 .

[27]  D. Chandler,et al.  Femtosecond time‐resolved studies of coherent vibrational Raman scattering in large gas‐phase molecules , 1995 .