A Review of the Theory and Application of Coherent Anti-Stokes Raman Spectroscopy (CARS)

1977 ◽  
Vol 31 (4) ◽  
pp. 253-271 ◽  
Author(s):  
W. M. Tolles ◽  
J. W. Nibler ◽  
J. R. McDonald ◽  
A. B. Harvey

Coherent anti-Stokes Raman spectroscopy (CARS) is a relatively new kind of Raman spectroscopy which is based on a nonlinear conversion of two laser beams into a coherent, laser-like Raman beam of high intensity in the anti-Stokes region. The emission is often many orders of magnitude greater than normal Raman scattering and, because of the coherent and anti-Stokes character of radiation, the method is very useful for obtaining Raman spectra of fluorescing samples, gases in discharges, plasmas, combustion, atmospheric chemistry. In this paper we outline the basic theory behind CARS and describe its unusual effects and drawbacks. We review the research to date on various materials, and indicate the possible future direction, utility and applications of CARS such as surface studies, fluctuation phenomena, reaction dynamics, photochemistry, kinetics, relaxation, and energy transfer.

2003 ◽  
Vol 57 (1) ◽  
pp. 93-99 ◽  
Author(s):  
Michael J. Papac ◽  
Jonathan D. Posner ◽  
Derek Dunn-Rankin

Coherent anti-Stokes Raman spectroscopy (CARS) is a nonlinear optical wave mixing process that is used in gas-phase systems to determine the energy distribution of the probed species (usually N2) and, through a fitting procedure, the temperature giving rise to it. CARS signal strengths are maximized when the phase matching condition is met. Because gases are generally non-dispersive, this phase matching condition can be found geometrically as a function of the crossing angles between the CARS beams and their wavelengths. In addition, perfect phase matching in non-dispersive media occurs automatically for collinear beams. To improve spatial resolution, however, intersecting the laser beams is desirable. Being a third-order process, phase matching for CARS in gases typically requires three input laser beams. This paper discusses and demonstrates the issues of phase matching for CARS when the medium is dispersive, and the ability for CARS phase matching to occur with only two crossed laser beams (one pump and one probe). This two-beam X-CARS in dispersive media can be used as an alignment tool for gas-phase CARS and may be relevant as a simpler diagnostic in high-pressure environments. The paper also discusses the effects of non-ideal phase matching in dispersive and non-dispersive media.


1982 ◽  
Vol 36 (5) ◽  
pp. 565-569 ◽  
Author(s):  
Haruhiko Kataoka ◽  
Shiro Maeda ◽  
Chiaki Hirose

The expression for the intensity in coherent anti-Stokes Raman spectroscopy (CARS) was derived for scanning CARS by taking into account the linewidths and phase relation of the two laser beams, and simulation procedures suited for practical applications were developed. The CARS spectra of p-xylene and N2 gas were observed, and the results were compared with the simulation curves based on two extreme cases of the statistical property of the laser source. It was shown that the effect of laser linewidth becomes remarkable when the Raman linewidth is comparable to or smaller than the laser linewidth, and that the degree of coherence among the frequency components within the laser linewidth is an important factor in determining the spectral profile.


1993 ◽  
Vol 57 (1) ◽  
pp. 56-62 ◽  
Author(s):  
S. Schneider ◽  
C.-J. Prenzel ◽  
G. Brehm ◽  
P. Gedeck ◽  
P. S. Maruthi Sai ◽  
...  

2006 ◽  
Vol 60 (10) ◽  
pp. 1097-1102 ◽  
Author(s):  
Zachary D. Schultz ◽  
Marc C. Gurau ◽  
Lee J. Richter

2001 ◽  
Vol 40 (6) ◽  
pp. 741 ◽  
Author(s):  
Thomas A. Reichardt ◽  
Paul E. Schrader ◽  
Roger L. Farrow

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