Spatial coherence, laser spectroscopy

Unlike the typical laser source, the zero-point blackbody field is spectrally white , providing all colours, CO2, that seek out all co - CO2 = coj resonances available in a given sample. Thus all possible Raman lines can be seen with a single incident source at tOp Such multiplex capability is now found in the Class II spectroscopies where broadband excitation is obtained either by using modeless lasers, or a femtosecond pulse, which on first principles must be spectrally broad [32]. Another distinction between a coherent laser source and the blackbody radiation is that the zero-point field is spatially isotropic. By perfonuing the simple wavevector algebra for SR, we find that the scattered radiation is isotropic as well. This concept of spatial incoherence will be used to explain a certain stimulated Raman scattering event in a subsequent section. 

Owing to aberrations, grating defects, and so on, it may not be adequate to approximate the response function by formulas based on idealized models. If a line source could be found having the spectrum that approximates a 8 function, then perhaps the measurement of such a line would adequately determine the response function. We have learned, however, that the spatial coherence of the source plays an important part in the shape of the response function. This precludes the use of a laser line source to measure the response function applicable to absorption spectroscopy. Furthermore, we... 

By contrast, laser scattering methods now permit temperature composition and flow measurements that are both nonintrusive and give very high spatial resolution. These light scattering methods include laser Raman spectroscopy, laser-induced fluorescence, coherent Raman spectroscopy as well as laser velocimetry... 

Although Raman spectroscopy does not employ absorption of infrared radiation as its fundamental principle of operation, it is combined with other infrared spectroscopies into a joint section. Results obtained with various Raman spectroscopies as described below cover vibrational properties of molecules at interfaces complementing infrared spectroscopy in many cases. A general overview of applications of laser Raman spectroscopy (LRS) as applied to electrochemical interfaces has been provided [342]. Spatially offset Raman spectroscopy (SORS) enables spatially resolved Raman spectroscopic investigations of multilayered systems based on the collection of scattered light from spatial regions of the samples offset from the point of illumination [343]. So far this technique has only been applied in various fields outside electrochemistry [344]. Fourth-order coherent Raman spectroscopy has been developed and applied to solid/liquid interfaces [345] applications in electrochemical systems have not been reported so far. 

On the other hand, many possible applications of this type of spectroscopy have remained elusive because of a lack of spectral intensity, monochromaticity, tunability and of spatial coherence of the thermal light sources. This situation changed drastically with the advent of the laser that not only brought along a renaissance of classical double resonance spectroscopy, but also the development of new coherent, nonlinear spectroscopic techniques. 

Many experiments in laser spectroscopy depend on the coherence properties of the radiation and on the coherent excitation of atomic or molecular levels. Some basic ideas about temporal and spatial coherence of optical fields and the density-matrix formalism for the description of coherence in atoms are therefore discussed at the end of this chapter. 

Two techniques, which appear well suited to the diagnostic probing of practical flames with good spatial and temporal resolution, are coherent anti-Stokes Raman spectroscopy (CARS) and saturated laser fluorescence. The two techniques are complementary in regard to their measurement capabilities. CARS appears most appropriate for thermometry and major species concentration measurements, saturated laser fluorescence to trace radical concentrations. With electronic resonant enhancement (6), CARS may be potentially useful for the latter as well. Fluorescence thermometry is also possible (7, 8) but generally, is more tedious to use than CARS. In this paper, recent research investi-... 

Another aspect of optical pumping is related to the coherent excitation of two or more molecular levels. This means that the optical excitation produces definite phase relations between the wave functions of these levels. This leads to interference effects, which influence the spatial distribution and the time dependence of the laser-induced fluorescence. This subject of coherent spectroscopy is covered in Chap. 7. 

Either two or more molecular levels of a molecule are excited coherently by a spectrally broad, short laser pulse (level-crossing and quantum-beat spectroscopy) or a whole ensemble of many atoms or molecules is coherently excited simultaneously into identical levels (photon-echo spectroscopy). This coherent excitation alters the spatial distribution or the time dependence of the total, emitted, or absorbed radiation amplitude, when compared with incoherent excitation. Whereas methods of incoherent spectroscopy measure only the total intensity, which is proportional to the population density and therefore to the square ir of the wave function iff, the coherent techniques, on the other hand, yield additional information on the amplitudes and phases of ir. 

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