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Nonlinear Optical Probes and Processes in Polymers and Liquid ...

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work I am present<strong>in</strong>g here describes several nonl<strong>in</strong>ear optical techniques <strong>and</strong> their<br />

applications for the study of physics of organic optical materials such as polymer<br />

composites <strong>and</strong> liquid crystals.<br />

In nonl<strong>in</strong>ear optics, the nonl<strong>in</strong>ear optical response is described by express<strong>in</strong>g the<br />

dipole moment per unit volume, or polarization density P (t) of a material, as a power<br />

series <strong>in</strong> the electric field E(t) as [1]<br />

P (t) = P0 + χ (1) E(t) + χ (2) E 2 (t) + χ (3) E 3 (t) + ..., (1.1)<br />

where P0 is the <strong>in</strong>tr<strong>in</strong>sic polarization, χ (1) is the l<strong>in</strong>ear susceptibility, χ (2) <strong>and</strong> χ (3)<br />

are the second- <strong>and</strong> third-order nonl<strong>in</strong>ear optical susceptibilities. Generally, the nth<br />

order optical susceptibility χ (n) is a tensor of rank n + 1.<br />

The polarization density is important for the description of nonl<strong>in</strong>ear optical phe-<br />

nomena s<strong>in</strong>ce a time-vary<strong>in</strong>g polarization acts as a source of new components of the<br />

electromagnetic field. This is described by the wave equation <strong>in</strong> nonl<strong>in</strong>ear optical<br />

form as<br />

∇ 2 E − n2<br />

c 2<br />

∂2E 4π<br />

=<br />

∂t2 c2 ∂2P ∂t2 where n is the refractive <strong>in</strong>dex <strong>and</strong> c is the speed of light <strong>in</strong> vacuum.<br />

(1.2)<br />

For nonl<strong>in</strong>ear optical studies, it appears convenient to work <strong>in</strong> the frequency do-<br />

ma<strong>in</strong> rather than <strong>in</strong> the time doma<strong>in</strong>. In this case, if the optical electric field of a<br />

laser beam is represented as E(t) = E exp(−iωt)+c.c., then the ω Fourier component

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