Electric field second harmonic generation

Many of the different susceptibilities in Equations (2.165)-(2.167) correspond to important experiments in linear and nonlinear optics. x<(>> describes a possible zero-order (permanent) polarization of the medium j(1)(0 0) is the first-order static susceptibility which is related to the permittivity at zero frequency, e(0), while ft> o>) is the linear optical susceptibility related to the refractive index n" at frequency to. Turning to nonlinear effects, the Pockels susceptibility j(2)(- to, 0) and the Kerr susceptibility X(3 —to to, 0,0) describe the change of the refractive index induced by an externally applied static field. The susceptibility j(2)(—2to to, to) describes frequency doubling usually called second harmonic generation (SHG) and j(3)(-2 to, to, 0) describes the influence of an external field on the SHG process which is of great importance for the characterization of second-order NLO properties in solution in electric field second harmonic generation (EFISHG). 

Dadap J I, Shan J, Weling A S, Misewich J A, Nahata A and Heinz T F 1999 Measurement of the vector character of electric fields by optical second-harmonic generation Opt. Lett. 24 1059-61... 

Ohihoff C, Lupke G, Meyer C and Kurz H 1997 Static and high-frequency electric fields in silicon MOS and MS structures probed by optical second-harmonic generation Phys. Rev. B 55 4596-606... 

As was proven later by Bishop [19], the coefficient A in the expansion (73) is the same for all optical processes. If the expansion (73) is extended to fourth-order [4,19] by adding the term the coefficient B is the same for the dc-Kerr effect and for electric field induced second-harmonic generation, but other fourth powers of the frequencies than are in general needed to represent the frequency-dependence of 7 with process-independent dispersion coefficients [19]. Bishop and De Kee [20] proposed recently for the all-diagonal components yaaaa the expansion... 

Table 1 Coefficients for 7[ (a ) for third harmonic generation (THG), degenerate four wave mixing (DFWM), electric field induced second harmonic generation (ESHG), and Kerr effect in methane at the experimental geometry rcH = 2.052 a.u. A CCSD wavefunction and the t-aug-cc-pVDZ basis were used. (Results given in atomic units, the number in parentheses indicate powers of ten.)...

The CCSD model gives for static and frequency-dependent hyperpolarizabilities usually results close to the experimental values, provided that the effects of vibrational averaging and the pure vibrational contributions have been accounted for. Zero point vibrational corrections for the static and the electric field induced second harmonic generation (ESHG) hyperpolarizability of methane have recently been calculated by Bishop and Sauer using SCF and MCSCF wavefunctions [51]. 

In addition to the fourth-order response field Tfourth, the probe light generates two SH fields of the same frequency 211, the pump-free SH field Eq(2 Q), and the pump-induced non-modulated SH field non(td> 211). The ground-state population is reduced by the pump irradiation and the SH field is thereby weakened. The latter term non(td, 211) is a virtual electric field to represent the weakened SH field. Time-resolved second harmonic generation (TRSHG) has been applied to observe E on (td, 211) with a picosecond time resolution [20-25]. The fourth-order field interferes with the two SH fields to be detected in a heterodyned form. 

Lantz, J. M. and Corn, R. M. (1994) Electrostatic field measurements and hand fiattening during electron-transfer processes at single-crystal Ti02 electrodes by electric field-induced optical second harmonic generation. J. Phys. Chem., 98, 4899-4905. 

Nonlinear second order optical properties such as second harmonic generation and the linear electrooptic effect arise from the first non-linear term in the constitutive relation for the polarization P(t) of a medium in an applied electric field E(t) = E cos ot. 

The first and third order terms in odd powers of the applied electric field are present for all materials. In the second order term, a polarization is induced proportional to the square of the applied electric field, and the. nonlinear second order optical susceptibility must, therefore, vanish in crystals that possess a center of symmetry. In addition to the noncentrosymmetric structure, efficient second harmonic generation requires crystals to possess propagation directions where the crystal birefringence cancels the natural dispersion leading to phase matching. 

Experimental and theoretical results are presented for four nonlinear electrooptic and dielectric effects, as they pertain to flexible polymers. They are the Kerr effect, electric field induced light scattering, dielectric saturation and electric field induced second harmonic generation. We show the relationship between the dipole moment, polarizability, hyperpolarizability, the conformation of the polymer and these electrooptic and dielectric effects. We find that these effects are very sensitive to the details of polymer structure such as the rotational isomeric states, tacticity, and in the case of a copolymer, the comonomer composition. 

Electric field Induced Second Harmonic Generation... 

We have shown in this paper the relationships between the fundamental electrical parameters, such as the dipole moment, polarizability and hyperpolarizability, and the conformations of flexible polymers which are manifested in a number of their electrooptic and dielectric properties. These include the Kerr effect, dielectric polarization and saturation, electric field induced light scattering and second harmonic generation. Our experimental and theoretical studies of the Kerr effect show that it is very useful for the characterization of polymer microstructure. Our theoretical studies of the NLDE, EFLS and EFSHG also show that these effects are potentially useful, but there are very few experimental results reported in the literature with which to test the calculations. More experimental studies are needed to further our understanding of the nonlinear electrooptic and dielectric properties of flexible polymers. 

Figure 9.3 Schematic illustration of second-order nonlinear optical effects, (a) Second-harmonic generation. Two light fields at frequency go are incident on medium with nonvanishing / 2. Nonlinear interaction with medium creates new field at frequency 2 go. (b) Frequency mixing. One light field at frequency GO and one at frequency go2 is incident on nonlinear medium. Nonlinear interaction with medium creates new field at frequency goi + go2. (c) electro-optic effect. Static electric field E (0) applied over nonlinear medium changes phase of an incoming light field.

Electric discharge ozone generator, 77 798 Electric-field-induced second harmonic generation (EFISH), 20 515 Electric field intensity, exponents of dimensions, 8 585t Electric field perturbations, 74 616 Electric fields... 

Non-linear second-order optical properties such as second harmonic generation (SHG) and the linear electrooptic effect are due to the non-linear susceptibility in the relation between the polarization and the applied electric field. SHG involves the... 

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