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Optically nonlinear Langmuir-Blodgett films: Influence of the substrate on film structure and linear optical properties Detailed measurements of the macroscopic second-order optical nonlinearity X(2) (2w,w,w) of Langmuir-Blodgett dye-doped monolayers are reported. The observed deviations from a linear behavior of X(2) with increasing surface density are shown to be due to local-field effects. In order to calculate these local-field factors for disordered systems, a novel Monte Carlo type calculation is introduced. This calculation not only accounts for density variations in the monolayers but also incorporates the effect of off-diagonal elements of the (microscopic) linear susceptibility tensor. Quantitative agreement is found between the calculations and the experimental results using only the molecular hyperpolarizability as a free parameter. A method is presented to determine the tilt angle of the chromophores in Langmuir-Blodgett monolayers from the anisotropy of the linear absorption. The tilt angle determined this way is in excellent agreement with a determination by secondharmonic generation.4512
Articles you may be interested inRotationally resolved photoelectron spectra in resonance enhanced multiphoton ionization of HCl via the F 1Δ2 Rydberg state J. Chem. Phys. 95, 8718 (1991); 10.1063/1.461256 Rotational branching ratios and photoelectron angular distributions in resonance enhanced multiphoton ionization of HBr via the F 1Δ2 Rydberg state J. Chem. Phys. 95, 7872 (1991); 10.1063/1.461316 A study of some Rydberg states of CO2 by (3+1) multiphoton ionization spectroscopy J. Chem. Phys. 91, 7399 (1989); 10.1063/1.457264 Multiphoton ionization photoelectron spectroscopy study of OCS: Rydberg vibronic structure and ion state selection J. Chem. Phys. 89, 5527 (1988); 10.1063/1.455559Resonant multiphoton ionization photoelectron spectroscopic study of benzene. Evidence for fast intramolecular vibrational relaxation within the 1 E 1u state ~i~eti,: energy r~solv.ed. electron detection is used to study resonance enhanced multiphoton 10mzatIOn and dissociation of molecular chlorine via the 2 III g Rydberg state. In the twop,hoton ener~ regio? bet~e~n 63 ~ and 73 600 cm -I, a long vibrational progression up to v = 1.5 associated with this mtermedlate gerade Rydberg state is observed. The regularity and magmtude of the vibrational spacing indicate that the 2 IIIg state, converging to the ionic ground state, has virtually unperturbed Rydberg character. However, the molecular signals in the photoelectron spectra show strong deviations from Franck-Condon behavior. In addition intense electron signals arising from one-photon ionization of excited chlorine atoms are ' observed. An interpretation in terms of a competition between electronic autoionization and dissociation from core-excited molecular Rydberg states situated above the lowest ionization energy is ~resent~d. Some of t?e excited atomic states observed are indicative for Rydberg-Rydberg mteracttons at large mtemuclear distances in the dissociation channel.6042
The lowest excited singlet 1 B 3u state of pyrazine is known to be coupled to a number of triplet 3 B states. Using a strongly collimated molecular beam and a single frequency laser it is sh~~ that the J I = 0 of the og transition contains at least 36 states. We have individually excited eight ofthese states and studied its decay. The lifetimes found (typically 450 ns) ~o.not scale with the intensities of the excitation spectrum. This deviation is caused by a nonradlatlve decay of the zero order 3 B 3" states. With a simple model it was possible to reconstruct the absorption spectrum, the energies of the zero order states and its coupling strengths. The zero order decay rates of the singlet and triplet s~ates have been determined. The value obtained for the zero order singlet state is 5 MHz; the values for the triplet states range from 0.6 to about 5 MHz.
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