Nonlinear optical properties of Langmuir–Blodgett monolayers: Local-field effects

Cnossen, Gerard; Drabe, Karel E.; Wiersma, Douwe A.

doi:10.1063/1.463895

Cited by 45 publications

(28 citation statements)

References 43 publications

(2 reference statements)

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“…Preliminary SHG measurements were carried out according to the method of Cnossen et al [ 18]. Assuming the total polymeric structure, including the side chains, to be rigid, poly(isocyanide)s prepared from racemic mixtures of monomers were not expected to generate any second-harmonic signal.…”

Section: Nlo Propertiesmentioning

confidence: 99%

Mixed mono- and multilayers of poly(isocyanide)s with non-linear optically active side chains

et al. 1994

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Take-down policy If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. AbstractThe properties and structure of Langmuir-Blodgett mono-and multilayers of several poly(isocyanide)s with non-linear optically active side-chains were studied. These polymers formed very rigid layers or layers which appeared to be unstable. To circumvent this problem they were mixed with other poly(isocyanide)s or with amylose-butyrate. Transmission electron microscopy studies of the polymeric mixtures revealed that phase separation occurred in all cases and that only poly(isocyanide)s substituted with hydrophilic side chains formed monomolecular layers. Depending on the nature of the polymer which was used for mixing, the dye polymers could be deposited with Y-or Z-type transfer. Second-harmonic intensities generated from these films were small in the case of the Y-type multilayered films and moderately high in the case of the Z-type films.

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Section: Nlo Propertiesmentioning

confidence: 99%

Mixed mono- and multilayers of poly(isocyanide)s with non-linear optically active side chains

et al. 1994

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“…Such films possess spectral peculiarities close to those of selfaggregated polymethine dyes in aqueous solution and the nonlinear optical properties characteristic for molecular organic materials with highly delocalized r-electron system. Study of primary processes of photoexcited LB films of dye aggregates as well as investigation of nonlinear properties of LB mono-and multilayers is of great importance aiming to the understanding of the relationship between the optical nonlinearity, relaxation rates and mechanisms, structure and dimensionality of molecular assembly [5][6][7][8][9].…”

Section: Introductionmentioning

confidence: 99%

Near‐Resonant Nonlinear OpticalProperties of Pseudoisocyanine J‐Aggregates in Langmuir‐BlodgettLayers

Feller

Gadonas²,

Moebius

1997

Laser Chemistry

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The nonlinear optical properties of pseudoisocyanine J-aggregates in Langmuir-Blodgett films have been investigated by means of degenerate four wave mixing (DFWM) process. The conversion efficiency of the DFWM signal and the estimated third order susceptibility were found to be comparable with those of pseudoisocyanine J-aggregates in solution under comparable resonance conditions. The intensity dependence of the converted (DFWM) signal is interpreted as resulting from different processes including saturation, exciton-exciton annihilation and secondary processes of dynamical disorder.

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“…43,44,45,46,47,48,49,50,51,81 Therefore, we shall neglect the image induced dipole term in the followed treatment.…”

Section: 89mentioning

confidence: 99%

“…26,59,60,61 There have been a few experimental and empirical theory studies on the SHG data from the interfacial monolayer, using different parameters of the macroscopic three layer model plus the microscopic local field factors. 43,44,45,46,47,48,49,50,51,62,63,64 In dealing with the macroscopic dielectric constant, generally one of the two bulk phase values were used, reducing the macroscopic problem to the same as the so-called two phase model.…”

Section: 25mentioning

confidence: 99%

“…the anisotropic two dimensional microscopic local field effect. 21,25,41,42,43,44,45,46,47,48,49,50,51,52,53 It has been well demonstrated that in majority cases the calculation of the molecular orientation is quite sensitive to the values used for these two factors. 21,25,42,51,52 In the currently accepted models of the nonlinear optics of interface, 4,34,41,53,54,55 the nonlinear radiation was treated as the result of an infinitesimally thin polarization sheet layer, and as the starting pint a macroscopic dielectric constant was assigned to this thin layer.…”

Section: Introductionmentioning

confidence: 99%

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Microscopic molecular optics theory of surface second harmonic generation and sum-frequency generation spectroscopy based on the discrete dipole lattice model

Dong¹,

Yuan²,

Liu³

et al. 2008

International Reviews in Physical Chemistry

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Two crucial issues in the interface studies with the interface specific nonlinear spectroscopy are on how to describe the macroscopic dielectric constant of the molecularly thin layer and how to calculate the anisotropic two dimensional microscopic local field effect. In the currently accepted models of the nonlinear optics, the nonlinear radiation was treated as the result of an infinitesimally thin polarization sheet layer, and a three layer model was generally employed. The direct consequence of this approach is that an apriori dielectric constant, which still does not have a clear definition, has to be assigned to this polarization layer. Because the Second Harmonic Generation (SHG) and the Sum-Frequency Generation vibrational Spectroscopy (SFG-VS) have been proven as the sensitive probes for interfaces with the submonolayer coverage, the treatment based on the more realistic discrete induced dipole model needs to be developed. Here we show that following the molecular optics theory approach the SHG, as well as the SFG-VS, radiation from the monolayer or submonolayer at an interface can be rigorously treated as the radiation from an induced dipole lattice at the interface. In this approach, the introduction of the polarization sheet is no longer necessary. Therefore, the ambiguity of the unaccounted dielectric constant of the polarization layer is no longer an issue. Moreover, the anisotropic two dimensional microscopic local field factors can be explicitly expressed with the linear polarizability tensors of the interfacial molecules. Based on the planewise dipole sum rule in the molecular monolayer, crucial experimental tests of this microscopic treatment with SHG and SFG-VS are discussed. Many puzzles in the literature of surface SHG and SFG spectroscopy studies can also be understood or resolved in this framework. This new treatment may provide a solid basis for the quantitative analysis in the surface SHG and SFG studies.

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Nonlinear optical properties of Langmuir–Blodgett monolayers: Local-field effects

Cited by 45 publications

References 43 publications

Mixed mono- and multilayers of poly(isocyanide)s with non-linear optically active side chains

Mixed mono- and multilayers of poly(isocyanide)s with non-linear optically active side chains

Near‐Resonant Nonlinear OpticalProperties of Pseudoisocyanine J‐Aggregates in Langmuir‐BlodgettLayers

Microscopic molecular optics theory of surface second harmonic generation and sum-frequency generation spectroscopy based on the discrete dipole lattice model

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