Optical Second Harmonic Generation Studies of Azobenzene Surfactant Adsorption and Photochemistry at the Water/1,2-Dichloroethane Interface

Naujok, Roberta R.; Paul, and Hillary J.; Corn, Robert M.

doi:10.1021/jp960558m

Cited by 64 publications

(43 citation statements)

References 87 publications

(179 reference statements)

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“…During the past two decades, much effort has been made to study this unique area mainly using surface-specific spectroscopic techniques. [1][2][3][4][5][6][7][8] The advantage of employing these techniques to monitor a buried interface between two bulk phases is that there are no mechanical perturbation problems during the measurement. However, due to the limited sensitivity of these spectroscopic techniques, target molecules were usually studied in a relatively high surface-density region.…”

mentioning

confidence: 99%

Confocal Fluorescence Microscope Studies of the Adsorptive Behavior of Dioctadecyl-rhodamine B Molecules at a Cyclohexane-Water Interface

Zheng

Harata

2001

ANAL. SCI.

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mentioning

confidence: 99%

Confocal Fluorescence Microscope Studies of the Adsorptive Behavior of Dioctadecyl-rhodamine B Molecules at a Cyclohexane-Water Interface

Zheng

Harata

2001

ANAL. SCI.

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“…42,52,58,67,68,69,70,71 In SFG-VS, some considered the film anisotropic and its optical constant is determined using the Clausius-Mossotti relationship with the ellipsometry data of the film.…”

Section: 64mentioning

confidence: 99%

“…59,60 In SHG, some considered the film isotropic and the optical constant can be obtained from the Kramers-Kronig dispersion relationship measured from the bulk or thin film UVVisible absorption spectra. 42,69,70 When the molecule is considered with uniaxial symmetry, the ratio between the dielectric constants of the fundamental and the SH frequency can be directly determined from the intensity ratio in the polarization measurements. 37,42 There are also efforts trying to show that the dielectric constant of the extremely thin monolayer is just the simple arithmetic average of the two bulk dielectric constants.…”

Section: 64mentioning

confidence: 99%

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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“…(41) are "left"-operations that act on the ket, it is possible to express the final result for the signal in Hilbert space, giving (42) Upon conversion of Eq. (41), the frequency-domain Liouville space propagators, (43) are replaced by Hilbert-space propagators…”

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confidence: 99%

Nonlinear optical spectroscopy of single, few, and many molecules: Nonequilibrium Green’s function QED approach

2008

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Nonlinear optical signals from an assembly of N noninteracting particles consist of an incoherent and a coherent component, whose magnitudes scale ~ N and ~ N(N − 1), respectively. A unified microscopic description of both types of signals is developed using a quantum electrodynamical (QED) treatment of the optical fields. Closed nonequilibrium Green's function expressions are derived that incorporate both stimulated and spontaneous processes. General (n + 1)-wave mixing experiments are discussed as an example of spontaneously generated signals. When performed on a single particle, such signals cannot be expressed in terms of the nth order polarization, as predicted by the semiclassical theory. Stimulated processes are shown to be purely incoherent in nature. Within the QED framework, heterodyne-detected wave mixing signals are simply viewed as incoherent stimulated emission, whereas homodyne signals are generated by coherent spontaneous emission.

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Optical Second Harmonic Generation Studies of Azobenzene Surfactant Adsorption and Photochemistry at the Water/1,2-Dichloroethane Interface

Cited by 64 publications

References 87 publications

Confocal Fluorescence Microscope Studies of the Adsorptive Behavior of Dioctadecyl-rhodamine B Molecules at a Cyclohexane-Water Interface

Confocal Fluorescence Microscope Studies of the Adsorptive Behavior of Dioctadecyl-rhodamine B Molecules at a Cyclohexane-Water Interface

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

Nonlinear optical spectroscopy of single, few, and many molecules: Nonequilibrium Green’s function QED approach

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