Second-Order Nonlinear Optical Effects at Surfaces and Interfaces

Heinz, Tony F.

doi:10.1016/b978-0-444-88359-9.50011-9

Cited by 257 publications

(291 citation statements)

References 188 publications

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“…In fact, further, increasing efforts have to be made to develop the field further in this direction. It has been impossible, in this short review to cover all innovative developments, in particular with respect to in situ experimental studies, where a lot of innovative approaches have been launched recently, including ambient pressure X-ray photoelectron spectroscopy [92], non-linear optical spectroscopy [93], ambient pressure scanning tunneling microscopy [94], in situ transmission electron microscopy with Cs correction [95] and many more, but we have rather chosen here to address the development of model systems that move towards capturing structural and functional features of real catalysts, which then in the future may be addressed with this increasing toolbox of new techniques, which are under rapid development at present.…”

Section: Discussionmentioning

confidence: 99%

Models in Catalysis

2014

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The paper discusses the hierarchy of model studies with increasing complexity towards an understanding of industrial catalysts under reaction conditions. We use three case studies to document the progress in systems complexity as well as the development of instruments that allow us to approach the study of acting catalysts: magnesium oxide clusters in the gas phase, gold nanoparticles on metal oxide surfaces, and palladium nanoparticles compared to crystal surfaces. While the examples are from the field of heterogeneous catalysis, we discuss the relation to homogeneous and enzymatic catalysis.

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Section: Discussionmentioning

confidence: 99%

Models in Catalysis

2014

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“…The expressions in the Eq.37 and the Eq.39 are exactly the same as those in the previous treatment by Heinz and Shen. 4,34,53,54,55 This indicates that the treatment with the square point-dipole lattice model together with a molecular optics approach is at least phenomenologically correct. It also further validates the treatment in the original literatures.…”

Section: 84mentioning

confidence: 99%

“…By solving the Maxwell's equations which satisfy the boundary conditions at the infinitesimally thin polarization sheet layer, Heinz and Shen provided the theoretical basis for the interface specific SHG, as well as the SFG-VS, in the interface studies. 4,34,54,55 Parallel to this macroscopic treatment, Ye and Shen employed a classical induced point-dipole model to include the microscopic local field effect on the nonlinear optical properties of adsorbed molecules on a substrate. 56 Shen later realized that from the theoretical point of view, the dielectric constant in the macroscopic model is not well defined for a monolayer because it is a macroscopic or mesoscopic property.…”

Section: Introductionmentioning

confidence: 99%

“…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. 4,34,54,55 This model was a natural extension of the original formulation by Bloembergen and Pershan, where a nonlinear plane parallel slab with a finite thickness embedded between two linear dielectrics was the source of the SHG radiation, and where the Maxwell's equations which satisfy the boundary conditions at the two plane interfaces were accurately solved.…”

Section: Introductionmentioning

confidence: 99%

“…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. 4,34,54,55 This model was a natural extension of the original formulation by Bloembergen and Pershan, where a nonlinear plane parallel slab with a finite thickness embedded between two linear dielectrics was the source of the SHG radiation, and where the Maxwell's equations which satisfy the boundary conditions at the two plane interfaces were accurately solved. 35 However, according to that treatment, Bloembergen and Pershan concluded that the surface dipolar contribution to the SHG signal should be overwhelmed by the quadrupolar radiation in the much thicker boundary layer.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

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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Optical Second-Harmonic Generation as a Semiconductor Surface and Interface Probe

McGilp

1999

phys. stat. sol. (a)

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Optical second‐harmonic generation, although a sophisticated technique, is making a significant contribution to the characterization of surfaces and interfaces. Advantages include: all pressure ranges being accessible; insulators being studied without the problem of charging effects; solid–solid and solid–liquid interfaces being characterized by utilizing the large penetration depth of optical radiation. Single wavelength studies yield information on the crystallographic and magnetic structure of surfaces and interfaces, and are particularly sensitive to symmetry changes. Spectroscopic and time‐resolved studies, which have recently become simpler due to the availability of high pulse power, tunable, broad band laser sources, additionally provide electronic structure and dynamics information, although interpretation may not be simple. Recent examples from well‐characterized semiconductor interfaces are discussed, and it is shown that the technique is now well understood at the phenomenological level, although theoretical calculations are proving to be difficult.

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Second-Order Nonlinear Optical Effects at Surfaces and Interfaces

Cited by 257 publications

References 188 publications

Models in Catalysis

Models in Catalysis

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

Optical Second-Harmonic Generation as a Semiconductor Surface and Interface Probe

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