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Optical Harmonics in Molecular Systems

Optical Harmonics in Molecular Systems

David L. Andrews, Philip Allcock

ISBN: 978-3-527-60274-2

Jan 2005

253 pages

Select type: O-Book


In recent years the generation of optical harmonics in molecular systems has become an area of increasing interest for a number of reasons. First, many organic crystals and polymeric solids prove not only to have usefully large optical nonlinearities but also to be surprisingly robust and thermally stable. Consequently the fabrication of organic materials for laser frequency conversion has become very much a growth area. At interfaces and in partially ordered systems, harmonic generation is now of considerable scientific interest through the detailed structural information it affords. And in molecular gases and liquids, processes of optical harmonic conversion present a powerful tool for the study of both static and dynamic effects of molecular orientation.

Where the detailed nonlinear optical response of molecules is required, the application of molecular quantum electrodynamics (QED) brings both rigour and conceptual facility. Using this approach the authors address topics of direct experimental concern in a general formulation of theory for optical harmonics, with a particular focus on quantum optical and molecular aspects. A detailed basis is provided for the applications, enabling the characteristic features of optical nonlinearity to be examined in general terms. A great many of the optical phenomena subsequently addressed find wide application in nonlinear optics and chemical physics. Specifically, the book deals with coherent harmonic generation, both within and at interfaces between different media. It addresses elastic second harmonic (Hyper-Rayleigh) light scattering as well as the inelastic case normally referred to as Hyper-Raman scattering. Full and detailed tables and results are provided for the analysis of experimental observations.
Bulk modes in terms of fields
Bulk modes in terms of potentials
Lorentz' classical model for the dielectric function of insulators
Drude's classical model for the dielectric function of metals
Dielectric function of a plasma
Static dielectric function for a dilute gas of permanent dipoles
Debye rotational relaxation
Dielectric properties of water
Superluminal speeds
Modes at a single interface
Modes in slab geometry
The Casimir effect
Metal surfaces
Quantum wells
Two molecules with permanent dipole moments
One ion and one molecule with permanent dipole moment
Two molecules one with and one without permanent dipole moment
Two molecules without permanent dipole moments
Two ions
Three or more polarizable atoms
Ineraction between macroscopic objects
Interaction between two spheres: limiting results
Interaction betweeen two spheres: general results
Gernal expression for small separations
Cylinders and half-spaces
Summation of pair interactions
Derivation of the van der Waals equations of state
Interaction energy at zero temperature
Interaction energy at finite temperature
Surface energy, method 1: no retardation
Surface energy, method 1: retardation
Surface energy, method 2: no retardation
Surface energy, method 2: retardation
Finite temperatures
Recent results for metals
Adhesion, cohersion, and wetting
Finding the pair interactions
Modes at the surface of a sphere
Modes at the surface of a cylinder
Modes at an edge
Modes in a needle (a paraboloid of revolution)
Polar semiconductors or ionic insulators
Metallic systems
Characterization of different surface mode types
Spatial dispersion
Surface roughness
The ATR method
Earthquakes, rainbow and optical glory
Stability of colloids
Formation of the double layer
Gouy and Chapman theory
Stern's theory of a flat double layer
The Zeta-potential
Interaction energy and force between