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Materials | Self-Trapped Excitons

Self-Trapped Excitons

Song, K.S., Williams, Richard T.

1993, XII, 404p. 219 illus., 2 illus. in color.


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  • About this book

In crystals as diverse as sodium chloride, silicon dioxide, sold xenon, pyrene, arsenic triselenide, and silver chloride, the fundamental electronicexcitation (exciton) is localized within its own lattice distortion field very shortly after its creation. This book discusses the structure if the self-trapped exciton (STE) and its evolution along the path of its return to the ground state or to a defect state of crytal. A comprehensive review of experiments on STEs in a wide range of materials has been assembled, including extensive tables of data. Throughout, emphasisis given to the basic physics underlying various manifestations of self-trapping. The role of the spontaneous symmetry-breaking or "off-center"relaxation in STE structure is examined thoroughly, and leads naturally to the subject of lattice defect formation as a product of STE relaxation. The theory of STEs is developed from a localized, atomistic perspective using self-consistent methods adapted from the theory of defects in solids. At this time of rapid progress in STEs, researchers will welcome the first monograph dedicaded solely to this topic.

Content Level » Research

Keywords » Alkali Halides - Defects - Excitons - Luminescene - Self-Trapping

Related subjects » Materials - Optics & Lasers - Physical Chemistry

Table of contents 

1 Introduction.- 1.1 Excitons.- 1.1.1 One-Electron Band State.- 1.1.2 Exciton State.- 1.1.3 Absorption Spectr.- 1.1.4 Luminescence Spectra.- 1.2 Charge Carriers and Excitons in a Deformable Lattice.- 1.2.1 Polarons.- 1.2.2 Self-Trapping in a Continuum Model.- 1.2.3 The Electron-Hole System in a Deformable Lattice.- 1.2.4 Exciton-Phonon Coupling Constant from the Urbach Edge.- 1.3 Scope of this Monograph.- 2 Investigation of Self-Trapped Excitons from a Defect Perspective.- 2.1 Atomistic Structure of Self-Trapped Carriers.- 2.1.1 Self-Trapped Holes.- 2.1.2 Self-Trapped Electrons.- 2.2 Self-Trapped Excitons.- 2.3 Experimental Methods.- 2.3.1 Transient Optical Absorption and Emission.- 2.3.2 Photoconversion Spectroscopy.- 2.3.3 Synchrotron Radiation Studies.- 2.3.4 Optically Detected Magnetic Resonance.- 2.4 Theoretical Methods.- 2.4.1 Extended-Ion Approximation.- 2.4.2 Semi-Empirical Methods.- 2.4.3 Hartree-Fock Cluster Methods.- 3 Condensed Rare Gases.- 3.1 Electronic Structure.- 3.2 Spectroscopy.- 3.2.1 Luminescence.- 3.2.2 Transient Absorption.- 3.2.3 Photoconversion Spectroscopy.- 3.2.4 Surface STE States.- 3.3 Theory of the Self-Trapped Exciton in Rare Gas Solids.- 3.3.1 Method Based on ab initio Ne*-Ne Potentials.- 3.3.2 Extended-Ion Approaches.- 3.3.3 Other Approaches.- 3.4 Desorption from the Surface.- 4 Alkaline Earth Fluorides.- 4.1 Electronic Structure.- 4.2 Lattice Defects.- 4.3 Theory of Self-Trapped Excitons in Fluorite Crystals.- 4.3.1 Extended-Ion Calculations for CaF2 and SrF2.- 4.3.2 Zero-Field Splitting of the Triplet STE.- 4.4 Spectroscopy.- 4.5 Lattice Defect Formation.- 5 Alkali Halides.- 5.1 Material Properties.- 5.2 Theory of Self-Trapped Exciton Structure.- 5.2.1 The STE as (Vk+e).- 5.2.2 Lattice Relaxation for the (Vk+e) Model.- 5.2.3 The Off-Center STE.- 5.2.4 ab initio Hartree-Fock Cluster Calculation of STE Structure.- 5.3 Luminescence.- 5.3.1 Survey of Luminescence Spectra.- 5.3.2 ?-Polarized Bands.- 5.3.3 Zero-Field Splitting and Triplet Sublevel Decay Kinetics.- 5.3.4 ?-Polarized Bands.- 5.3.5 Band Positions.- 5.3.6 Band Shape.- 5.3.7 Pressure and Dilatation Effects.- 5.3.8 Excitation Spectra.- 5.4 Magneto-Optics, ODMR, and ODENDOR.- 5.4.1 Magnetic Circular Polarization.- 5.4.2 Optically Detected Magnetic Resonance.- 5.4.3 Optically Detected Electron Nuclear Double Resonance.- 5.5 Excited-State Absorption.- 5.5.1 Characteristic Features and Binding Energies.- 5.5.2 Photoconversion and Polarization Analysis.- 5.6 Resonant Raman Scattering.- 5.7 Dynamics.- 5.7.1 Conversion of Excitons from Free to Self-Trapped States.- 5.7.2 Hole Self-Trapping Dynamics.- 5.7.3 STE Formation from Free Carriers and Relaxation from Excited States.- 5.7.4 Hot Luminescence of Self-Trapped Excitons.- 5.8 Kinetics.- 5.8.1 Quenching of STE Luminescence.- 5.8.2 Diffusion of Self-Trapped Excitons.- 6 Defect Formation in Alkali Halide Crystals.- 6.1 Self-Trapped Excitons as Nascent Defect Pairs.- 6.2 Thermally Activated Conversion.- 6.2.1 Primary Defect Formation versus Stabilization.- 6.2.2 Diffusion of the H Center from the STE.- 6.3 Dynamic Conversion Process.- 6.3.1 The Rabin-Kliek Diagram.- 6.3.2 Time-Resolved Studies.- 6.3.3 Dynamic Mechanisms.- 6.4 Stabilization of the Primary Defects.- 6.5 Defects and Desorption at Surfaces.- 6.5.1 Desorption Induced by Excitonic Processes.- 6.5.2 Atomic Force Microscopy.- 6.5.3 Defect Processes in Alkali Halide Clusters.- 7 Silicon Dioxide.- 7.1 Material Properties.- 7.1.1 Crystal Structure.- 7.1.2 Electronic Structure.- 7.2 Theory of Self-Trapped Excitons.- 7.2.1 Semiempirical (INDO) Approach.- 7.2.2 ab initio Approach.- 7.3 Experiments on Crystalline SiO2.- 7.3.1 Luminescence.- 7.3.2 Optically Detected Magnetic Resonance.- 7.3.3 Transient Absorption, Volume Change, and Photoconversion Spectroscopy.- 7.4 Experiments on Amorphous SiO2.- 7.5 Self-Trapped Holes in SiO2.- 7.6 Defect Generation Processes.- 8 Simple Organic Molecular Crystals.- 8.1 Material Properties.- 8.2 Pyrene.- 8.3 Anthracene.- 8.4 Perylene.- 9 Silver Halides.- 9.1 Electronic Structure and Exciton Spectra.- 9.2 Self-Trapped Hole in AgCl.- 9.2.1 Optical Transitions.- 9.2.2 The Self-Trapping Barrier and Hole Transport.- 9.3 Self-Trapped Exciton in AgCl.- 9.3.1 Optical Transitions.- 9.3.2 Optically Detected Magnetic Resonance.- 9.3.3 AgBr and the AgBr1?xClx Alloy System.- 10 As2Se3 and Other Chalcogenides.- 10.1 Structure and Electronic States of As2Se3.- 10.2 The Self-Trapped Exciton.- 10.3 Spectroscopy.- 10.4 STE to Defect Conversion in Amorphous Chalcogenides.- 10.5 Spectroscopy in Crystalline Trigonal Selenium.- 11 Other Materials, Extrinsic Self-Trapping, and Low-Dimensional Systems.- 11.1 Ammonium Halides.- 11.2 KMgF3 and Related Perovskites.- 11.3 Alkaline-Earth Fluorohalides.- 11.4 Alkali Silver Halides.- 11.5 LiYF4.- 11.6 Extrinsic Self-Trapping in ZnSe1?xTex.- 11.7 Quasi-One-Dimensional Systems.- References.

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