Electronic Processes on Semiconductor Surfaces during Chemisorption
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1 Electronic Processes on Semiconductor Surfaces during Chemisorption T. Wolkenstein Translatedfrom Russian by E. M. Yankovskii Translation edited in part by Roy Morrison CONSULTANTS BUREAU NEW YORK AND LONDON
2 CONTENTS CHAPTER 1. ELECTRONS AND HOLES IN A SEMICONDUCTOR Order and Disorder in Crystals Types of Defects Properties of Defects Electrical Conduction of Nonmetallic Crystals Factors Influencing Conduction Types of Electrical Conduction The Mechanism of n- and/?-type Conduction Free Electrons, Holes, and Excitons in a Lattice Energy Levels of Electrons and Holes The Energy Spectrum of an Electron in an Infinite Crystal Lattice Statement of the Problem Eigenfunctions and Eigenvalues A Three-Dimensional Lattice The Energy Spectrum of a Hole The Energy Spectrum of an Electron in a Finite Crystal Lattice, Statement of the Problem Eigenfunctions and Eigenvalues Tamm and Shockley Surface Levels Statistics of Electrons and Holes in Semiconductors The Fermi-Dirac Distribution Function n- and/7-type Semiconductors 25 ix
3 x Contents Statistics of Local States The Position of the Fermi Level Limits of the Band Theory of Semiconductors Characteristic Features of the Band Theory The Validity of the Band Theory The Valence Band 33 CHAPTER 2. THE VARIOUS TYPES OF ADSORPTION The Main Laws of Adsorption The Main Prerequisites for Langmuir's Theory The Kinetics of Adsorption Adsorption Equilibrium Physical and Chemical Adsorption The Difference between Physical and Chemical Adsorption Calculating the Adsorption Minimum Activated Adsorption The Nature of the Activation Barrier "Strong" and "Weak" Bonds in Chemisorption "Weak" and "Strong" Donor and "Strong" Acceptor Forms of Chemisorption The Various Forms of Chemisorption on Ionic Crystals Examples Radical and Valence-Saturated Forms of Chemisorption Free Valences of a Surface The Reactivity of Chemisorbed Particles Examples of Radical and Valence-Saturated Forms of Chemisorption The Dissociation of Molecules in Adsorption and the Recombination of Chemisorbed Atoms The One-Electron Bond in Chemisorption Statement of the Problem Eigenfunctions and Eigenvalues The Polarization of a Chemisorbed Atom The Two-Electron Bond in Chemisorption Statement of the Problem Eigenfunctions and Eigenvalues Free Lattice Electrons as Adsorption Centers Allowing for "Weak" Bonding Quantum-Mechanical Caiculations in Adsorption Theory The Cluster Approximation 79
4 Contents xi "Covalent" Clusters for Oxide Lattices "Ionic" Clusters for Oxide Lattices 81 CHAPTER 3. ELECTRON TRANSITIONS IN CHEMISORPTION Transitions between Various Forms of Chemisorption Transitions between Energy Levels Transitions between Adsorption Curves Equilibrium of Various Forms of Chemisorption The Notion of Electron Transitions in Chemisorption Theories Adsorption Equilibrium Adsorptivity of a Surface Surface Charging in Adsorption The Kinetics of Adsorption Statement of the Problem Adsorption at a Constant Surface Potential: The General Case Adsorption at a Constant Surface Potential: Particular Cases Adsorption with a Varying Surface Potential The Kinetics of Desorption Desorption with Electronic Equilibrium Violation of Electronic Equilibrium in Desorption Incomplete Desorption The Role of the Fermi Level in Chemisorption The Fermi Level as Regulator of the Chemisorptive Properties of a Surface The Origin of non-langmuiran Relations The Approximations of the "Boundary Layer Theory" 123 CHAPTER 4. THE INTERACTION OF THE SURFACE WITH THE BULK IN A SEMICONDUCTOR The Connection between Surface and Bulk Properties of a Semiconductor The Connection between the Position of the Fermi Levels at the Surface and in the Bulk of a Semiconductor The Surface Potential 127
5 xii Contents The Dependence of the Surface Potential on Various Factors Effects due to the Charging of the Surface Effect of Adsorption on Work Function Surface Conduction Effect of External Field and Adsorption on Conduction The "Quasiisolated" Surface The Notion of a "Quasiisolated" Surface Some Properties of "Quasiisolated" Surfaces The Continuous and Quasicontinuous Spectra of Surface States Adsorptive Properties of a Charged Semiconductor The Adsorptivity of a Charged Semiconductor The Electroadsorptive Effect Adsorption of Ions on a Semiconductor The Influence of the Surface on the Impurity Distribution inside a Semiconductor Statement of the Problem Impurity Distribution in the Surface Layer of Semiconductors Effect of Impurity on the Adsorptivity of Semiconductors Irreversible Adsorption The Adsorptivity of Semiconductor Films on Metals The Variation of the Potential in the Film The Adsorptivity of the Film for a Positively Charged Surface The Adsorptivity of the Film for a Negatively Charged Surface Growth of a Semiconductor Film on a Metal Statement of the Problem The Electric Field in the Film The Logarithmic Law of Film Growth The Parabolic and Linear Laws of Film Growth Succession of Laws of Film Growth with Temperature and Pressure Variation 195 CHAPTER 5. THE CATALYTIC EFFECT OF A SEMICONDUCTOR The Basics Semiconductors as Catalysts of Chemical Reactions 199
6 Contents xiii The Activity and Selectivity of a Catalyst The Activation Energy The Electronic Theory of Catalysis The Role of the Permi Level in Catalysis Radical Mechanisms of Heterogeneous Reactions Acceptor and Donor Reactions Electronic Mechanisms of Catalytic Reactions Oxidation of Hydrogen Decomposition of Alcohol Oxidation of Carbon Monoxide Hydrogen-Deuterium Exchange The Relationship between the Catalytic Activity of a Semiconductor and Its Electronic Properties The Origin of the Relationship between Catalytic Activity, Work Function, and Electrical Conductivity Experimental Results Variations in Electrical Conductivity and Work Function in the Course of a Reaction Correlation between Catalytic Activity and the Forbidden Gap Width in the Energy Spectrum of a Semiconductor The Effect of Various Factors on Catalytic Activity The Effect of an External Electric Field Catalytic Properties of a Semiconductor Film on a Metal The Mechanism of the Action of an Impurity The Experimental Data on the Effect of Impurities The Compensation Effect 255 CHAPTER 6. PROCESSES ON A REAL SURFACE Deviations from Langmuir's Theory on a Real Surface The Concept of an Inhomogeneous Surface The Concept of Interaction The Adsorption-Heat Distribution Function Inhomogeneity due to Irregularities in the Impurity Distribution The Relation between the Impurity Concentration Gradient and the Adsorption-Heat Distribution Function Examples of Inhomogeneous Surfaces The Role of Surface Structural Defects in Adsorption Adsorption on a Structural Defect Adsorption on Defects of Thermal Origin 278
7 xiv Contents Adsoiption on the Surface of a Disordered Semiconductor Adsorption on Dispersed Semiconductors Adsorptive Properties ofa Dispersed Semiconductor The Compensation Effect on Dispersed Semiconductors Controlling the Stoichiometry of Crystals Theoretical Aspects of the Problem Experimental Results 291 CHAPTER 7. THE EFFECT OF ILLUMINATION ON THE ADSORPTIVE AND CATALYTIC PROPERTIES OF A SEMICONDUCTOR The Photoadsorption Effect Positive and Negative Photoadsorption Effects The Photoadsorption Effect on Ideal and Real Surfaces Review of Basic Experimental Data The Photoadsorption Effect at an Ideal Surface The Effect of Illumination on the Amount of Various Forms of Chemisorption Allowing for the Annihilation of Excitons at Chemisorbed Particles The Mechanism of the Influence of Illumination on the Adsorptivity of a Surface The Magnitude of the Photoadsorption Effect The Sign and Absolute Value of the Photoadsorption Effect at an Ideal Surface Statement of the Problem Solution for a Simplified Potential Function The Case of the Excitonic Mechanism of Light Absorption A Graphic Representation of the Results The Case of High Excitation Adsorption Centers in Photoadsorption The Nature of Adsorption Centers The Concentration of Adsorption Centers Variation of Adsorption Center Concentration under Illumination The Photoadsorption Effect at a Real Surface Adsorption after Illumination The Sign and Magnitude of the Photoadsorption Effect "Direct" Photodesorption The Aftereffect 338
8 Contents xv 7.6. Comparison of the Theory of the Photoadsorption Effect with the Experimental Data Influence of Illumination on the Adsorptivity of a Surface "Memory" Effects in Photoadsorption Some Theoretical Predictions The Photocatalytic Effect The Mechanism of the Photocatalytic Effect Hydrogen-Deuterium Exchange Oxidation of Carbon Monoxide: The Experimental Data and the Reaction Mechanism Oxidation of CO: Comparison of Theoretical Results with Experimental Data Synthesis of Hydrogen Peroxide: The Experimental Data and the Reaction Mechanism Synthesis of Hydrogen Peroxide: Comparison of Theoretical Results with Experimental Data 365 CHAPTER 8. ADSORPTION AND LUMINESCENCE Basic Facts on Luminescence of Crystals The Various Types of Luminescence Luminescence Centers Traps and Quenching Centers The Effect of Adsorption on Luminescence The Various Mechanisms of Influence of Adsorption on Photoluminescence Recombination Luminescence: Statement of the Problem Recombination Luminescence: Limiting Cases Recombination Luminescence: Experimental Data Excitonic Luminescence: Statement of the Problem Excitonic Luminescence: A Discussion The Basic Laws of Radical-Recombination Luminescence The Spectral Composition of Radical-Recombination Luminescence Emission The Effect of Temperature on Intensity of RRL Spectra The Effect of Electric Field on Intensity of RRL Spectra The Effect of Illumination on RRL Intensity The Mechanism of Radical-Recombination Luminescence The Excitation Mechanism The Mechanism of Luminescence 398
9 xvi Contents The Dependence of RRL Intensity on the Position of the Fermi Level The Dependence of RRL Intensity on an External Electric Field The Temperature Dependence of RRL Intensity Radical Photoluminescence Adsorption Luminescence The Fundamentals of Adsorption Luminescence The Mechanism and Kinetics of Adsorption Luminescence Adsorption Luminescence at Adsorption Equilibrium Adsorption Luminescence and the Adsorption Emission of Electrons Luminescence Emission Accompanying Catalytic Reactions at Surfaces 417 CHAPTER 9. CONCLUSION The "Local" and "Collective" Effects in Chemisorption and Catalysis The Basic Concepts of the Electronic Theory of Chemisorption The Electronic Theory of Chemisorption and Experiment 425 REFERENCES 427
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