THE CHEMICAL PHYSICS OF SOLID SURFACES
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1 THE CHEMICAL PHYSICS OF SOLID SURFACES EDITED BY D.A.KING B.Sc, Ph.D. (Rand), Sc.D. (East Anglia), F.R.S Professor of Physical Chemistry, University of Cambridge AND D.P.WOODRUFF B.Sc. (Bristol), Ph.D., D.Sc. (Warwick) Professor ofphysics, University of Warwick VOLUME 7 PHASE TRANSITIONS AND ADSORBATE RESTRUCTURING AT METAL SU RFACES ELSEVIER AMSTERDAM - LONDON - NEW YORK - TOKYO 1994
2 IX Contents Preface Chapter 1 (P. Bak and M. Paczuski) Principles of phase transitions in two-dimensional Systems 1. Introduction 1 2. Surface reconstructions Au and Pt (2x1) reconstmction: die mystery of the missing row The W{ 100} (V2 x V2) reconstmction 9 3. Commensurate-incommensurate transitions More complicated CI transitions: hexagonal incommensurate structures Surface roughening Roughening and the missing row reconstmction 29 References 32 Chapter 2 (J. Jupille and D.A. King) Instabilities and adsorbate restructuring at W{100} 1. Introduction Clean (V2 x V2)R45 ->(lxl) reconstmction Structural parameters Low-temperature phase The multilayer reconstmction High-temperature phase The roleof Steps Dynamics The high frequency mode The soft phonon mode The fractional-order beam The nature of the transition The order-disorder character The displacive character Microscopic mechanism Hydrogen-induced reconstmction The low-coverage limit Changes in critical temperature The symmetry switching 56
3 X 3.2 The phase diagram The c(2x2)-h layer The commensurate-incommensurate transition The streaked phase Reconstruction and reactivity The W{ 100} p(lxl)-h short bridge site The 118 mevline The nonadiabatically damped mode Conclusion 67 Acknowledgements 68 References 69 Chapter 3 (J.C. Campuzano) The Au{110} (1x2) <=> (lxl) phase transition 1. Introduction The surface structure of Au{ 110} Fundamentals of phase transitions Universality classes Conformal invariance Detecting surface phase transitions Universal transitions The roughening transition The Au{ 110} transitions Introduction Phase diagram of the {110} surface Ising lineshapes The Ising transition Conformal invariance in the Ising model The roughening transition lineshapes The Auf 110} roughening transition References 111 Chapter 4 (M. den Nijs) Roughening, preroughening, and reconstruction transitions in crystal surfaces 1. Introduction Surface reconstruction Topology of domain wall excitations Cell spin modeis Domain wall entropy Chirality Reconstructed phases with partial disorder 133
4 XI 8. Fractals and conformal invariance Surface roughening Roughening induced reconstruction Preroughening transitions DOF phase and particle-hole symmetry 157 Acknowledgements 159 References 160 Chapter 5 (A.G. Naumovets) Two-dimensional phase transitions in alkali-metal adlayers 1. Introduction Interactions in alkali-metal adlayers Models of AM bonding on surfaces Lateral interactions Conditions of equilibrium Atomic structure of alkali-metal adlayers Rarefied disordered phases Commensurate phases Smooth Substrates Rough Substrates Furrowed Substrates Incommensurate solid phases Phase transitions and phase diagrams Transitions in fluid (disordered) phases Phase transitions in and between commensurate structures Transitions on varying coverage Thermal disordering of C-phases Commensurate-to-incommensurate (C-I) phase transitions Phase transitions in incommensurate structures Melting transitions Rotational transitions Effect of the phase transitions in AM overlayers on physicochemical properties of covered surfaces Work function and other electron properties Binding energy, catalytic activity Surface diffusion Conclusion 206 Acknowledgements 206 References 207
5 Xll Chapter 6 (M.C. Tringides) Growth kinetics in two-dimensional phase transitions 1. Introduction Non-equilibrium processes Searching for growth laws in non-equilibrium processes Theoretical background Ordering growth laws What parameters control ordering growth laws? Growth exponents: conserved vs. non-conserved order parameter The role of disorder Scaling of the non-equilibrium structure factor Theoretical techniques to measure non-equilibrium growth laws Disordering process Chemical potential quenches in non-equilibrium processes Diffusion measurements in growth kinetics Experimental Preliminary experimental considerations Techniques for studying growth kinetics general Comparision of diffraction techniques Measures of the growth Other techniques: Ion scattering, STM, LEEM, atom probe Experimental results T-9 plane: Single phase region, non-conserved order parameter T-0 plane: Growth kinetics in the two-phase region T-9 plane: Growth kinetics studies with X-rays T-9 plane: Growth of the average domain size vs coverage T-9 plane: Growth kinetics in Systems wih disorder T-9 plane: The decay of order Why is there Saturation in growth kinetics at long times? i-9 plane: Ordering experiments Growm kinetics results obtained with other techniques (ion scattering, STM, LEEM, atom probe) Conclusions future problems 252 Acknowledgements 254 References 254
6 Xlll Chapter 7 (J.W.M. Frenken and H.M. van Pinxteren) Surface melting: an experimental overview 1. Introduction Historical background General concepts Macroscopic observations Heatcapacity Optical behaviour Microscopic observations Short-range Order Long-range Order Density profile Surface mobility Related surface behaviour Incomplete surface melting Surface-melting induced faceting Surface non-melting and bulk superheating Conclusion 285 Acknowledgements 286 References 287 Chapter 8 (K. Kern) Thermal roughening of surfaces: experimental aspects 1. Introduction: thermal restructuring at surfaces Equilibrium crystal shape (ECS) and surface roughening The surface free energy and the ECS The step free energy and the roughening transition in the ECS Detection of Steps at surfaces Surface microscopy Surface diffraction Diffraction peak width and height Diffraction line shapes Roughening of nonvicinal surfaces Nonreconstructed fcc {110}surfaces The precursors to surface roughening: vibrational disordering and adatom-vacancy creation Thermal roughening of fcc {110} (lxl) surfaces Missing row-reconstructed fcc {110} (1x2) surfaces: deconstruction versus roughening The close packed fcc {100} and (111) surfaces 325
7 XIV 5. Roughening of vicinal surfaces The kink free energy and Step roughening The Step roughening transition of fcc {lln} surfaces Consequences of surface roughening on crystal growth Thin film epitaxy Crystal growth and ECS 335 References 337 Chapter 9 (A.C. Levi) Roughening, wetting and surface melting: theoretical considerations 1. Introduction Roughening Wetting Surface melting 369 Acknowledgements 383 References Appendix: renormalization group analysis 393 Chapter 10 (R.M. Lynden-Bell) Computer Simulation of atomic dynamics on metal surfaces 1. Introduction Simulation methods Potentials for simulations of metals Insights into surface structure Limitations of many body potentials Simulations of flat surfaces Faceting of stepped surfaces Adatom diffusion on surfaces Diffusion on stepped surfaces Interacting surfaces Interaction of two flat surfaces Fracture of bridges and perfect crystals Simulations of tip-flat interactions Conclusions 440 References 441 Chapter 11 (L.D. Marks and N. Doraiswamy) Structural fluctuations in small particles 1. Introduction Background Experimental evidence for structural fluctuations 449
8 XV 3. Theoretical modeis Kinetics Discussion Acknowledgements References 460 Chapter 12 (D.P. Woodruff) Adsorbate-induced restructuring of f.c.c. {100} surfaces 1. Introduction Adsorbate-induced distortions in 'simple' adsorption structures Adsorbate-induced parallel distortions; p4g Space group 'clock' reconstructions Large mass transport reconstructions; missing rows Wider stability of some {100} adsorption structures? 493 References 495 Chapter 13 (CJ. Barnes) Adsorbate induced reconstruction of f.c.c.{110} surfaces 1. Introduction Alkali metal induced surface reconstruction Phenomenological observations Geometrie strueture of the reconstrueted (1x2) phase Driving force behind the (lxl) >(lx2) transition Mechanism of coverage-dependent structural transitions Alkali induced reconstructions of Au{110} Reconstruction of f.c.c. {110} bimetallic surfaces Hydrogen induced surface reconstructions Hydrogen induced paired and missing row reconstructions of NiandPd{110} The hydrogen induced missing row reconstruction of Cu{110} Weak reconstruetive adsorption of hydrogen on Rh{ 110} Surface reconstruction induced by oxygen, nitrogen, carbon and sulphur Oxygen-induced added row reconstructions Nitrogen induced (2x3) surface reconstruction: the (2x3) strueture on Cu{ 110} Surface reconstruction induced by sulphur and carbon Molecularly-induced reconstruction The CO-induced "missing-row" reconstruction of Pd{110} Conclusions 561 Acknowledgements 562
9 XVI References 562 Chapter 14 (F. Besenbacher and I. Stensgaard) Microscopic studies of adsorbate restructuring at metal surfaces 1. Introduction STM imaging Adsorbate-mediated reconstructive transformations O-induced 'added-row' growth mode on Cu{110} The high-coverage c(6x2)0 phase on Cu {110} O-induced 'added-row' growth on Ni{110} O-induced 'missing-row' reconstruction of Cu{100} Alkali-induced missing-row reconstructions Growth of the 'streaky' (lx2)h phase on Ni{110} Adsorption-induced lifting of reconstructions on Pt surfaces Adsorption of S on Nif 110): new phases and atom-resolved surface reactions The p(4xl)s reconstruction of Ni{110} Reaction between S and preadsorbed O on Ni{ 110} Complex structures with large unit cells A displacive reconstruction: C on Ni{ 100} General trends Effective-medium theory Oxygen-induced reconstructions Hydrogen- and alkali-induced reconstructions of Nif 110} and Cu{110} Sulphur-induced reconstructions on Ni{ 110} Growth mode of the adsorbate-induced reconstructions Summary Acknowledgements 621 References 622 Index 631
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