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This two-volume work covers ultrafast structural and electronic dynamics of elementary processes at solid surfaces and interfaces, presenting the current status of photoinduced processes. Providing valuable introductory information for newcomers to this booming field of research, it investigates concepts and experiments, femtosecond and attosecond time-resolved methods, as well as frequency domain techniques.
The whole is rounded off by a look at future developments.
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Seitenzahl: 496
Veröffentlichungsjahr: 2012
Contents
Cover
Related Titles
Title Page
Copyright
Preface
List of Contributors
Chapter 1: The Electronic Structure of Solids
1.1 Single-Electron Approximation
1.2 From Bloch Theory to Band Structure Calculations
1.3 Beyond the Band Picture
1.4 Electronic Structure of Correlated Materials
References
Chapter 2: Quasi-Particles and Collective Excitations
2.1 Introduction
2.2 Quasi-Particles
2.3 Collective Excitations
2.4 Experimental Access to Quasi-Particle and Collective Excitations
2.5 Summary
References
Chapter 3: Surface States and Adsorbate-Induced Electronic Structure
3.1 Intrinsic Surface States
3.2 Crystal-Induced Surface States
3.3 Barrier-Induced Surface States
3.4 Experimental Methods
3.5 Adsorbate-Induced Electronic Structure
References
Chapter 4: Basic Theory of Heterogeneous Electron Transfer
4.1 Resonant Charge Transfer in Chemisorbed Systems
4.2 Electron Transfer in the Presence of Polar/Polarizable Media
4.3 Transient Electronic Coupling: Crossover between Limiting Cases
4.4 Conclusions
References
Chapter 5: Electromagnetic Interactions with Solids
5.1 Dielectric Function of Metals
5.2 Band Mapping of Solids by Photoemission Spectroscopy
5.3 Optical Excitations in Metals
5.4 Plasmonic Excitations at Surfaces and Nanostructures
References
Colour Plates
Index
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© 2012 Wiley-VCH Verlag & Co. KGaA, Boschstr. 12, 69469 Weinheim, Germany
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Composition Thomson Digital, Noida, India
Cover Design Adam Design, Weinheim
Print ISBN: 978-3-527-40924-2
ePDF ISBN: 978-3-527-64649-4
oBook ISBN: 978-3-527-64646-3
ePub ISBN: 978-3-527-64648-7
Preface
The dynamics of elementary processes in solids are decisive for various physical properties of solid state materials and their application in devices. This book intends to provide an introductory and comprehensive overview of the fundamental concepts, techniques and underlying elementary processes in the field of ultrafast dynamics of solid state surfaces and interfaces. While the first volume addresses recent research on quasiparticle dynamics, collective excitations, electron transfer and photoinduced dynamics, the focus of this second volume lies on fundamentals and provides introductory information on elementary processes and light-matter interaction. Our goal is to make these concepts accessible also to non-experts and, in particular, to newcomers and younger researchers in the field of ultrafast dynamics of solids, their interfaces and nanostructured materials. We hope that both volumes will help to further new research directions and developments in this field.
We acknowledge support from our funding agencies, important contributions from our co-workers, stimulating discussions with colleagues and the understanding from our families that were essential to realize this book.
Duisburg, Pittsburgh and Berlin, January 2012
Uwe Bovensiepen,Hrvoje Petek,Martin Wolf
List of Contributors
Silke BiermannÉcole PolytechniqueCentre de Physique Theorique91128 Palaiseau CedexFrance
Uwe BovensiepenUniversität Duisburg-EssenFakultät für PhysikLotharstr. 147048 DuisburgGermany
Pawel BuczekMax-Planck-Institut fürMikrostrukturphysikWeinberg 206120 HalleGermany
Evgueni V. ChulkovDonostia International Physics Center(DIPC)Paseo de Manuel Lardizabal 420018 San Sebastián/DonostiaBasque CountrySpain
and
Centro de Física de Materiales (CFM)Departamento de Física de MaterialesPaseo de Manuel Lardizabal 420018 San Sebastian/DonostiaBasque CountrySpain
Thomas FausterUniversität Erlangen-NürnbergLehrstuhl für FestkörperphysikStaudtstr. 791058 ErlangenGermany
Kunie IshiokaUniversity of TsukubaNational Institute for Materials ScienceGraduate School of Pure and AppliedSciencesAdvanced Nano Characterization Center1-2-1 SengenTsukuba 305-0047Japan
Mackillo KiraPhilipps-UniversitätFachbereich PhysikRenthof 535032 MarburgGermany
Stephan W. KochPhilipps-UniversitätFachbereich PhysikRenthof 535032 MarburgGermany
Eugen E. KrasovskiiUniversität KielInstitut für Theoretische Physik undAstrophysikLeibnizstraße 1524098 KielGermany
Christoph LienauCarl von Ossietzky UniversitätInstitut für Physik26129 OldenburgGermany
Ricardo Díez MuiñoDonostia International Physics Center (DIPC)Paseo de Manuel Lardizabal 420018 San Sebastián/DonostiaSpain
Luca PerfettiÉcole Polytechnique91128 Palaiseau CedexFrance
Hrvoje PetekUniversity of PittsburghPhysics and Astronomy Department100 Allen Hall3941 O'Hara StreetPittsburgh, PA 15260USA
Jose M. PitarkeEuskal Herriko UnibertsitateaMateria Kondentsatuaren Fisika SailaZientzi Fakultatea644 Posta kutxatila48080 BilboBasque CountrySpain
Daniel Sánchez-PortalDonostia International Physics Centre(DIPC)Paseo Manuel Lardizábal 420018 San SebastiánSpain
and
Dep. Física de Materiales (UPV/EHU)Facultad de QuímicaApartado 107220080 San SebastiánSpain
Leonid M. SandratskiiMax-Planck-Institut für MikrostrukturphysikWeinberg 206120 HalleGermany
Jörg SchäferUniversität WürzburgPhysikalisches InstitutAm Hubland97074 WürzburgGermany
Wolfgang SchattkeUniversität KielInstitut für Theoretische Physik und AstrophysikLeibnizstraße 1524098 KielGermany
Irina SklyadnevaDonostia International Physics Center(DIPC)Paseo de Manuel Lardizabal 420018 San Sebastián/DonostiaBasque CountrySpain
and
Tomsk State Universitypr. Lenina 36634050 TomskRussian Federation
Julia StählerFritz-Haber-Institut der Max-Planck-GesellschaftAbteilung für Physikalische ChemieFaradayweg 4-614195 BerlinGermany
Martin WeineltFreie Universität BerlinFachbereich PhysikArnimallee 1414195 BerlinGermany
Martin WolfFritz-Haber-Institut der Max-Planck-GesellschaftAbteilung für Physikalische ChemieFaradayweg 4-614195 BerlinGermany
Xiaoyang ZhuUniversity of Texas at AustinDepartment of Chemistry &Biochemistry1 University Station A5300 Austin, TX 78712USA
Chapter 1
The Electronic Structure of Solids
Uwe Bovensiepen, Silke Biermann, and Luca Perfetti,
The discussion of dynamics at interfaces is based on the motion of ion cores and electronic excitations that are mostly optically driven. Hence, the electronic structure is of fundamental importance here. In solids such as molecular or ionic crystals, the valence electron distribution is not considerably distorted from the respective isolated atoms, ions, or molecules. Hence, their cohesion is entirely given by the classical potential energy of negligibly deformed electron distributions of bare particles, and van der Waals or Coulomb interactions are responsible for the formation of solid materials. This ceases to be so in metals and covalent crystals because the valence electron distribution plays the decisive role in bonding the constituents to a solid. In turn, the valence electron distribution can be considerably modified from the isolated atom or ion. A general description of solids must, therefore, consider the electronic structure in the first place. Furthermore, the dynamical processes discussed in this book are mostly optically excited or electron mediated.
This chapter introduces the basic concepts widely used in the description of the electronic structure in solid materials. In Section 1.1, we present the description of the nearly free electron approximation that is motivated by optical excitations of a solid following the Drude model. We introduce the Fermi sphere and the dispersion of electronic bands in momentum space. In Section 1.2, the influence of the periodic potential in a crystal is considered, which leads to the description of the electronic band structure by Bloch's theory for delocalized states. There is a considerable variety of materials that is not described by band theory, which originates from electron–electron interaction. In Section 1.3, we introduce Mott insulators that manifest deviations from the band picture. In Section 1.4, we introduce established concepts to describe the electronic structure of materials with strong electron correlations and give examples.
Although a solid contains about 1023 electrons/cm3, for a number of materials (but not for all) it is sufficient to neglect the explicit interaction among these particles. In this one-electron approximation, the energy of individual electrons is renormalized to account for the electron–electron interaction, which simplifies the description enormously. These electrons in the material are then termed quasi-particles.
We start by considering propagation of electrons in a metal. Such dynamical processes have been essential for Drude's theory of electrical conductivity in metals [1] and will be discussed in detail in Chapter 5. Here, we introduce the concept briefly in order to motivate the description of the electronic structure in solids.
Drude applied the kinetic theory of gases to a metal that is represented by a gas of electrons occupying the interstitial region between the ion cores. Without an electric field E, the current density averages to zero because the electrons have no preferential direction to move at velocity v in between two collisions with scattering centers (which Drude imagined to be the ion cores); here, represents the electron density and the elementary charge. In the presence of an electric field, a net current density develops because during the time interval between two collisions the electron is accelerated in a preferential direction to . The electrical DC conductivity is hence proportional to the time between two scattering events.
(1.1)
Here, is the electron mass. To estimate the order of magnitude of , the measured DC conductivity is taken, for example, for Cu at a temperature K and one finds s or 210 fs being well in the femtosecond regime.
If the electric field is time dependent, the result can be generalized for a frequency to
(1.2)
Using the wave equation for the electric field , the complex dielectric function is introduced.
(1.3)
With being the plasma frequency, the dielectric constant according to Drude's theory reads after linearization in
(1.4)
Considering the reflectivity with and , an electromagnetic wave cannot penetrate into the bulk of a metal for because it is reflected. For large frequencies , it does propagate in a metal. The absorption is proportional to the scattering rate and . The latter is usually referred to as the free carrier response, which will become clear further below. Please note that Drude's considerations are very fundamental throughout this book and will be used with emphasis on different aspects in Chapter 5.
The absorption is determined by and can be deduced from a measurement of the reflectivity using, for example, the Kramers–Kronig relations. Figure 1.1 shows the experimental results for alkali metals. At low frequency, the pronounced increase in absorption according to the free carrier response () is readily visible. At higher frequency, the behavior exhibits particular signatures that are characteristic for the respective material. For an understanding of the absorption spectrum in the visible and the ultraviolet spectral range, we consider next the electronic structure in the single (or independent) electron approximation.
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