First Principles Approaches To Spectroscopic Properties Of Complex Materials

The series Topics in Current Chemistry presents critical reviews of the present and future trends in modern chemical research. The scope of coverage is all areas of chemical science including the interfaces with related disciplines such as biology, medicine and materials science. The goal of each thematic volume is to give the non-specialist reader, whether in academia or industry, a comprehensive insight into an area where new research is emerging which is of interest to a larger scientific audience. Each review within the volume critically surveys one aspect of that topic and places it within the context of the volume as a whole. The most significant developments of the last 5 to 10 years are presented using selected examples to illustrate the principles discussed. The coverage is not intended to be an exhaustive summary of the field or include large quantities of data, but should rather be conceptual, concentrating on the methodological thinking that will allow the non-specialist reader to understand the information presented. Contributions also offer an outlook on potential future developments in the field. Review articles for the individual volumes are invited by the volume editors. Readership: research chemists at universities or in industry, graduate students.

This book studies the dynamics of fundamental collective excitations in quantum materials, focusing on the use of state-of-the-art ultrafast broadband optical spectroscopy. Collective behaviour in solids lies at the origin of several cooperative phenomena that can lead to profound transformations, instabilities and phase transitions. Revealing the dynamics of collective excitations is a topic of pivotal importance in contemporary condensed matter physics, as it provides information on the strength and spatial distribution of interactions and correlation. The experimental framework explored in this book relies on setting a material out-of-equilibrium by an ultrashort laser pulse and monitoring the photo-induced changes in its optical properties over a broad spectral region in the visible or deep-ultraviolet. Collective excitations (e.g. plasmons, excitons, phonons...) emerge either in the frequency domain as spectral features across the probed range, or in the time domain as coherent modes triggered by the pump pulse. Mapping the temporal evolution of these collective excitations provides access to the hierarchy of low-energy phenomena occurring in the solid during its path towards thermodynamic equilibrium. This methodology is used to investigate a number of strongly interacting and correlated materials with an increasing degree of internal complexity beyond conventional band theory.

​​This is the first book that provides a detailed summary of one of the most successful new condensed matter theories - dynamical mean-field theory (DMFT) - in both static and dynamical cases of systems of different sizes. DMFT is one of the most successful approaches to describe the physical properties of systems with strong electron-electron correlations such as bulk materials, multi-layers, surfaces, 2D materials and nanostructures in both metallic and insulating phases. Strongly correlated materials usually include partially-filled localized d- or f-orbitals, and DMFT takes into account crucial for these systems time-resolved interaction between electrons when they “meet” on one atom and occupy one of these orbitals. The First Part of the book covers the general formalism of DMFT as a many-body theory, followed by generalizations of the approach on the cases of finite systems and out-of-equilibrium regime. In the last Chapter of the First Part we discuss generalizations of the approach on the case when the non-local interactions are taken into account. The Second Part of the book covers methodologies of merging DMFT with ab initio static Density Functional Theory (DFT) and Time-Dependent DFT (TDDFT) approaches. Such combined DFT+DMFT and DMFT+TDDFT computational techniques allow one to include the effects of strong electron-electron correlations at the accurate ab initio level. These tools can be applied to complex multi-atom multi-orbital systems currently not accessible to DMFT. The book helps broad audiences of students and researchers from the theoretical and computational communities of condensed matter physics, material science, and chemistry to become familiar with this state-of-art approach and to use it for reaching a deeper understanding of the properties of strongly correlated systems and for synthesis of new technologically-important materials.

The many-body-theoretical basis and applications of theoretical spectroscopy of condensed matter, e.g. crystals, nanosystems, and molecules are unified in one advanced text for readers from graduate students to active researchers in the field. The theory is developed from first principles including fully the electron-electron interaction and spin interactions. It is based on the many-body perturbation theory, a quantum-field-theoretical description, and Green's functions. The important expressions for ground states as well as electronic single-particle and pair excitations are explained. Based on single-particle and two-particle Green's functions, the Dyson and Bethe-Salpeter equations are derived. They are applied to calculate spectral and response functions. Important spectra are those which can be measured using photoemission/inverse photoemission, optical spectroscopy, and electron energy loss/inelastic X-ray spectroscopy. Important approximations are derived and discussed in the light of selected computational and experimental results. Some numerical implementations available in well-known computer codes are critically discussed. The book is divided into four parts: (i) In the first part the many-electron systems are described in the framework of the quantum-field theory. The electron spin and the spin-orbit interaction are taken into account. Sum rules are derived. (ii) The second part is mainly related to the ground state of electronic systems. The total energy is treated within the density functional theory. The most important approximations for exchange and correlation are delighted. (iii) The third part is essentially devoted to the description of charged electronic excitations such as electrons and holes. Central approximations as Hedin's GW and the T-matrix approximation are discussed.(iv) The fourth part is focused on response functions measured in optical and loss spectroscopies and neutral pair or collective excitations.

Spectroscopic Methods in Mineralogy and Material Science covers significant advances in the technological aspects and applications of spectroscopic and microscopic techniques used in the Earth and Materials Sciences. The current volume compliments the now classic Volume 18, Spectroscopic Methods in Mineralogy and Geology, which became an essential resource to many scientists and educators for the past two decades. This volume updates techniques covered in Volume 18, and introduces new techniques available for probing the secrets of Earth materials, such as X-ray Raman and Brillouin spectroscopy. Other important topics including Transmission Electron Microscopy (TEM) and Atomic Force Microscopy (AFM) are also covered.

The first reference of its kind in the rapidly emerging field of computational approachs to materials research, this is a compendium of perspective-providing and topical articles written to inform students and non-specialists of the current status and capabilities of modelling and simulation. From the standpoint of methodology, the development follows a multiscale approach with emphasis on electronic-structure, atomistic, and mesoscale methods, as well as mathematical analysis and rate processes. Basic models are treated across traditional disciplines, not only in the discussion of methods but also in chapters on crystal defects, microstructure, fluids, polymers and soft matter. Written by authors who are actively participating in the current development, this collection of 150 articles has the breadth and depth to be a major contributor toward defining the field of computational materials. In addition, there are 40 commentaries by highly respected researchers, presenting various views that should interest the future generations of the community. Subject Editors: Martin Bazant, MIT; Bruce Boghosian, Tufts University; Richard Catlow, Royal Institution; Long-Qing Chen, Pennsylvania State University; William Curtin, Brown University; Tomas Diaz de la Rubia, Lawrence Livermore National Laboratory; Nicolas Hadjiconstantinou, MIT; Mark F. Horstemeyer, Mississippi State University; Efthimios Kaxiras, Harvard University; L. Mahadevan, Harvard University; Dimitrios Maroudas, University of Massachusetts; Nicola Marzari, MIT; Horia Metiu, University of California Santa Barbara; Gregory C. Rutledge, MIT; David J. Srolovitz, Princeton University; Bernhardt L. Trout, MIT; Dieter Wolf, Argonne National Laboratory.

This book reviews various aspects of molecular spectroscopy and its application in materials science, chemistry, physics, medicine, the arts and the earth sciences. Written by an international group of recognized experts, it examines how complementary applications of diverse spectroscopic methods can be used to study the structure and properties of different materials. The chapters cover the whole spectrum of topics related to theoretical and computational methods, as well as the practical application of spectroscopic techniques to study the structure and dynamics of molecular systems, solid-state crystalline and amorphous materials, surfaces and interfaces, and biological systems. As such, the book offers an invaluable resource for all researchers and postgraduate students interested in the latest developments in the theory, experimentation, measurement and application of various advanced spectroscopic methods for the study of materials.

This book describes the state-of-the-art research topics in theoretical materials science. It encompasses the computational methods and techniques which can advance more realistic calculations for understanding the physical principles in new growth methods of optoelectronic materials and related surface problems. These principles also govern the photonic, electronic, and structural properties of materials which are essential for device applications. They will also provide the crucial ingredients for the growth of future novel materials. Contents:Advances in Algorithmic Development in the Electronic Structure of Large Systems (E B Stechel)Plane Wave Pseudopotential Electronic Structure Calculations on Parallel Supercomputers (J S Nelson & S J Plimpton)First-Principles Theory of Electron Excitation Energies in Solids, Surfaces, and Defects (S G Louie)Photonic Band Structure (R Biswas et al.)Tight-Binding Parametrization of First-Principles Results (M J Mehl & D A Papaconstantopoulos)First Principles Studies of Stability of Intermetallic Binary Alloys (Z W Lu & B M Klein)Simulation of Semiconductor Growth Mechanisms in the Presence of Adsorbate Layers (E Kaxiras)Bond Saturation Model: A Lattice Gas Approach for Studying Close Packed Metallic Surfaces (M C Fallis & C Y Fong) Readership: Materials scientists. keywords:Linear Scaling;Density Matrix Algorithm;Quasi-Particle Excitations;Self-Energy;GW Approximation;Density Functional Theory – Based Slater Koster Tight-Binding Parametrization;Intermetallic Binary Alloys;Short-Range Order;Alloy Stability;Semiconductor Growth;Activation Energy;Kinetic Monte Carlo Simulations;Lattice Gas Approach;Metallic Surfaces;Bond Saturation Model;Cluster Energetics;Embedded Atom Method