Light-Matter Response in Nonrelativistic Quantum Electrodynamics.
TL;DR: The presented framework leads to a shift in paradigm by highlighting how electronically excited states arise as a modification of the photon field and that experimentally observed effects are always due to a complex interplay between light and matter.
Abstract: We derive the full linear-response theory for nonrelativistic quantum electrodynamics in the long wavelength limit and provide a practical framework to solve the resulting equations by using quantu...
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TL;DR: In this article, the authors present a detailed account of the physics of the relativistic Lorentz model of a charged particle coupled to its own electromagnetic field, which is the basis for our work.
Abstract: The motion of a charged particle interacting with its own electromagnetic field is an area of research that has a long history; this problem has never ceased to fascinate its investigators. On the one hand the theory ought to be straightforward to formulate: one has Maxwell's equations that tell the field how to behave (given the motion of the particle), and one has the Lorentz-force law that tells the particle how to move (given the field). On the other hand the theory is fundamentally ambiguous because of the field singularities that necessarily come with a point particle. While each separate sub-problem can easily be solved, to couple the field to the particle in a self-consistent treatment turns out to be tricky. I believe it is this dilemma (the theory is straightforward but tricky) that has been the main source of the endless fascination. For readers of Classical and Quantum Gravity, the fascination does not end there. For them it is also rooted in the fact that the electromagnetic self-force problem is deeply analogous to the gravitational self-force problem, which is of direct relevance to future gravitational wave observations. The motion of point particles in curved spacetime has been the topic of a recent Topical Review [1], and it was the focus of a recent Special Issue [2]. It is surprising to me that radiation reaction is a subject that continues to be poorly covered in the standard textbooks, including Jackson's bible [3]. Exceptions are Rohrlich's excellent text [4], which makes a very useful introduction to radiation reaction, and the Landau and Lifshitz classic [5], which contains what is probably the most perfect summary of the foundational ideas (presented in characteristic terseness). It is therefore with some trepidation that I received Herbert Spohn's book, which covers both the classical and quantum theories of a charged particle coupled to its own field (the presentation is limited to flat spacetime). Is this the text that graduate students and researchers should turn to in order to get a complete and accessible education in radiation reaction? My answer is that while the book does indeed contain a lot of useful material, it is not a very accessible source of information, and it is certainly not a student-friendly textbook. Instead, the book presents a technical account of the author's personal take on the theory, and represents a culminating summary of the author's research contributions over more than a decade. The book is written in a fairly mathematical style (the author is Professor of Mathematical Physics at the Technische Universitat in Munich), and it very much emphasises mathematical rigour. This makes the book less accessible than I would wish it to be, but this is perhaps less a criticism than a statement about my taste, expectation, and attitude. The presentation of the classical theory begins with a point particle, but Spohn immediately smears the charge distribution to eliminate the vexing singularities of the retarded field. He considers both the nonrelativistic Abraham model (in which the extended particle is spherically symmetric in the laboratory frame) and the relativistic Lorentz model (in which the particle is spherical in its rest frame). In Spohn's work, the smearing of the charge distribution is entirely a mathematical procedure, and I would have wished for a more physical discussion. A physically extended body, held together against electrostatic repulsion by cohesive forces (sometimes called Poincar? stresses) would make a sound starting point for a classical theory of charged particles, and would have nicely (and physically) motivated the smearing operation adopted in the book. Spohn goes on to derive energy?momentum relations for the extended objects, and to obtain their equations of motion. A compelling aspect of his presentation is that he formally introduces the 'adiabatic limit', the idea that the external fields acting on the charged body should have length and time scales that are long compared with the particle's internal scales (respectively the electrostatic classical radius and its associated time scale). As a consequence, the equations of motion do not involve a differentiated acceleration vector (as is the case for the Abraham?Lorentz?Dirac equations) but are proper second-order differential equations for the position vector. In effect, the correct equations of motion are obtained from the Abraham?Lorentz?Dirac equations by a reduction-of-order procedure that was first proposed (as far as I know) by Landau and Lifshitz [5]. In Spohn's work this procedure is not {\it ad hoc}, but a natural consequence of the adiabatic approximation. An aspect of the classical portion of the book that got me particularly excited is Spohn's proposal for an experimental test of the predictions of the Landau?Lifshitz equations. His proposed experiment involves a Penning trap, a device that uses a uniform magnetic field and a quadrupole electric field to trap an electron for very long times. Without radiation reaction, the motion of an electron in the trap is an epicycle that consists of a rapid (and small) cyclotron orbit superposed onto a slow (and large) magnetron orbit. Spohn shows that according to the Landau?Lifshitz equations, the radiation reaction produces a damping of the cyclotron motion. For reasonable laboratory situations this damping occurs over a time scale of the order of 0.1 second. This experiment might well be within technological reach. The presentation of the quantum theory is based on the nonrelativistic Abraham model, which upon quantization leads to the well-known Pauli-Fierz Hamiltonian of nonrelativistic quantum electrodynamics. This theory, an approximation to the fully relativistic version of QED, has a wide domain of validity that includes many aspects of quantum optics and laser-matter interactions. As I am not an expert in this field, my ability to review this portion of Spohn's book is limited, and I will indeed restrict myself to a few remarks. I first admit that I found Spohn's presentation to be tough going. Unlike the pair of delightful books by Cohen-Tannoudji, Dupont-Roc, and Grynberg [6, 7], this is not a gentle introduction to the quantum theory of a charged particle coupled to its own electromagnetic field. Instead, Spohn proceeds rather quickly through the formulation of the theory (defining the Hamiltonian and the Hilbert space) and then presents some applications (for example, he constructs the ground states of the theory, he examines radiation processes, and he explores finite-temperature aspects). There is a lot of material in the eight chapters devoted to the quantum theory, but my insufficient preparation and the advanced nature of Spohn's presentation were significant obstacles; I was not able to draw much appreciation for this material. One of the most useful resources in Spohn's book are the historical notes and literature reviews that are inserted at the end of each chapter. I discovered a wealth of interesting articles by reading these, and I am grateful that the author made the effort to collect this information for the benefit of his readers. References [1] Poisson E 2004 Radiation reaction of point particles in curved spacetime Class. Quantum Grav 21 R153?R232 [2] Lousto C O 2005 Special issue: Gravitational Radiation from Binary Black Holes: Advances in the Perturbative Approach, Class. Quantum Grav22 S543?S868 [3] Jackson J D 1999 Classical Electrodynamics Third Edition (New York: Wiley) [4] Rohrlich F 1990 Classical Charged Particles (Redwood City, CA: Addison?Wesley) [5] Landau L D and Lifshitz E M 2000 The Classical Theory of Fields Fourth Edition (Oxford: Butterworth?Heinemann) [6] Cohen-Tannoudji C Dupont-Roc J and Grynberg G 1997 Photons and Atoms - Introduction to Quantum Electrodynamics (New York: Wiley-Interscience) [7] Cohen-Tannoudji C, Dupont-Roc J and G Grynberg G 1998 Atom?Photon Interactions: Basic Processes and Applications (New York: Wiley-Interscience)
258 citations
Max Planck Society1, Lawrence Livermore National Laboratory2, Georgia Institute of Technology3, École normale supérieure de Lyon4, University of Zaragoza5, University of Padua6, Harvard University7, University of Liège8, University of the Basque Country9, Martin Luther University of Halle-Wittenberg10, Lille University of Science and Technology11, University of California, Merced12, University of Tsukuba13
TL;DR: The Octopus project as mentioned in this paper provides a unique framework that allows us to describe non-equilibrium phenomena in molecular complexes, low dimensional materials, and extended systems by accounting for electronic, ionic, and photon quantum mechanical effects within a generalized time-dependent density functional theory.
Abstract: Over the last few years, extraordinary advances in experimental and theoretical tools have allowed us to monitor and control matter at short time and atomic scales with a high degree of precision. An appealing and challenging route toward engineering materials with tailored properties is to find ways to design or selectively manipulate materials, especially at the quantum level. To this end, having a state-of-the-art ab initio computer simulation tool that enables a reliable and accurate simulation of light-induced changes in the physical and chemical properties of complex systems is of utmost importance. The first principles real-space-based Octopus project was born with that idea in mind, i.e., to provide a unique framework that allows us to describe non-equilibrium phenomena in molecular complexes, low dimensional materials, and extended systems by accounting for electronic, ionic, and photon quantum mechanical effects within a generalized time-dependent density functional theory. This article aims to present the new features that have been implemented over the last few years, including technical developments related to performance and massive parallelism. We also describe the major theoretical developments to address ultrafast light-driven processes, such as the new theoretical framework of quantum electrodynamics density-functional formalism for the description of novel light-matter hybrid states. Those advances, and others being released soon as part of the Octopus package, will allow the scientific community to simulate and characterize spatial and time-resolved spectroscopies, ultrafast phenomena in molecules and materials, and new emergent states of matter (quantum electrodynamical-materials).
215 citations
TL;DR: Experiments at the interface of quantum optics and chemistry have revealed that strong coupling between light and matter can substantially modify the chemical and physical properties of molecules a... as mentioned in this paper, which can be seen as an example of the relationship between quantum mechanics and chemistry.
Abstract: Experiments at the interface of quantum optics and chemistry have revealed that strong coupling between light and matter can substantially modify the chemical and physical properties of molecules a...
91 citations
Max Planck Society1, Lawrence Livermore National Laboratory2, Georgia Institute of Technology3, École normale supérieure de Lyon4, University of Zaragoza5, University of Padua6, Harvard University7, University of Liège8, University of the Basque Country9, Martin Luther University of Halle-Wittenberg10, Lille University of Science and Technology11, University of California, Merced12, University of Tsukuba13
TL;DR: The major theoretical developments to address ultrafast light-driven processes, such as the new theoretical framework of quantum electrodynamics density-functional formalism for the description of novel light-matter hybrid states are described.
Abstract: Over the last years extraordinary advances in experimental and theoretical tools have allowed us to monitor and control matter at short time and atomic scales with a high-degree of precision. An appealing and challenging route towards engineering materials with tailored properties is to find ways to design or selectively manipulate materials, especially at the quantum level. To this end, having a state-of-the-art ab initio computer simulation tool that enables a reliable and accurate simulation of light-induced changes in the physical and chemical properties of complex systems is of utmost importance. The first principles real-space-based Octopus project was born with that idea in mind, providing an unique framework allowing to describe non-equilibrium phenomena in molecular complexes, low dimensional materials, and extended systems by accounting for electronic, ionic, and photon quantum mechanical effects within a generalized time-dependent density functional theory framework. The present article aims to present the new features that have been implemented over the last few years, including technical developments related to performance and massive parallelism. We also describe the major theoretical developments to address ultrafast light-driven processes, like the new theoretical framework of quantum electrodynamics density-functional formalism (QEDFT) for the description of novel light-matter hybrid states. Those advances, and other being released soon as part of the Octopus package, will enable the scientific community to simulate and characterize spatial and time-resolved spectroscopies, ultrafast phenomena in molecules and materials, and new emergent states of matter (QED-materials).
83 citations
TL;DR: New algorithms and computational approaches to predict and understand the behavior of correlated quantum matter are reviewed, presenting the state-of-the-art in the field toward algorithms with nonexponential complexity for correlated quantum Matter with applications in grand-challenge problems.
Abstract: Discoveries in quantum materials, which are characterized by the strongly quantum-mechanical nature of electrons and atoms, have revealed exotic properties that arise from correlations. It is the p...
76 citations
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TL;DR: In this paper, the Hartree and Hartree-Fock equations are applied to a uniform electron gas, where the exchange and correlation portions of the chemical potential of the gas are used as additional effective potentials.
Abstract: From a theory of Hohenberg and Kohn, approximation methods for treating an inhomogeneous system of interacting electrons are developed. These methods are exact for systems of slowly varying or high density. For the ground state, they lead to self-consistent equations analogous to the Hartree and Hartree-Fock equations, respectively. In these equations the exchange and correlation portions of the chemical potential of a uniform electron gas appear as additional effective potentials. (The exchange portion of our effective potential differs from that due to Slater by a factor of $\frac{2}{3}$.) Electronic systems at finite temperatures and in magnetic fields are also treated by similar methods. An appendix deals with a further correction for systems with short-wavelength density oscillations.
47,477 citations
TL;DR: In this paper, the self-interaction correction (SIC) of any density functional for the ground-state energy is discussed. But the exact density functional is strictly selfinteraction-free (i.e., orbitals demonstrably do not selfinteract), but many approximations to it, including the local spin-density (LSD) approximation for exchange and correlation, are not.
Abstract: The exact density functional for the ground-state energy is strictly self-interaction-free (i.e., orbitals demonstrably do not self-interact), but many approximations to it, including the local-spin-density (LSD) approximation for exchange and correlation, are not. We present two related methods for the self-interaction correction (SIC) of any density functional for the energy; correction of the self-consistent one-electron potenial follows naturally from the variational principle. Both methods are sanctioned by the Hohenberg-Kohn theorem. Although the first method introduces an orbital-dependent single-particle potential, the second involves a local potential as in the Kohn-Sham scheme. We apply the first method to LSD and show that it properly conserves the number content of the exchange-correlation hole, while substantially improving the description of its shape. We apply this method to a number of physical problems, where the uncorrected LSD approach produces systematic errors. We find systematic improvements, qualitative as well as quantitative, from this simple correction. Benefits of SIC in atomic calculations include (i) improved values for the total energy and for the separate exchange and correlation pieces of it, (ii) accurate binding energies of negative ions, which are wrongly unstable in LSD, (iii) more accurate electron densities, (iv) orbital eigenvalues that closely approximate physical removal energies, including relaxation, and (v) correct longrange behavior of the potential and density. It appears that SIC can also remedy the LSD underestimate of the band gaps in insulators (as shown by numerical calculations for the rare-gas solids and CuCl), and the LSD overestimate of the cohesive energies of transition metals. The LSD spin splitting in atomic Ni and $s\ensuremath{-}d$ interconfigurational energies of transition elements are almost unchanged by SIC. We also discuss the admissibility of fractional occupation numbers, and present a parametrization of the electron-gas correlation energy at any density, based on the recent results of Ceperley and Alder.
16,027 citations
TL;DR: It is found that these pseudopotentials are extremely efficient for the cases where the plane-wave expansion has a slow convergence, in particular, for systems containing first-row elements, transition metals, and rare-earth elements.
Abstract: We present a simple procedure to generate first-principles norm-conserving pseudopotentials, which are designed to be smooth and therefore save computational resources when used with a plane-wave basis. We found that these pseudopotentials are extremely efficient for the cases where the plane-wave expansion has a slow convergence, in particular, for systems containing first-row elements, transition metals, and rare-earth elements. The wide applicability of the pseudopotentials are exemplified with plane-wave calculations for copper, zinc blende, diamond, \ensuremath{\alpha}-quartz, rutile, and cerium.
13,174 citations
Book•
[...]
01 Jan 1980
TL;DR: In this article, a modern pedagogic introduction to the ideas and techniques of quantum field theory is presented, with a brief overview of particle physics and a survey of relativistic wave equations and Lagrangian methods.
Abstract: This book is a modern pedagogic introduction to the ideas and techniques of quantum field theory. After a brief overview of particle physics and a survey of relativistic wave equations and Lagrangian methods, the quantum theory of scalar and spinor fields, and then of gauge fields, is developed. The emphasis throughout is on functional methods, which have played a large part in modern field theory. The book concludes with a brief survey of 'topological' objects in field theory and, new to this edition, a chapter devoted to supersymmetry.
8,581 citations
TL;DR: In this paper, the three-parameter Lee-Yang-Parr (B3LYP) functional was used to compute low-lying electronic excitations of N2, ethylene, formaldehyde, pyridine and porphin.
5,087 citations