Radiative transition of atomic electrons radiative transitions between discrete states in atomic systems atomic photoprocesses involving free particles coherent phenomena in radiative transitions atoms in strong fields.
Radiative transitions are quantum-state transitions in matter quantum systems (such as atoms， ions， and molecules) caused by their interaction with the electromagnetic field， and accompanied by the emission or absorption of photons.Their theoretical description involves physical theories including quantum mechanics and quantum electrodynamics， as well as mathematical tools such as spherical tensors and group theory.Focusing on radiative transitions of doped ions in solids， this paper summarizes earlier related theories and aims to concisely introduce fundamental theories and mathematical expressions while maintaining rigor， and to clearly describe the underlying physical pictures and mechanisms.The topics covered include atomic quantum states， the quantized electromagnetic field， multipole radiative transitions and selection rules， stimulated absorption， stimulated emission and spontaneous emission， transition probability and excited-state lifetimes.The article also discusses f-f and 4f-5d transitions of rare-earth ions and dd transitions of transition-metal ions， involving Judd -Ofelt theory， crystal-field theory， electronvibration coupling， and the Dorenbos model， as well as statistical analysis， machine learning， and firstprinciples methods.This work may provide a theoretical reference for the study of rare-earth-and transition-metaldoped luminescent materials.Keywords： radiative transition； theory； physical picture； f-f transition； d-d transition； 4f-5d transition 文章编号： 1000-7032(XXXX)XX
Radiation can change the energy state of matter via three optical processes: spontaneous emission, absorption and stimulated emission. In spontaneous emission, an excited atomic or molecular state decays to a lower energy state with the emission of a photon of energy equal to the difference in the quantum state energies. Photon absorption is the reverse process, with a photon causing excitation from a lower to an excited quantum state. Stimulated emission was first proposed by Einstein in a paper published in 1917. He attempted to balance spontaneous emission and photon absorption, but could not get the correct balance without the postulated process of stimulated emission (see Section 4.2). With stimulated emission, an excited quantum state is stimulated to decay to a lower quantum state by an impinging photon. The existing photon survives with another identical photon being created (so that energy is conserved). The rates at which radiative transitions occur can be calculated using quantum mechanics. The time-dependent Schrodinger equation is used with the system wavefunction comprising time-varying linear combinations of the two wavefunctions for the lower and upper quantum states. In semi-classical treatments, an atom is treated quantum mechanically with the radiation field treated classically. There is a perturbation in energy associated with, say, the electric field of the radiation interacting with the electric dipole of the atom, though other interactions can be significant if the electric dipole interaction energy is small. In absorption, for example, a differential equation representing the change in ‘weighting’ of the wavefunction from the lower to upper state is obtained. A ‘time constant’ for the speed of change represents the rate of the radiative process. We examine the quantum mechanical nature of radiation absorption in Section 10.1 before discussing (Section 10.3) another important parameter arising with radiative transitions between discrete bound quantum states: the lineshape function. Quantum Theory of the Atom–Radiation Interaction An expression for the Einstein B-coefficient for photo-absorption is derived using quantum mechanics in this section. Einstein determined the detailed balance relationship between the rates of spontaneous emission, photo-absorption and stimulated emission when light interacts with an atom by considering an atomic system of two energy levels which are in equilibrium with a black-body radiation field. We use a semi-classical treatment where the atom is treated quantum mechanically and the radiation field is treated as a classical oscillating electric field.
This book presents and describes a series of unusual and striking strong-field phenomena concerning atoms and free electrons. Some of these phenomena are: multiphoton stimulated bremsstrahlung, free-electron lasers, wave-packet physics, above-threshold ionization, and strong-field stabilization in Rydberg atoms. The theoretical foundations and causes of the phenomena are described in detail, with all the approximations and derivations discussed. All the known and relevant experiments are described too, and their results are compared with those of the existing theoretical models.An extensive ge
A reduced-density-operator description is developed for coherent optical phenomena in many-electron atomic systems, utilizing a Liouville-space, multiple-mode Floquet–Fourier representation. The Liouville-space formulation provides a natural generalization of the ordinary Hilbert-space (Hamiltonian) R-matrix-Floquet method, which has been developed for multi-photon transitions and laser-assisted electron–atom collision processes. In these applications, the R-matrix-Floquet method has been demonstrated to be capable of providing an accurate representation of the complex, multi-level structure of many-electron atomic systems in bound, continuum, and autoionizing states. The ordinary Hilbert-space (Hamiltonian) formulation of the R-matrix-Floquet method has been implemented in highly developed computer programs, which can provide a non-perturbative treatment of the interaction of a classical, multiple-mode electromagnetic field with a quantum system. This quantum system may correspond to a many-electron, bound atomic system and a single continuum electron. However, including pseudo-states in the expansion of the many-electron atomic wave function can provide a representation of multiple continuum electrons. The 'dressed' many-electron atomic states thereby obtained can be used in a realistic non-perturbative evaluation of the transition probabilities for an extensive class of atomic collision and radiation processes in the presence of intense electromagnetic fields. In order to incorporate environmental relaxation and decoherence phenomena, we propose to utilize the ordinary Hilbert-space (Hamiltonian) R-matrix-Floquet method as a starting-point for a Liouville-space (reduced-density-operator) formulation. To illustrate how the Liouville-space R-matrix-Floquet formulation can be implemented for coherent atomic radiative processes, we discuss applications to electromagnetically induced transparency, as well as to related pump–probe optical phenomena, and also to the unified description of radiative and dielectronic recombination in electron–ion beam interactions and high-temperature plasmas.
Abstract In this introductory chapter, we consider the elementary radiative processes for both free atomic particles (atoms, ions, and molecules) and particles interacting with a monochromatic laser field. For more advanced considerations, the reader is advised to refer to the classical textbooks (Loudon 1973; Sargent et al. 1974; Allen and Eberly 1975; Sobelman 1979; Haken 1981; Knight and Allen 1983; Meystre and Sargent 1990; Cohen-Tannoudji et al. 1992; Foot 2004). Extensions of this material are treated in subsequent chapters, wherein various light field configurations, atomic particles, and the processes of interaction between atomic particles and laser fields are considered in detail.
Classically, a charged particle in a magnetic field emits radiation, losing momentum and experiencing the Abraham-Lorentz (AL) / Landau-Lifshitz (LL) radiation reaction (RR) force. However, at atomic scales and outside the range of their applicability, the AL/LL equations fail and RR destroys the coherent state of an electron-undermining the very concept of a RR force. This process can be described by the coupled Schrödinger-Maxwell (SM) system under appropriate limits, but the system's nonlinear complexity has long limited purely analytical studies. We present geometric structure-preserving algorithms for the SM system that preserve gauge invariance, symplecticity, and unitarity on the discrete space-time lattice, which are implemented in our Structure-Preserving scHrodINger maXwell (SPHINX) code. By constructing coherent states from the Landau levels, SPHINX simulates the fully-coupled nonlinear dynamics of an electron coherent state, the energy partition evolution, and decoherence/relaxation of the electron wave packet in time due to RR. These simulations indicate that, in an external magnetic field, an electron prepared in an atomic-scale coherent state can radiate strongly, rapidly losing coherence and dispersing into a decoherent wave packet. Additionally, we also present the fully-coupled nonlinear evolution of the non-degenerate ground- and first-excited Landau levels themselves to understand how the coupled SM system modifies the well-known ideal (i.e., Schrödinger-only) dynamics of the Landau Levels. With appropriate boundary conditions, simulations show that the Landau levels are renormalized into stationary dressed eigenstates with constant electromagnetic and kinetic energies. This opens a new computational window into RR physics and advances modeling of extreme-field phenomena in fusion plasmas, astrophysics, and next-generation laser experiments