In this paper, four different ways are described in which homogeneous, isotropic, nonferromagnetic, Maxwellian media at rest may exhibit absorption and stimulated emission. These four ways may be identified by a positive or negative conductivity, a sink or source-type electric field, a complex dielectric constant, and a complex permeability. The forms of the electromagnetic waves, the refractive index, and the positive or negative extinction coefficient are determined for each process for both absorbing and active media. Spontaneous emission is associated with source-type electric and magnetic fields which generate conduction or displacement currents in the medium with improper phases to contribute to the radiant flux in the incident electromagnetic wave. Stimulated emission is characterized by exponentially increasing incident electric and magnetic fields and an excess of the time average of the outflow of radiant flux over the surfaces of an arbitrary volume. Stimulated emission appears when the time average of the rate at which the source-type electric and magnetic fields do work in carrying certain conduction or displacement currents in directions opposite to the incident electric and magnetic fields is greater than the time average of the rate at which the incident electric and magnetic fields dissipate energy by doing work in carrying other conduction or displacement currents in directions parallel to the incident electric and magnetic fields.
In this paper, four different ways are described in which homogeneous, isotropic, nonferromagnetic, Maxwellian media at rest may exhibit absorption and stimulated emission. These four ways may be identified by a positive or negative conductivity, a sink or source-type electric field, a complex dielectric constant, and a complex permeability. The forms of the electromagnetic waves, the refractive index, and the positive or negative extinction coefficient are determined for each process for both absorbing and active media. Spontaneous emission is associated with source-type electric and magnetic fields which generate conduction or displacement currents in the medium with improper phases to contribute to the radiant flux in the incident electromagnetic wave. Stimulated emission is characterized by exponentially increasing incident electric and magnetic fields and an excess of the time average of the outflow of radiant flux over the surfaces of an arbitrary volume. Stimulated emission appears when the time average of the rate at which the source-type electric and magnetic fields do work in carrying certain conduction or displacement currents in directions opposite to the incident electric and magnetic fields is greater than the time average of the rate at which the incident electric and magnetic fields dissipate energy by doing work in carrying other conduction or displacement currents in directions parallel to the incident electric and magnetic fields.
It is generally believed that absorption and stimulated emission are inverse processes, as both are driven by an external field, their strength is quantified by the same Einstein B coefficient, and they occur with a defined phase, opposite to each other, namely in phase and in anti-phase with the driving field, whereas spontaneous emission is a different process that occurs with an arbitrary phase with respect to a potential incident field. Recently, the phase relation in absorption and emission was shown to differ from this believe. Here it is verified via the amplitude–phase diagram and via the interference of sine waves that, precisely speaking, only the absorption process, in which a number φ + 1 of incident photons is decreased by one photon, and the emission process, in which a number φ of incident photons is increased by one photon, are truly inverse processes also in their phase. Particularly, this implies that absorption of a single incident photon and spontaneous emission of a photon into an empty mode are inverse processes in the amplitude–phase diagram.
We consider the spontaneous emission in an absorbing medium by calculating the quantum flow of energy from an emitting atom. For this purpose, we extend the analysis by Power and Thirunamachandran of quantized Maxwell fields in the vicinity of an atom in the free space to a situation where the emitter is in a dielectric medium. We represent the quantum flow in terms of the non-equal time commutators involving electric and magnetic fields, as well as the local displacement field. The commutators are calculated applying a previously developed microscopic theory of quantization of radiation in dielectrics. Consequently, we derive from first principles the rate of spontaneous emission in an absorbing medium containing local field factors and other refractive contributions. The results support the previous introduction of the (virtual cavity) local field correction by Barnett et al on a phenomenological basis, as well as our previous approach in which the spontaneous emission is considered as a resonance energy transfer to the far-zone atoms. A distinctive feature of the present formalism is that it deals with the spontaneous emission directly by calculating the quantum flow from the emitting atom. Therefore, the method is free from divergences appearing in other approaches analysing the spontaneous decay in absorbing media.
Abstract In his celebrated 1916–17 papers in which he proposed the A and B coefficients for the spontaneous and stimulated emission of energy quanta from excited atoms, Einstein conjectured that stimulated emission involves the release of individual quanta (later dubbed “photons”) along the direction of an incident photon with the same energy, momentum, phase, and polarization state as that of the incident photon. According to classical electrodynamics, of course, an oscillating dipole must radiate an azimuthally symmetric electromagnetic field around its axis of oscillation. Nevertheless, Einstein suggested that the release of stored energy from excited atoms in the form of discrete quanta (photons) must be directional, and that, in the case of stimulated emission, the direction of the emitted photon must coincide with that of the incident photon. The goal of the present paper is to show that some of the prominent features of absorption and stimulated emission emerge from Maxwellian electrodynamics in conjunction with the simple mass-and-spring model of an atom known as the Lorentz oscillator model.
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.
In the literature one finds several conflicting accounts of the phase difference of stimulated and spontaneous emission, as well as absorption, with respect to an existing (triggering) electromagnetic field. One of these approaches proposes that stimulated emission and absorption occur in phase and out of phase with their driving field, respectively, whereas spontaneous emission occurs under an arbitrary phase difference with respect to an existing field. It has served as a basis for explaining quantum-mechanically the laser linewidth, its narrowing by a factor of 2 around the laser threshold, as well as its broadening due to amplitude–phase coupling, resulting in Henry’s α-factor. Assuming the validity of Maxwell’s equations, all three processes would, thus, violate the law of energy conservation. In semi-classical approaches, we investigate stimulated emission in a Fabry–Perot resonator, analyze the Lorentz oscillator model, apply the Kramers–Kronig relations to the complex susceptibility, understand the summation of quantized electric fields, and quantitatively interpret emission and absorption in the amplitude–phase diagram. In all cases, we derive that the phase of stimulated emission is 90° in lead of the driving field, and the phase of absorption lags 90° behind the transmitted field. Also spontaneous emission must obey energy conservation, hence it occurs with 90° phase in lead of an existing field. These semi-classical findings agree with recent experimental investigations regarding the interaction of attosecond pulses with an atom, thereby questioning the physical explanation of the laser linewidth and its narrowing or broadening.
Nonlinear optics is the study of the response of dielectric media to strong optical fields. The fields are sufficiently strong that the response of the medium is, as its name implies, nonlinear. That is, the polarization, which is the dipole moment per unit volume in the medium, is not a linear function of the applied electric field. In the equation for the polarization, there is a linear term, but, in addition, there are terms containing higher powers of the electric field. This leads to significant new types of behavior, one of the most notable being that frequencies different from that of the incident electromagnetic wave, such as harmonics or subharmonics, can be generated. Linear media do not change the frequency of light incident upon them. The first observation of a nonlinear optical effect was, in fact, second-harmonic generation – a laser beam entering a nonlinear medium produced a second beam at twice the frequency of the original. Another type of behavior that becomes possible in nonlinear media is that the index of refraction, rather than being a constant, is a function of the intensity of the light. For a light beam with a nonuniform intensity profile, this can lead to self-focusing of the beam. Most nonlinear optical effects can be described using classical electromagnetic fields, and, in fact, the initial theory of nonlinear optics was formulated assuming the fields were classical. When the fields are quantized, however, a number of new effects emerge. Quantized fields are necessary if we want to describe fields that originate from spontaneous emission. For example, in a process known as spontaneous parametric down-conversion, a beam of light at one frequency, the pump, produces a beam at half the original frequency, the signal. This second beam is a result of spontaneous emission.