The coherent energy transfer efficiency of a pair of two-level atoms is studied theoretically and its mathematical expression has been deduced. The problem of atoms coherent energy transfer theory is treated by quantum perturbation theory and equivalent method replacing atomic dipole field with light field of the same frequency. The detuning between the donor atom transition frequency and the acceptor atom transition frequency has been studied in the theory. With the increase of the detuning of the two-atomic transition frequency, the energy transfer efficiency decays rapidly. In the case of two-atomic transition frequency resonance, the coherent resonance energy transfer efficiency is directly proportional to the square of the sine of the minus three power of the distance between two atoms and the energy transfer efficiency is periodically decaying over time. The coherent resonance energy transfer efficiency is inversely proportional to the six power of the distance between the two atoms in the first-order approximation.
The coherent energy transfer efficiency of a pair of two-level atoms is studied theoretically and its mathematical expression has been deduced. The problem of atoms coherent energy transfer theory is treated by quantum perturbation theory and equivalent method replacing atomic dipole field with light field of the same frequency. The detuning between the donor atom transition frequency and the acceptor atom transition frequency has been studied in the theory. With the increase of the detuning of the two-atomic transition frequency, the energy transfer efficiency decays rapidly. In the case of two-atomic transition frequency resonance, the coherent resonance energy transfer efficiency is directly proportional to the square of the sine of the minus three power of the distance between two atoms and the energy transfer efficiency is periodically decaying over time. The coherent resonance energy transfer efficiency is inversely proportional to the six power of the distance between the two atoms in the first-order approximation.
The quantum electrodynamical theory of coherent fluorescence resonance energy transfer (FRET) between two dipoles (free atoms, molecules or dopant centres in crystalline matrices at low temperature conditions) in an arbitrary non-dissipative environment is elaborated using a canonical quantization scheme. It is shown that population dynamics of both atoms can be expressed in terms of a classical Green function. This general theory corresponds well to the problem of description of controllable quantum manipulations under the donor-acceptor system (e.g. its application for FRET scanning near-field optical microscopy-based quantum computing). In addition, its usefulness is illustrated for the case of coherent FRET in free space and for the case when atoms are placed near an ideally conducting plane. The possibility of creating an entangled state of three atoms is demonstrated.
The nonlinear interaction of two intense optical waves with three energy levels of an atomic system is analyzed theoretically. The frequencies of the applied fields are assumed to be on or near two of the resonances involving the three levels. Particular attention is given to the generation of power at the difference frequency of the two applied fields where their frequency separation lies in the far-infrared range of the spectrum. In the limit of large input fields where atomic transitions are driven to saturation, the generated difference-frequency power is no longer proportional to the product of the two input powers. It is shown that, in this limit, the total rate of emission of photons at the difference frequency may, in principle, approach a value given by TrN, where N is the total number of atoms, T is the average time of coherent interaction of atoms and the radiation field, and r is a factor which in favorable cases approaches unity at low temperatures. Also, a number of additional effects are encountered due to coherent double-quantum transitions among various levels which may be ignored only for weak input powers. These effects are highly dependent on the modes of relaxations of atomic levels and the details of the line shape. The results are applied to several cases, in which the resonance condition yields large efficiency in nonlinear frequency mixing.
The interaction of simple, two- and three-level atomic systems with monochromatic and nonmonochromatic laser radiation near resonance transitions is discussed based on the Schroedinger equation with radiation decay and no collisional relaxation, outside the framework of the usual perturbation theory. The mathematical schemes employed include the resonance approximation, exact methods, the quasi-energy method, the adiabatic approximation, etc. A large number of physical phenomena, such as oscillating and inverted populations, self-induced resonances, processes of first order in the weak field, Raman scattering, coherent population transfer, etc. are considered. The review is intended for a broad readership.
We study coherent energy transfer of a single excitation and quantum entanglement in a dimer, which consists of a donor and an acceptor modeled by two two-level systems. Between the donor and the acceptor, there exists a dipole-dipole interaction, which provides the physical mechanism for coherent energy transfer and entanglement generation. The donor and the acceptor couple to two independent heat baths with diagonal couplings that do not dissipate the energy of the noncoupling dimer. Special attention is paid to the effect on single-excitation energy transfer and entanglement generation of the energy detuning between the donor and the acceptor and the temperatures of the two heat baths. It is found that, the probability for single-excitation energy transfer largely depends on the energy detuning in the low temperature limit. Concretely, the positive and negative energy detunings can increase and decrease the probability at steady state, respectively. In the high temperature limit, however, the effect of the energy detuning on the probability is negligibly small. We also find that the probability is negligibly dependent on the bath temperature difference of the two heat baths. In addition, it is found that quantum entanglement can be generated in the process of coherent energy transfer. As the bath temperature increases, the generated steady-state entanglement decreases. For a given bath temperature, the steady-state entanglement decreases with the increase of the absolute value of the energy detuning.
Excitation energy transfer is a photophysical process upon which many chemical and biological phenomena are built. From natural small systems to synthetic multichromophoric macromolecules, energy transfer deals with the process of migration of electronic excitation energy from an excited donor to an acceptor. Although this phenomenon has been extensively studied in the past, the rapid evolution of quantum-enabled technologies has led to the question of whether nonclassical sources of light, such as entangled photon pairs, may provide us with better control (or enhancement) of energy transfer at the nanoscale. In this work we provide a comprehensive study of the joint excitation of two noninteracting two-level atoms by time-frequency-correlated photon pairs (whose central frequencies are not resonant with the individual particles) generated by means of spontaneous parametric down-conversion (SPDC). We demonstrate that while strong frequency anticorrelation between photons guarantees a large two-photon excitation (TPE) probability, photons bearing a sine cardinal spectral shape exhibit an approximately 3.8 times larger TPE signal than photons with a Gaussian spectrum. More importantly, we find that suppression of time-ordered excitation pathways does not substantially modify the TPE probability for two-photon states with a Gaussian spectral shape, whereas photons with a sine cardinal spectrum exhibit the strongest TPE signals when two-photon excitation pathways are not suppressed. Our results not only help elucidate the role of time-frequency correlations in resonance energy transfer with SPDC photons, but also provide valuable information regarding the optimal source to be used in the experimental implementation of said process.
We derive a unified quantum theory of coherent and incoherent energy transfer between two atoms (donor and acceptor) valid in arbitrary Markovian nanophotonic environments. Our theory predicts a fundamental bound ηmax=γd+γaγa for energy transfer efficiency arising from the spontaneous emission rates γd and γa of the donor and acceptor. We propose the control of the acceptor spontaneous emission rate as a new design principle for enhancing energy transfer efficiency. We predict an experiment using mirrors to enhance the efficiency bound by exploiting the dipole orientations of the donor and acceptor. Of fundamental interest, we show that while quantum coherence implies the ultimate efficiency bound has been reached, reaching the ultimate efficiency does not require quantum coherence. Our work paves the way towards nanophotonic analogues of efficiency enhancing environments known in quantum biological systems.