We develop a rigorous theory for nanophotonic cooperative spontaneous emission of an ensemble of quantum emitters near matter, which also incorporates absorption. Such theory is highly requested since one should expect that in the field of nanophotonics the close-by emitters will emit cooperatively simultaneously with strong interaction with the exotic metamaterial complex dielectric function. The closed-form model developed here considers the buildup both of interemitter correlation over time through emitter transitions via the mutual field and of geometry-induced spatial correlation. The presence of matter alters the local density of states (LDOS), resulting in modified decay rate and emission intensity for the entire ensemble relative to values of spontaneous emission in free space. The superradiant total emission is separable into a quantum-mechanical time-dependent part and a classical space-dependent part, both being functions of the LDOS. Two distinct radiative emitter--far-field coupling mechanisms, which together account for the superradiant emission, are obtained---the coupling of every individual emitter with the far field and the coupling of emitter pairs to the far field. The calculations for superradiating emitters near silver and near-zero epsilon (NZE) materials were performed with the following results: the silver sphere augments the superradiant far-field intensity and rate by up to 400 and 1000%, respectively, while the NZE sphere enhances the far-field intensity and rate of the superradiance by approximately 1400 and 400%, respectively.
We develop a rigorous theory for nanophotonic cooperative spontaneous emission of an ensemble of quantum emitters near matter, which also incorporates absorption. Such theory is highly requested since one should expect that in the field of nanophotonics the close-by emitters will emit cooperatively simultaneously with strong interaction with the exotic metamaterial complex dielectric function. The closed-form model developed here considers the buildup both of interemitter correlation over time through emitter transitions via the mutual field and of geometry-induced spatial correlation. The presence of matter alters the local density of states (LDOS), resulting in modified decay rate and emission intensity for the entire ensemble relative to values of spontaneous emission in free space. The superradiant total emission is separable into a quantum-mechanical time-dependent part and a classical space-dependent part, both being functions of the LDOS. Two distinct radiative emitter--far-field coupling mechanisms, which together account for the superradiant emission, are obtained---the coupling of every individual emitter with the far field and the coupling of emitter pairs to the far field. The calculations for superradiating emitters near silver and near-zero epsilon (NZE) materials were performed with the following results: the silver sphere augments the superradiant far-field intensity and rate by up to 400 and 1000%, respectively, while the NZE sphere enhances the far-field intensity and rate of the superradiance by approximately 1400 and 400%, respectively.
Spontaneous emission from ensembles of quantum emitters (QEs) such as atoms, molecules or semiconductor quantum dots can be greatly enhanced by cooperative effects arising from electromagnetic correlations. We describe a cooperative mechanism for emission of light by an ensemble of QEs based upon cooperative energy transfer from QEs to localized surface plasmons in metal-dielectric structures followed by plasmon radiation at a rate that scales with the ensemble size. For large QE ensembles saturating the plasmon mode volume, we derive universal, i.e. independent of local field distribution, expression for cooperative Purcell factor that can by far exceed the field enhancement limits for individual QE in a hot spot. We also derive radiated power spectrum that retains the plasmon resonance lineshape and, in contrast to common cooperative mechanisms, is insensitive to natural variations of QEs' emission frequencies.
Indistinguishable quantum emitters confined to length scales smaller than the wavelength of the light become superradiant. Compared to uncorrelated and distinguishable emitters, superradiance results in qualitative modifications of optical signals such as photon coincidences. However, recent experiments revealed that similar signatures can also be obtained in situations where emitters are too far separated to be superradiant if correlations between emitters are induced by the wave-function collapse during an emission-angle-selective photon detection event. Here, we compare two sources for cooperative emission, superradiance and measurement-induced cooperativity, and analyze their impact on time-dependent optical signals. We find that an antidip in photon coincidences at zero time delay is a signature of interemitter correlations in general but does not unambiguously prove the presence of superradiance. This suggests that photon coincidences at zero time delay alone are not sufficient and time-dependent data are necessary to clearly demonstrate a superradiant enhancement of the spontaneous radiative decay rate.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nanometers from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nm from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
In recent years, the study of quantum electrodynamics (QED) in light-matter interactions has discovered various interesting phenomenons that orient many applications. However, due to the ambient entanglement among photons and atoms, few-particle dynamics remains challenging to analyze precisely and limits the progress in several fields. In few-particle systems, different number of atoms interacting with the light field generates drastically different results, even when there is only a single photon involved in the system. The interference between individual atom’s spontaneous emission wavefunctions can cooperatively alter the effective atom-light coupling strength. Depending on the spatial distance between individual of atoms and the involved cavities in the interaction progresses, the collective spontaneous emission rate can alter drastically from superradiance, where the emission rate is enhanced to a high value proportional to the atom number, to subradiance, where the excited atom ensemble stays in a dark state with the light trapped forever. Superradiance provides a promising mechanism to create an ultra-strong light-matter coupling environment, which is an important ingredient for the design of ultra-fast optical devices, frequency comb generation and quantum mirrors. The dark state of subradiance, on the other hand, is essential for the quantum memory implementation. Also, nontrivial phenomenons also occur when multiple photons interacting with a single atom simultaneously. When a finite number of photons incidents on an atom, their scattering through an atom is highly nonlinear, and one special eigenstate component of such nonlinear process, namely photonic bound states, exhibits many interesting properties in nonlinear quantum optical systems. The photons in such state are strongly bunched with each other, as if a virtual attractive force is in effect. Also, the frequency of photons are anti-correlated so that their total frequency remains a constant value, no matter how arbitrary the frequency of any individual is. Thesefeatures benefit certain nonlinear quantum processes for quantum computing and quantum imaging. Specially for two-photon excitation imaging, the same-parity two-level fluorophore molecules suffers from extremely low excitation efficiencies due to the far off-resonant intermediate states. However, by replacing the current commonly used ultrashort laser pulse illuminations with two photon bound state photon pairs, namely photonic dimers, the efficiency can be enhanced to orders of magnitude higher. Such exceptionally high excitation efficiency can potentially bring the current in vivo deep brain imaging depth from millimeter level to several centimeters. To obtain a stable source of such photonic dimers, it is found that a laser structure with gain medium of two-photon emission materials is capable of generating the coherent state of photonic dimer and can serve as a promising light source for nonlinear quantum optical devices.
Matter coupled to light can emit photons. In the absence of an external field this process is known as spontaneous emission. The radiation properties depends in detail the nature of the emitter. In this thesis we consider a two level point-source emitter, and examine how the emission is affected by engineering the local environment. We begin by studying analytically how embedding an emitter in a multi-layer cylindrical structure with radius much smaller than the emission wavelength alters the intensity of the emitted light. We find that for carefully chosen metal-dielectric interfaces, the emission can be strongly enhanced by the plasmonic effect. With this intuition, we experimentally study an InGaN semiconductor quantum dot-in-wire structure as our two level emitter, and manipulate the local field environment by coupling to a lossy plasmonic cavity. We find that the strong enhancement of the field around the quantum dot due to the metal more than compensates for the non-radiative losses, leading to order-of-magnitude increases in the radiative spontaneous emission rate, as well as overall brightness. We then examine how the emission of light can be affected by other nearby emitters. The cooperative effects are strongly dependent on the dimension of the system which controls the electromagnetic mode overlap of the emitters. We present a unified formalism capturing how these cooperative effects change from one dimension to the next. Cooperative light scattering between emitters underpins collective effects such as super- and sub-radiance, and we numerically investigate how our previous results give rise to the key experimental signatures that can be used to identify those phenomena. Specifically, we study how the superadiant decay rate scales with the size of a 2-dimensional atomic cloud, and how cooperative effects between a small number of emitters alter the emission spectrum of strongly driven resonance fluorescence.