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Mutual Interaction Induced Multi-particle Physics in QED Systems – Cooperative Spontaneous Emission and Photonic Dimer Enhanced Two-photon Excitation

Zhou, Yao

Published Oct 11, 2021• 0 citations
Publisher

Abstract

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.

DOI
10.7936/mfb2-yd15

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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.
The interaction between light and matter has captivated physicists for centuries, from early studies of vision and refraction in ancient Greece to the development of quantum mechanics and quantum electrodynamics in the past century. While the response of a single quantum emitter to light is well understood, the radiative properties of an ensemble of closely spaced emitters are far more intricate. Coupling to a shared electromagnetic environment induces coherent and dissipative interactions between emitters, giving rise to a collective response that cannot be captured by treating them independently. In the regime of few excitations, the system hosts delocalized subradiant states, that is, coherent superpositions that are largely decoupled from the electromagnetic field and thus decay at suppressed rates. While this weak coupling makes subradiant states attractive for quantum technologies, it also renders them difficult to manipulate. At higher excitation densities, the intrinsic nonlinearity of emitters and the exponential growth of the Hilbert space make theoretical and numerical descriptions of the system and its dynamics increasingly challenging. This thesis explores two fundamental questions: How can subradiant and dark states be selectively accessed and harnessed for practical applications in quantum technologies? And how can interacting ensembles of quantum emitters be efficiently simulated to uncover their many-body physics? The first part of the thesis develops protocols for controlling and addressing dark states in free-space and waveguide-coupled atomic arrays, demonstrating their utility in quantum storage and the deterministic generation of entangled photonic states. Incorporating atomic motion, we further show that collective subradiant states can enhance cooling in dense atomic arrays, offering new avenues for controlling motional dynamics. In the second part, we introduce cumulant expansions of the equations of motion as a powerful tool to analytically and numerically investigate collective decay in the many-body regime. We first examine the collective decay of fully excited atomic arrays in free space, characterizing the onset and scaling of the superradiant burst across different geometries. In collaboration with experiments on ultracold erbium atoms in optical lattices, we provide the first direct observations of many-body collective effects in free-space ordered arrays, including early-time superradiant bursts, late-time subradiant tails, and the emergence of atomic correlations throughout the dynamics. Finally, we theoretically and numerically explore the transient formation of multi-excitation subradiant states, and demonstrate how the existence of multiple dissipation channels suppresses steady-state superradiance in extended arrays.
Coupling between quantum emitters and modes of light is foundational to studies of quantum systems. Coherent interactions between matter and light have greatly advanced the development of quantum technologies. When an ensemble of atoms interacts with light that is confined within a cavity---a resonator for photons---light also mediates atom-atom interactions, leading to collective phenomena that cannot be extrapolated from microscopic behaviors. Understanding how interactions among quantum particles lead to macroscopic phenomena, such as phase transitions and breaking of symmetries, remains a challenge in modern physics. In this dissertation, I present results addressing this challenge in the context of mesoscopic arrays of optical-tweezer-trapped atoms interfaced with a high-finesse optical cavity. In particular, the physics we investigate arises from the collective scattering of light. Utilizing the ability to place atoms with nanometer-scale precision, we engineer superradiant and subradiant states, where control over interference of the emission from multiple atoms leads to collectively enhanced or suppressed amounts of scattered light. Building on this work, we investigate the emergence of optomechanical self-organization, mediated by superradiance in the cavity electromagnetic field. By coupling atoms to the same cavity mode, the atoms exert forces on one another through the exchange of photons, leading them to autonomously order themselves spatially. We characterize mesoscopic fluctuations and their effect on symmetry-breaking dynamics associated with self-organization. Finally, we extend this framework to theoretically investigate how the phase of the atom-cavity coupling can be altered to generate higher symmetries. Our analysis reveals first-order phase transitions and instabilities induced by non-reciprocal forces. Altogether, this work establishes a path towards realizing mesoscopic systems of complex phases of matter in cavity quantum electrodynamics with unprecedented programmability.
Modification of spontaneous decay in space and time is a central topic of quantum physics. It has been predominantly investigated in the context of cavity quantum electrodynamics (QED), gaining new interest recently in the domain of nano-optics. Beyond cavity-QED, spontaneous emission may be modified also in free space due to correlations among the photon emitters, a phenomenon known as super- and sub-radiance. Correlations may stem either from direct interactions between the particles, from long-range exchange of photons, or by measuring single photons in a common mode. Yet, the genuine spatial spontaneous emission pattern of an atomic ensemble in an entangled quantum state has not been observed so far, due to the lack of ultra-fast cameras with high spatial resolution suited for recording single photons from single atoms. Preparing two trapped ions in free space in entangled Dicke states via photon detection, we study the resulting collective spontaneous emission patterns. Depending on the symmetry of the Dicke states, associated with the direction of detection of the first state-determining photon, we observe fundamentally different emission patterns for the subsequently scattered photon, including super- and sub-radiance. Our results demonstrate that the detection of a single photon can profoundly modify the collective emission of an atomic array, here represented by its most elementary building block of two atoms in free space.
Atom coherence in the cooperative interaction between the atoms and a single photon creates ultrafast spontaneous emission and ultrastrong intensity peaks, namely single-photon superradiance, which has attracted considerable research interest in the recent years. As the investigation for such a single-photon superradiance usually involves only quantum emitters, in this paper we present the cooperative atom-photon interaction in a system including whispering gallery mode resonators, which are one of the most essential components in nanophotonic devices. Here we both analytically and computationally show that the separated atoms on a resonator can obtain cooperative interaction, manifesting superradiant coupling strength, which results in the ultrafast spontaneous emission and ultrastrong intensity peaks. The conditions of such single-photon superradiance are called whispering gallery mode superradiance conditions. Furthermore, the atoms are proved to have cooperative interaction on a cascade of resonators by a renormalization approach.
Reduced abstract. This Thesis explores emergent cooperative phenomena in collective light-matter systems. We study ensembles of interacting quantum emitters coherently driven by a laser field and coupled to photonic structures, focusing on the hybrid description of emitters dressed by light. The interplay among quantum emitters, coherent driving, and photonic environments reveals a rich landscape of cooperative effects. While single-emitter dressing has been widely studied, we address collective phenomena in two non-identical emitters modelled as two-level systems. Strong interaction forms a dimer exhibiting superradiant and subradiant states, with two-photon resonances directly connecting ground and doubly excited states. This nonlinear process, central to the Thesis, enables new regimes of cooperative light-matter physics. Analytical studies show how interactions reshape observables such as emission intensity, photon statistics, and spectra, offering implications for quantum metrology. The sensitivity of two-photon processes to emitter distance and driving strength enables high-precision sensing and sub-wavelength imaging. Unexpectedly, we find that off-resonant virtual states may gain population through dissipation, redefining their role in open systems. To capture this, we develop a hierarchical adiabatic elimination method for metastable dynamics. We also analyze entanglement in emitters coupled to a lossy cavity, identifying five mechanisms, including the frequency-resolved Purcell effect introduced here. This selective enhancement stabilizes cooperative states and enables scalable entanglement. Our models, tailored to solid-state platforms such as quantum dots and molecular aggregates, address challenges like inhomogeneous broadening and decoherence, demonstrating the feasibility of harnessing cooperative light-matter effects for quantum technologies.
When atoms are coupled to a common electromagnetic environment, the exchange of photons through dipole-dipole interactions leads to the emergence of cooperative effects. As a particular example, superradiance arises from spontaneous emission when this exchange leads to constructive interference of the emitted photons. Here, we introduce an integrated method for studying cooperative radiation in many-body systems. This method, which allows to study extended systems with arbitrarily large number of particles, can be formulated by an effective, nonlinear, two-atom master equation that describes the dynamics using a closed form which treats single- and many-body terms on an equal footing. We apply this method to a homogeneous gas of initially inverted two-level atoms, and demonstrate the appearance of both superradiance and subradiance, identifying a many-body coherence term as the source of these cooperative effects. We describe the many-body induced broadening -- which is analytically found to scale with the optical depth of the system -- and light shifts, and distinguish spontaneous effects from induced ones. In addition, we theoretically predict the time-dependence of subradiance, and the phase change of the radiated field during the cooperative decay.