We provide a framework to theoretically describe long-range energy transfer in single and twisted two-dimensional hyperbolic slabs. We demonstrate that phonon polaritons (PhPs, quantum superpositions of photons and lattice vibrations in polar dielectrics) can mediate and enhance room-temperature energy transfer at ranges far exceeding those of conventional mid-infrared (MIR) platforms, and with extreme directionality. This is because the dipole-dipole interaction potential energy diverges along the asymptotes of the real-space hyperbolic opening angle. Our findings allow us to extend classical and quantum interactions between dipoles, typically strictly confined to the near-field, beyond several free-space MIR wavelengths. We use $α$-MoO$_3$ as a representative material, but this mechanism is not limited to the MIR: it is general to anisotropic media across the whole electromagnetic spectrum.
We provide a framework to theoretically describe long-range energy transfer in single and twisted two-dimensional hyperbolic slabs. We demonstrate that phonon polaritons (PhPs, quantum superpositions of photons and lattice vibrations in polar dielectrics) can mediate and enhance room-temperature energy transfer at ranges far exceeding those of conventional mid-infrared (MIR) platforms, and with extreme directionality. This is because the dipole-dipole interaction potential energy diverges along the asymptotes of the real-space hyperbolic opening angle. Our findings allow us to extend classical and quantum interactions between dipoles, typically strictly confined to the near-field, beyond several free-space MIR wavelengths. We use α-MoO3 as a representative material, but this mechanism is not limited to the MIR: it is general to anisotropic media across the whole electromagnetic spectrum.
Hyperbolic media enable ultra-strong light-matter interactions through their extreme field localization and small mode volumes, but low-loss realizations are fundamentally limited to the mid-infrared, owing to the long lifetimes of optical phonons in high-quality crystals. Here we show that bright emitters operating at visible or near-infrared frequencies can be used to generate radiation in this regime by inducing mid-infrared population dynamics, thereby creating a source in the hyperbolic frequency band without a corresponding dipole transition. We demonstrate that even a source with vanishing dipole and higher multipole moments - strictly non-radiating in any isotropic medium - becomes radiatively active in a hyperbolic environment. This enables visible and near-infrared control of light-matter interactions in polaritonic hyperbolic materials, establishing a new low-loss solid-state quantum optics platform.
Hyperbolic phonon polaritons (HPPs) in hexagonal boron nitride (hBN) confine mid-infrared light to deep-subwavelength scales and may offer a powerful route to strong light-matter interactions. Generation and control of HPPs are typically accessed using classical near-field probes, which limits experiments at the quantum level.A complementary frontier in hBN research focuses on color centers: bright, stable, atomically localized emitters that have rapidly emerged as a promising platform for solid-state quantum optics. Here we establish a key connection between these two directions by developing a cavity-QED framework in which a single hBN color center serves as a quantum source of HPPs. We quantify the emitter-HPP interaction and analyze two generation schemes. The first is spontaneous emission into the phonon sideband, which can produce single-HPP events and, in ultrathin slabs, becomes single-mode with an enhanced decay rate. The second is a stimulated Raman process that provides frequency selectivity, tunable conversion rate, and narrowband excitation. This drive launches spatially confined, ray-like HPPs that propagate over micrometer distances. We also outline a two-emitter correlation measurement that can directly test the single-polariton character of these emissions. By connecting color-center quantum optics with hyperbolic polaritonics, our approach enables quantum emitters to act as on-chip quantum sources and controls for HPPs, while HPPs provide long-range channels that couple spatially separated emitters. Together, these capabilities point to a new direction for mid-infrared photonic experiments that unite strong coupling, spectral selectivity, and spatial reach within a single material system.
Quantum properties like coherence and entanglement can lead to enhanced performance characteristics in a wide range of applications including quantum computation, quantum memory storage, optical sensing, and energy harvesting. Entanglement is very sensitive to static and dynamical disorder. Similarly, the generation of highly-entangled states requires strong coupling or strong driving fields. Satisfying all of these requirements is generally quite difficult. In the first part of this thesis, we present an approach to overcome these limitations through the use of exotic light-matter states in hyperbolic media which provide a new approach to control quantum correlations and interatomic interactions. We reveal a class of excited-state, long-range interactions, referred to as Super-Coulombic interactions that are singular along a material-dependent resonance angle. In practical systems, the Super-Coulombic interaction achieves dipole-dipole coupling that is orders of magnitude larger than conventional approaches, while also occurring across a large frequency bandwidth making it robust to static energy-level disorder. This unique hyperbolic response is not only naturally occurring, found in materials like h-BN, BiTe2, BiSe2, and mono-layered black phosphorus, but can also be designed with artificial nanostructured materials (metamaterials) to create the desired hyperbolic dispersion across different parts of the electromagnetic spectrum. Our theoretical prediction motivated an intense search for the effect and was confirmed by an experimental demonstration at room temperature. To obtain agreement with experimental results, we present a rigorous theoretical framework that takes into account ensemble effects, finite-sized effects, and dimensional effects that arise from confined geometries ultimately modifying the Super-Coulombic spatial scaling law. In the second part of this thesis, we solve an outstanding theoretical problem dealing with the control of resonance energy transfer in nanophotonic environments in both the incoherent and coherent coupling limits. Resonance energy transfer is a fundamental process that is the subject of intense research across all sciences. For example, in chemistry for drug delivery and chemical monitoring, in engineering for photovoltatic and up-conversion devices, and in biology for exciton transport within photosynthetic complexes. First, we consider the disordered and weak coupling limit of resonance energy transfer often encountered in chemistry. We propose new design principles for enhancing and suppressing the energy transfer rate and efficiency quantitatively captured by a simple image dipole model. Our theory explains a wide range of experimental results which have been the subject of an ongoing debate for the past 15 years. Second, we present our recent result aimed at understanding the fundamental role of entanglement and quantum coherence in resonance energy transfer. To uncover the role of these effects, we develop a unified theory of energy transfer valid from the incoherent to quantum coherent coupling regimes. Ultimately, our theory reveals a fundamental bound ηmax = γa for energy transfer efficiency arising from γd+γa the spontaneous emission rates γd and γa of the donor and acceptor. This bound provides an upper limit to the efficiency of energy transfer regardless of quantum coherence or entanglement, suggesting new design principles for achieving near-unity energy transfer efficiency in coherent systems. The result has important implications for the two-chromophore model found in photosynthetic complexes and paves the way for nanophotonic analogues of efficiency-enhancing environments mimicking biological photosynthetic systems.
) between closely spaced atoms and molecules are related to real photon and virtual photon exchange between them and decrease in the near field connected with the characteristic Coulombic dipole field law. The control and modification of this marked scaling with distance have become a long-standing theme in quantum engineering since dipole-dipole interactions govern Van der Waals forces, collective Lamb shifts, atom blockade effects, and Förster resonance energy transfer. We show that metamaterials can fundamentally modify these interactions despite large physical separation between interacting quantum emitters. We demonstrate a two orders of magnitude increase in the near-field resonant dipole-dipole interactions at intermediate field distances (10 times the near field) and observe the distance scaling law consistent with a super-Coulombic interaction theory curtailed only by absorption and finite size effects of the metamaterial constituents. We develop a first-principles numerical approach of many-body dipole-dipole interactions in metamaterials to confirm our theoretical predictions and experimental observations. In marked distinction to existing approaches of engineering radiative interactions, our work paves the way for controlling long-range dipole-dipole interactions using hyperbolic metamaterials and natural hyperbolic two-dimensional materials.
The rate of energy transfer in donor-acceptor systems can be manipulated via the common interaction with the confined electromagnetic modes of a micro-cavity. We analyze the competition between the near-field short range dipole-dipole energy exchange processes and the cavity mediated long-range interactions in a simplified model consisting of effective two-level quantum emitters that could be relevant for molecules in experiments under cryogenic conditions. We find that free-space collective incoherent interactions, typically associated with sub- and superradiance, can modify the traditional resonant energy transfer scaling with distance. The same holds true for cavity-mediated collective incoherent interactions in a weak-coupling but strong-cooperativity regime. In the strong coupling regime, we elucidate the effect of pumping into cavity polaritons and analytically identify an optimal energy flow regime characterized by equal donor/acceptor Hopfield coefficients in the middle polariton. Finally we quantify the build-up of quantum correlations in the donor-acceptor system via the two-qubit concurrence as a measure of entanglement.
The rate of energy transfer in donor-acceptor systems can be manipulated via the common interaction with the confined electromagnetic modes of a micro-cavity. We analyze the competition between the near-field short range dipole-dipole energy exchange processes and the cavity mediated long-range interactions in a simplified model consisting of effective two-level quantum emitters that could be relevant for molecules in experiments under cryogenic conditions. We find that free-space collective incoherent interactions, typically associated with sub-and superradiance, can modify the traditional resonant energy transfer scaling with distance. The same holds true for cavity-mediated collective incoherent interactions in a weak-coupling but strong-cooperativity regime. In the strong coupling regime, we elucidate the effect of pumping into cavity polaritons and analytically identify an optimal energy flow regime characterized by equal donor/acceptor Hopfield coefficients in the middle polariton. Finally we quantify the build-up of quantum correlations in the donor-acceptor system via the two-qubit concurrence as a measure of entanglement.