Regime Of Light-matter Interaction Research Articles

Molecular Energy Transfer under the Strong Light-Matter Interaction Regime.

Research into strong light-matter interactions continues to fascinate, being spurred on by unforeseen and often spectacular experimental observations. Properties that were considered to depend exclusively on material composition have been found to be drastically altered when a material is placed inside a resonant optical cavity. This is nowhere more the case than in the field of intermolecular energy transfer, where polaritonic states formed as a result of strong light-matter interactions have been shown to promote energy transfer over distances vastly exceeding conventional limits. In this review, we provide the reader with a succinct account of the fundamental concepts of intermolecular energy transfer, and how they are modified by strong light-matter interactions. We also summarize recent experimental advances in the area, including in optoelectronic device contexts, and highlight both the potential and challenges that remain in this exciting field of research going forward.

Tunable virtual gain in resonantly absorbing media

Virtual gain refers to the simulation of real light amplification using radiation with exponentially decaying amplitude, so that its complex frequency corresponds to the scattering pole. We theoretically study virtual gain in a two-level resonant medium for different regimes of light-matter interaction depending on the radiation intensity. We show that virtual gain at the pole can be most clearly observed for low intensities, when the medium is absorbing, in contrast to the saturated medium at high intensities. The efficiency of virtual gain can be tuned with the light intensity and can be controlled dynamically through the population inversion of the medium. Our results show that resonantly absorbing media paradoxically mimics gain-like response, which admit a number of related phenomena and methods to mold both optical signals and material properties without relying on instability-prone gain media.

Many-Body Correlations and Exciton Complexes in CsPbBr3 Quantum Dots.

All-inorganic lead-halide perovskite (LHP) (CsPbX3 , X=Cl, Br, I) quantum dots (QDs) have emerged as a competitive platform for classical light-emitting devices (in the weak light-matter interaction regime, e.g., LEDs and laser), as well as for devices exploiting strong light-matter interaction at room temperature. Many-body interactions and quantum correlations among photogenerated exciton complexes play an essential role, for example, by determining the laser threshold, the overall brightness of LEDs, and the single-photon purity in quantum light sources. Here, by combining cryogenic single-QD photoluminescence spectroscopy with configuration-interaction (CI) calculations, the size-dependent trion and biexciton binding energies are addressed. Trion binding energies increase from 7to 17meV for QD sizes decreasing from 30to 9nm, while the biexciton binding energies increase from 15to 30meV, respectively. CI calculations quantitatively corroborate the experimental results and suggest that the effective dielectric constant for biexcitons slightly deviates from the one of the single excitons, potentially as a result of coupling to the lattice in the multiexciton regime. The findings here provide a deep insight into the multiexciton properties in all-inorganic LHP QDs, essential for classical and quantum optoelectronic devices.

Radiative properties of an artificial atom coupled to a Josephson-junction array

We study the radiative properties -- the Lamb shift, Purcell decay rate and the spontaneous emission dynamics -- of an artificial atom coupled to a long, multimode cavity formed by an array of Josephson junctions. Introducing a tunable coupling element between the atom and the array, we demonstrate that such a system can exhibit a crossover from a perturbative to non-perturbative regime of light-matter interaction as one strengthens the coupling between the atom and the Josephson junction array (JJA). As a consequence, the concept of spontaneous emission as the occupation of the local atomic site being governed by a single complex-valued exponent breaks down. This breakdown, we show, can be interpreted in terms of formation of hybrid atom-resonator modes with radiative losses that are non-trivially related to the effective coupling between individual modes. We develop a singular function expansion approach for the description of the open quantum system dynamics in such a multimode non-perturbative regime. This modal framework generalizes the normal mode description of quantum fields in a finite volume, incorporating exact radiative losses and incident quantum noise at the delimiting surface. Our results are pertinent to recent experiments with Josephson atoms coupled to high impedance Josephson junction arrays.

Nonlocal Exciton-Photon Interactions in Hybrid High-Q Beam Nanocavities with Encapsulated MoS_{2} Monolayers.

Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of nonlocal interactions of "free" trions in pristine hBN/MoS_{2}/hBN heterostructures coupled to single mode (Q>10^{4}) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stems from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS_{2} monolayer. We observe a nonmonotonic temperature dependence of the cavity-trion interaction strength, consistent with the nonlocal light-matter interactions in which the extent of the center-of-mass (c.m.) wave function is comparable to the cavity mode volume in space. Our approach can be generalized to other optically active 2D materials, opening the way toward harnessing novel light-matter interaction regimes for applications in quantum photonics.

A Theoretical Perspective on Molecular Polaritonics.

In the past decade, much theoretical research has focused on studying the strong coupling between organic molecules (or quantum emitters, in general) and light modes. The description and prediction of polaritonic phenomena emerging in this light–matter interaction regime have proven to be difficult tasks. The challenge originates from the enormous number of degrees of freedom that need to be taken into account, both in the organic molecules and in their photonic environment. On one hand, the accurate treatment of the vibrational spectrum of the former is key, and simplified quantum models are not valid in many cases. On the other hand, most photonic setups have complex geometric and material characteristics, with the result that photon fields corresponding to more than just a single electromagnetic mode contribute to the light–matter interaction in these platforms. Moreover, loss and dissipation, in the form of absorption or radiation, must also be included in the theoretical description of polaritons. Here, we review and offer our own perspective on some of the work recently done in the modeling of interacting molecular and optical states with increasing complexity.

Regimes of cavity QED under incoherent excitation: From weak to deep strong coupling

The prototypical system constituted by a two-level atom interacting with a quantized single-mode electromagnetic field is described by the quantum Rabi model (QRM). The QRM is potentially valid at any light-matter interaction regime, ranging from the weak (where the decay rates exceeds the coupling rate) to the deep strong coupling (where the interaction rate exceeds the bare transition frequencies of the subsystems). However, when reaching the ultrastrong coupling regime, several theoretical issues may prevent the correct description of the observable dynamics of such a system: (i) the standard quantum optics master equation fails to correctly describe the interaction of this system with the reservoirs; (ii) the correct output photon rate is no longer proportional to the intracavity photon number; and (iii) they appear to violate gauge invariance. Here, we study the photon flux emission rate of this system under the incoherent excitation of the two-level atom for any light-matter interaction strength and consider different effective temperatures. The dependence of the emission spectra on the coupling strength is the result of the interplay between energy levels, matrix elements of the observables, and the density of states of the reservoirs. Within this approach, we also study the occurrence of light-matter decoupling in the deep strong-coupling regime and show how all of the obtained results are gauge invariant.

Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity: A First-Principles Study.

Ultrastrong coupling (USC) is a distinct regime of light-matter interaction in which the coupling strength is comparable to the resonance energy of the cavity or emitter. In the USC regime, common approximations to quantum optical Hamiltonians, such as the rotating wave approximation, break down as the ground state of the coupled system gains photonic character due to admixing of vacuum states with higher excited states, leading to ground-state energy changes. USC is usually achieved by collective coherent coupling of many quantum emitters to a single mode cavity, whereas USC with a single molecule remains challenging. Here, we show by time-dependent density functional theory (TDDFT) calculations that a single organic molecule can reach USC with a plasmonic dimer, consisting of a few hundred atoms. In this context, we discuss the capacity of TDDFT to represent strong coupling and its connection to the quantum optical Hamiltonian. We find that USC leads to appreciable ground-state energy modifications accounting for a non-negligible part of the total interaction energy, comparable to kBT at room temperature.

Trends in angle-resolved molecular photoelectron spectroscopy.

The field of angle-resolved molecular photoelectron spectroscopy is reviewed, with emphasis on foundations and most recent applications in different regimes of light-matter interaction. The basic formalism underlying one-photon electron angular distributions is presented, from the primary molecular frame (MF) photoemission i.e. emission from fully oriented molecules to laboratory frame (LF) observables produced from randomly oriented targets, extensions to multiphoton and strong field processes being briefly described, followed by a survey of current quantum mechanical computational approaches. The description of experimental developments is focused on the advancements in two major instrumentation fields for angle-resolved PES of molecules in the last two decades, namely charged-particle imaging spectrometers and adiabatically or impulsively laser-induced molecular alignment, together with their interplay with the remarkable characteristics achieved nowadays by the ionizing light sources and the challenging control of complex molecules in the gas phase. Aspects and applications of LF angular observables from unoriented targets are presented, with contemporary applications, especially as probes of the target electronic structure, including higher angular observables, in particular photoelectron circular dichroism (PECD) from chiral molecules, which is confirmed as a powerful chiral technique, and higher terms arising from multiphoton or non-dipole terms. Molecular frame photoelectron angular distributions (MFPADs), which stand out as the most complete observables of molecular photoionization stereodynamics in different excitation regimes, now broadly extended to characterize molecular structure and dynamics, are then discussed stemming from fully oriented molecules tackled by electron-ion momentum coincidence techniques, or from laser aligned samples. Finally, novel developments and challenging perspectives, notably the implementation of PAD in time-resolved schemes at ultrashort time scales, high energy, and high intensity regimes are drawn.

Cavity exciton polaritons in two-dimensional semiconductors from first principles

Two-dimensional (2D) semiconducting microcavity, where exciton-polaritons can be formed, constitues a promising setup for exploring and manipulating various regimes of light-matter interaction. Here, the coupling between 2D excitons and metallic cavity photons is studied by using first-principles propagator technique. The strength of exciton-photon coupling is characterised by its Rabi splitting to two exciton-polaritons, which can be tuned by cavity thickness. Maximum splitting of 128 meV is achieved in phosporene cavity, while remarkable value of about 440 meV is predicted in monolayer hBN device. The obtained Rabi splittings in WS$_2$ microcavity are in excellent agreement with the recent experiments. Present methodology can aid in predicting and proposing potential setups for trapping robust 2D exciton-polariton condensates.

Polarization-dependent mode coupling in hyperbolic nanospheres

Abstract Hyperbolic materials offer much wider freedom in designing optical properties of nanostructures than ones with isotropic and elliptical dispersion, both metallic or dielectric. Here, we present a detailed theoretical and numerical study on the unique optical properties of spherical nanoantennas composed of such materials. Hyperbolic nanospheres exhibit a rich modal structure that, depending on the polarization and direction of incident light, can exhibit either a full plasmonic-like response with multiple electric resonances, a single, dominant electric dipole or one with mixed magnetic and electric modes with an atypical reversed modal order. We derive conditions for observing these resonances in the dipolar approximation and offer insight into how the modal response evolves with the size, material composition, and illumination. Specifically, the origin of the magnetic dipole mode lies in the hyperbolic dispersion and its existence is determined by two diagonal permittivity components of different sign. Our analysis shows that the origin of this unusual behavior stems from complex coupling between electric and magnetic multipoles, which leads to very strong scattering or absorbing modes. These observations assert that hyperbolic nanoantennas offer a promising route towards novel light–matter interaction regimes.

Circuit quantum electrodynamics

Quantum mechanical effects at the macroscopic level were first explored in Josephson junction-based superconducting circuits in the 1980's. In the last twenty years, the emergence of quantum information science has intensified research toward using these circuits as qubits in quantum information processors. The realization that superconducting qubits can be made to strongly and controllably interact with microwave photons, the quantized electromagnetic fields stored in superconducting circuits, led to the creation of the field of circuit quantum electrodynamics (QED), the topic of this review. While atomic cavity QED inspired many of the early developments of circuit QED, the latter has now become an independent and thriving field of research in its own right. Circuit QED allows the study and control of light-matter interaction at the quantum level in unprecedented detail. It also plays an essential role in all current approaches to quantum information processing with superconducting circuits. In addition, circuit QED enables the study of hybrid quantum systems interacting with microwave photons. Here, we review the coherent coupling of superconducting qubits to microwave photons in high-quality oscillators focussing on the physics of the Jaynes-Cummings model, its dispersive limit, and the different regimes of light-matter interaction in this system. We discuss coupling of superconducting circuits to their environment, which is necessary for coherent control and measurements in circuit QED, but which also invariably leads to decoherence. Dispersive qubit readout, a central ingredient in almost all circuit QED experiments, is also described. Following an introduction to these fundamental concepts that are at the heart of circuit QED, we discuss important use cases of these ideas in quantum information processing and in quantum optics.

Nonlinear one-way edge-mode interactions for frequency mixing in topological photonic crystals

Topological photonics aims to utilize topological photonic bands and corresponding edge modes to implement robust light manipulation, which can be readily achieved in the linear regime of light-matter interaction. Importantly, unlike solid state physics, the common test bed for new ideas in topological physics, topological photonics provide an ideal platform to study wave mixing and other nonlinear interactions. These are well-known topics in classical nonlinear optics but largely unexplored in the context of topological photonics. Here, we investigate nonlinear interactions of one-way edge-modes in frequency mixing processes in topological photonic crystals. We present a detailed analysis of the band topology of two-dimensional photonic crystals with hexagonal symmetry and demonstrate that nonlinear optical processes, such as second- and third-harmonic generation can be conveniently implemented via one-way edge modes of this setup. Moreover, we demonstrate that more exotic phenomena, such as slow-light enhancement of nonlinear interactions and harmonic generation upon interaction of backward-propagating (left-handed) edge modes can also be realized. Our work opens up new avenues towards topology-protected frequency mixing processes in photonics.

Ultrastrong coupling regimes of light-matter interaction

Recent experiments have demonstrated that light and matter can mix together to an extreme degree, and previously uncharted regimes of light-matter interactions are currently being explored in a variety of settings. The so-called ultrastrong coupling (USC) regime is established when the light-matter interaction energy is a comparable fraction of the bare frequencies of the uncoupled systems. Furthermore, when the interaction strengths become larger than the bare frequencies, the deep-strong coupling (DSC) regime emerges. This article reviews advances in the field of the USC and DSC regimes, in particular, for light modes confined in cavities interacting with two-level systems. An overview is first provided on the theoretical progress since the origins from the semiclassical Rabi model until recent developments of the quantum Rabi model. Next, several key experimental results from a variety of quantum platforms are described, including superconducting circuits, semiconductor quantum wells, and other hybrid quantum systems. Finally, anticipated applications are highlighted utilizing USC and DSC regimes, including novel quantum optical phenomena, quantum simulation, and quantum computation.

Resolution of gauge ambiguities in ultrastrong-coupling cavity quantum electrodynamics

Gauge invariance is the cornerstone of modern quantum field theory. Recently, it has been shown that the quantum Rabi model, describing the dipolar coupling between a two-level atom and a quantized electromagnetic field, violates this principle. This widely used model describes a plethora of quantum systems and physical processes under different interaction regimes. In the ultrastrong coupling regime, it provides predictions which drastically depend on the chosen gauge. This failure is attributed to the finite-level truncation of the matter system. We show that a careful application of the gauge principle is able to restore gauge invariance even for extreme light-matter interaction regimes. The resulting quantum Rabi Hamiltonian in the Coulomb gauge differs significantly from the standard model and provides the same physical results obtained by using the dipole gauge. It contains field operators to all orders that cannot be neglected when the coupling strength is high. These results shed light on subtleties of gauge invariance in nonperturbative and extreme interaction regimes, which are now experimentally accessible, and solve all the long-lasting controversies arising from gauge ambiguities in the quantum Rabi and Dicke models.

Transition metal dichalcogenide nanodisks as high-index dielectric Mie nanoresonators

Monolayer transition metal dichalcogenides (TMDCs) have recently been proposed as an excitonic platform for advanced optical and electronic functionalities1-3. However, in spite of intense research efforts, it has not been widely appreciated that TMDCs also possess a high refractive index4,5. This characteristic opens up the possibility to utilize them to construct resonant nanoantennas based on subwavelength geometrical modes6,7. Here, we show that nanodisks, fabricated from exfoliated multilayer WS2, support distinct Mie resonances and anapole states8 that can be tuned in wavelength over the visible and near-infrared range by varying the nanodisk size and aspect ratio. As a proof of concept, we demonstrate a novel regime of light-matter interaction-anapole-exciton polaritons-which we realize within a single WS2 nanodisk. We argue that the TMDC material anisotropy and the presence of excitons enrich traditional nanophotonics approaches based on conventional high-index materials and/or plasmonics.

Second harmonic generation in graphene dressed by a strong terahertz field

We observe enhanced second-harmonic generation in monolayer graphene in the presence of an ultra-strong terahertz field pulse with a peak amplitude of 250 kV/cm. This is a strongly nonperturbative regime of light-matter interaction in which particles get accelerated to energies exceeding the initial Fermi energy of 0.2 eV over a timescale of a few femtoseconds. The second-harmonic current is generated as electrons drift through the region of momenta corresponding to interband transition resonance at an optical frequency. The resulting strongly asymmetric distortion of carrier distribution in momentum space gives rise to an enhanced electric-dipole nonlinear response at the second harmonic. We develop an approximate analytic theory of this effect which accurately predicts observed intensity and polarization of the second-harmonic signal.

Strong coupling of a two-dimensional electron ensemble to a single-mode cavity resonator

We investigate the regime of strong coupling of an ensemble of two-dimensional electrons to a single-mode cavity resonator. In particular, we realized such a regime of light-matter interaction by coupling the cyclotron motion of a collection of electrons on the surface of liquid helium to the microwave field in a semi-confocal Fabry-Perot resonator. For the co-rotating component of the microwave field, the strong coupling is pronouncedly manifested by the normal-mode splitting in the spectrum of coupled field-particle motion. We present a complete description of this phenomenon based on classical electrodynamics, as well as show that the full quantum treatment of this problem results in mean-value equations of motion that are equivalent to our classical result. For the counter-rotating component of the microwave field, we observe a strong resonance when the microwave frequency is close to both the cyclotron and cavity frequencies. We show that this surprising effect, which is not expected to occur under the rotating-wave approximation, results from the mixing between two polarization components of the microwave field in our cavity.

Light-Emitting Metasurfaces: Simultaneous Control of Spontaneous Emission and Far-Field Radiation.

Light-emitting sources and devices permeate every aspect of our lives and are used in lighting, communications, transportation, computing, and medicine. Advances in multifunctional and "smart lighting" would require revolutionary concepts in the control of emission spectra and directionality. Such control might be possible with new schemes and regimes of light-matter interaction paired with developments in light-emitting materials. Here we show that all-dielectric metasurfaces made from III-V semiconductors with embedded emitters have the potential to provide revolutionary lighting concepts and devices, with new functionality that goes far beyond what is available in existing technologies. Specifically, we use Mie-resonant metasurfaces made from semiconductor heterostructures containing epitaxial quantum dots. By controlling the symmetry of the resonant modes, their overlap with the emission spectra, and other structural parameters, we can enhance the brightness by 2 orders of magnitude, as well as reduce its far-field divergence significantly.

Near-Ground-State Cooling of Atoms Optically Trapped 300 nm Away from a Hot Surface

Laser-cooled atoms coupled to nanophotonic structures constitute a powerful research platform for the exploration of new regimes of light-matter interaction. While the initialization of the atomic internal degrees of freedom in these systems has been achieved, a full preparation of the atomic quantum state also requires controlling the center of mass motion of the atoms at the quantum level. Obtaining such control is not straightforward, due to the close vicinity of the atoms to the photonic system that is at ambient temperature. Here, we demonstrate cooling of individual neutral Cesium atoms, that are optically interfaced with light in an optical nanofiber, preparing them close to their three-dimensional motional ground state. The atoms are localized less than 300nm away from the hot fiber surface. Ground-state preparation is achieved by performing degenerate Raman cooling, and the atomic temperature is inferred from the analysis of heterodyne fluorescence spectroscopy signals. Our cooling method can be implemented either with externally applied or guided light fields. Moreover, it relies on polarization gradients which naturally occur for strongly confined guided optical fields. Thus, this method can be implemented in any trap based on nanophotonic structures. Our results provide an ideal starting point for the study of novel effects such as light-induced self-organization, the measurement of novel optical forces, and the investigation of heat transfer at the nanoscale using quantum probes.