Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons.

Controlling quantum materials with light is of fundamental and technological importance. By utilizing the strong coupling of light and matter in optical cavities1-3, recent studies were able to modify some of their most defining features4-6. Here we study the magneto-optical properties of a van der Waals magnet that supports strong coupling of photons and excitons even in the absence of external cavity mirrors. In this material-the layered magnetic semiconductor CrSBr-emergent light-matter hybrids called polaritons are shown to substantially increase the spectral bandwidth of correlations between the magnetic, electronic and optical properties, enabling largely tunable optical responses to applied magnetic fields and magnons. Our results highlight the importance of exciton-photon self-hybridization in van der Waals magnets and motivate novel directions for the manipulation of quantum material properties by strong light-matter coupling.

Electroluminescence as a Probe of Strong Exciton-Plasmon Coupling in Few-Layer WSe2.

The manipulation of coupled quantum excitations is of fundamental importance in realizing novel photonic and optoelectronic devices. We use electroluminescence to probe plasmon-exciton coupling in hybrid structures consisting of a nanoscale plasmonic tunnel junction and few-layer two-dimensional transition-metal dichalcogenide transferred onto the junction. The resulting hybrid states act as a novel dielectric environment that affects the radiative recombination of hot carriers in the plasmonic nanostructure. We determine the plexcitonic spectrum from the electroluminescence and find Rabi splittings exceeding 50 meV in the strong coupling regime. Our experimental findings are supported by electromagnetic simulations that enable us to explore systematically and in detail the emergence of plexciton polaritons as well as the polarization characteristics of their far-field emission. Electroluminescence modulated by plexciton coupling provides potential applications for engineering compact photonic devices with tunable optical and electrical properties.

Lindblad Master Equation Capable of Describing Hybrid Quantum Systems in the Ultrastrong Coupling Regime.

Despite significant theoretical efforts devoted to studying the interaction between quantized light modes and matter, the so-called ultrastrong coupling regime still presents significant challenges for theoretical treatments and prevents the use of many common approximations. Here we demonstrate an approach that can describe the dynamics of hybrid quantum systems in any regime of interaction for an arbitrary electromagnetic (EM) environment. We extend a previous method developed for few-mode quantization of arbitrary systems to the case of ultrastrong light-matter coupling, and show that even such systems can be treated using a Lindblad master equation where decay operators act only on the photonic modes by ensuring that the effective spectral density of the EM environment is sufficiently suppressed at negative frequencies. We demonstrate the validity of our framework and show that it outperforms current state-of-the-art master equations for a simple model system, and then study a realistic nanoplasmonic setup where existing approaches cannot be applied.

Plexcitonic Quantum Light Emission from Nanoparticle-on-Mirror Cavities.

We investigate the quantum-optical properties of the light emitted by a nanoparticle-on-mirror cavity filled with a single quantum emitter. Inspired by recent experiments, we model a dark-field setup and explore the photon statistics of the scattered light under grazing laser illumination. Exploiting analytical solutions to Maxwell's equations, we quantize the nanophotonic cavity fields and describe the formation of plasmon-exciton polaritons (or plexcitons) in the system. This way, we reveal that the rich plasmonic spectrum of the nanocavity offers unexplored mechanisms for nonclassical light generation that are more efficient than the resonant interaction between the emitter natural transition and the brightest optical mode. Specifically, we find three different sample configurations in which strongly antibunched light is produced. Finally, we illustrate the power of our approach by showing that the introduction of a second emitter in the platform can enhance photon correlations further.

Artificial Metaphotonics Born Naturally in Two Dimensions.

Recently, two rich and exciting research fields, layered two-dimensional (2D) materials and metamaterials, have started overlapping. Metamaterials are artificial, engineered materials with broad metaphotonic prospects such as negative refraction, perfect lensing, subwavelength imaging, and cloaking. The possibility of achieving metaphotonic properties using metamaterials based on layered 2D materials has been extensively exploited. Because they are highly tunable and adjustable with the ease of micro- and nanofabrication, 2D materials exhibit diverse optical properties such as natural negative refraction, natural anisotropic behavior, and even hyperbolic dispersion. A combination of 2D materials with conventional metamaterials promises a variety of prospective applications. In this review, we illustrate how the concept of metamaterials and their associated metaphotonic capabilities are naturally born in 2D materials. The multifunctionality of 2D materials may enable the manufacture of novel optical devices that work in a broad frequency range, from visible to terahertz, with particularly low loss, high speed, gated tunability, and miniaturized sizes. This new area of research links the fields of photonics, optoelectronics, and plasmonics with that of metamaterials and may provide insights to future innovations for 2D-material-inspired metaphotonic devices.

Few-Mode Field Quantization of Arbitrary Electromagnetic Spectral Densities.

We develop a framework that provides a few-mode master equation description of the interaction between a single quantum emitter and an arbitrary electromagnetic environment. The field quantization requires only the fitting of the spectral density, obtained through classical electromagnetic simulations, to a model system involving a small number of lossy and interacting modes. We illustrate the power and validity of our approach by describing the population and electric field spatial dynamics in the spontaneous decay of an emitter placed in a complex hybrid plasmonic-photonic structure.

Radiative heat transfer in the extreme near field.

Radiative transfer of energy at the nanometre length scale is of great importance to a variety of technologies including heat-assisted magnetic recording, near-field thermophotovoltaics and lithography. Although experimental advances have enabled elucidation of near-field radiative heat transfer in gaps as small as 20-30 nanometres (refs 4-6), quantitative analysis in the extreme near field (less than 10 nanometres) has been greatly limited by experimental challenges. Moreover, the results of pioneering measurements differed from theoretical predictions by orders of magnitude. Here we use custom-fabricated scanning probes with embedded thermocouples, in conjunction with new microdevices capable of periodic temperature modulation, to measure radiative heat transfer down to gaps as small as two nanometres. For our experiments we deposited suitably chosen metal or dielectric layers on the scanning probes and microdevices, enabling direct study of extreme near-field radiation between silica-silica, silicon nitride-silicon nitride and gold-gold surfaces to reveal marked, gap-size-dependent enhancements of radiative heat transfer. Furthermore, our state-of-the-art calculations of radiative heat transfer, performed within the theoretical framework of fluctuational electrodynamics, are in excellent agreement with our experimental results, providing unambiguous evidence that confirms the validity of this theory for modelling radiative heat transfer in gaps as small as a few nanometres. This work lays the foundations required for the rational design of novel technologies that leverage nanoscale radiative heat transfer.

Reconfigurable Photon Sources Based on Quantum Plexcitonic Systems.

A single photon in a strongly nonlinear cavity is able to block the transmission of a second photon, thereby converting incident coherent light into antibunched light, which is known as the photon blockade effect. Photon antipairing, where only the entry of two photons is blocked and the emission of bunches of three or more photons is allowed, is based on an unconventional photon blockade mechanism due to destructive interference of two distinct excitation pathways. We propose quantum plexcitonic systems with moderate nonlinearity to generate both antibunched and antipaired photons. The proposed plexcitonic systems benefit from subwavelength field localizations that make quantum emitters spatially distinguishable, thus enabling a reconfigurable photon source between antibunched and antipaired states via tailoring the energy bands. For a realistic nanoprism plexcitonic system, chemical and optical schemes of reconfiguration are demonstrated. These results pave the way to realize reconfigurable nonclassical photon sources in a simple quantum plexcitonic platform.

Erratum: Tensor Network Simulation of Non-Markovian Dynamics in Organic Polaritons [Phys. Rev. Lett. 121, 227401 (2018)].

This corrects the article DOI: 10.1103/PhysRevLett.121.227401.

Coupling of Molecular Emitters and Plasmonic Cavities beyond the Point-Dipole Approximation.

As the size of a molecular emitter becomes comparable to the dimensions of a nearby optical resonator, the standard approach that considers the emitter to be a point-like dipole breaks down. By adoption of a quantum description of the electronic transitions of organic molecular emitters, coupled to a plasmonic electromagnetic field, we are able to accurately calculate the position-dependent coupling strength between a plasmon and an emitter. The spatial distribution of excitonic and photonic quantum states is found to be a key aspect in determining the dynamics of molecular emission in ultrasmall cavities both in the weak and strong coupling regimes. Moreover, we show that the extreme localization of plasmonic fields leads to the selection rule breaking of molecular excitations.

Plasmonic Nanocavities Enable Self-Induced Electrostatic Catalysis.

The potential of strong interactions between light and matter remains to be further explored within a chemical context. Towards this end herein we study the electromagnetic interaction between molecules and plasmonic nanocavities. By means of electronic structure calculations, we show that self-induced catalysis emerges without any external stimuli through the interaction of the molecular permanent and fluctuating dipole moments with the plasmonic cavity modes. We also exploit this scheme to modify the transition temperature T1/2 of spin-crossover complexes as an example of how strong light-matter interactions can ultimately be used to control a materials responses.

Tensor Network Simulation of Non-Markovian Dynamics in Organic Polaritons.

We calculate the exact many-body time dynamics of polaritonic states supported by an optical cavity filled with organic molecules. Optical, vibrational, and radiative processes are treated on an equal footing employing the time-dependent variational matrix product states algorithm. We demonstrate signatures of non-Markovian vibronic dynamics and its fingerprints in the far-field photon emission spectrum at arbitrary light-matter interaction scales, ranging from the weak to the strong coupling regimes. We analyze both the single- and many-molecule cases, showing the crucial role played by the collective motion of molecular nuclei and dark states in determining the polariton dynamics and the subsequent photon emission.

Plasmonic Waveguide-Integrated Nanowire Laser.

Next-generation optoelectronic devices and photonic circuitry will have to incorporate on-chip compatible nanolaser sources. Semiconductor nanowire lasers have emerged as strong candidates for integrated systems with applications ranging from ultrasensitive sensing to data communication technologies. Despite significant advances in their fundamental aspects, the integration within scalable photonic circuitry remains challenging. Here we report on the realization of hybrid photonic devices consisting of nanowire lasers integrated with wafer-scale lithographically designed V-groove plasmonic waveguides. We present experimental evidence of the lasing emission and coupling into the propagating modes of the V-grooves, enabling on-chip routing of coherent and subdiffraction confined light with room-temperature operation. Theoretical considerations suggest that the observed lasing is enabled by a waveguide hybrid photonic-plasmonic mode. This work represents a major advance toward the realization of application-oriented photonic circuits with integrated nanolaser sources.

Many-Molecule Reaction Triggered by a Single Photon in Polaritonic Chemistry.

The second law of photochemistry states that, in most cases, no more than one molecule is activated for an excited-state reaction for each photon absorbed by a collection of molecules. In this Letter, we demonstrate that it is possible to trigger a many-molecule reaction using only one photon by strongly coupling the molecular ensemble to a confined light mode. The collective nature of the resulting hybrid states of the system (the so-called polaritons) leads to the formation of a polaritonic "supermolecule" involving the degrees of freedom of all molecules, opening a reaction path on which all involved molecules undergo a chemical transformation. We theoretically investigate the system conditions for this effect to take place and be enhanced.

Exploiting Vibrational Strong Coupling to Make an Optical Parametric Oscillator Out of a Raman Laser.

When the collective coupling of the rovibrational states in organic molecules and confined electromagnetic modes is sufficiently strong, the system enters into vibrational strong coupling, leading to the formation of hybrid light-matter quasiparticles. In this Letter, we demonstrate theoretically how this hybridization in combination with stimulated Raman scattering can be utilized to widen the capabilities of Raman laser devices. We explore the conditions under which the lasing threshold can be diminished and the system can be transformed into an optical parametric oscillator. Finally, we show how the dramatic reduction of the many final molecular states into two collective excitations can be used to create an all-optical switch with output in the midinfrared.

Uncoupled Dark States Can Inherit Polaritonic Properties.

When a collection of quantum emitters interacts with an electromagnetic field, the whole system can enter into the collective strong coupling regime in which hybrid light-matter states, i.e., polaritons can be created. Only a small portion of excitations in the emitters are coupled to the light field, and there are many dark states that, in principle, retain their pure excitonic nature. Here we theoretically demonstrate that these dark states can have a delocalized character, which is inherent to polaritons, despite the fact that they do not have a photonic component. This unexpected behavior only appears when the electromagnetic field displays a discrete spectrum. In this case, when the main loss mechanism in the hybrid system stems from the radiative losses of the light field, dark states are even more efficient than polaritons in transferring excitations across the structure.

Conformal surface plasmons propagating on ultrathin and flexible films.

Surface plasmon polaritons (SPPs) are localized surface electromagnetic waves that propagate along the interface between a metal and a dielectric. Owing to their inherent subwavelength confinement, SPPs have a strong potential to become building blocks of a type of photonic circuitry built up on 2D metal surfaces; however, SPPs are difficult to control on curved surfaces conformably and flexibly to produce advanced functional devices. Here we propose the concept of conformal surface plasmons (CSPs), surface plasmon waves that can propagate on ultrathin and flexible films to long distances in a wide broadband range from microwave to mid-infrared frequencies. We present the experimental realization of these CSPs in the microwave regime on paper-like dielectric films with a thickness 600-fold smaller than the operating wavelength. The flexible paper-like films can be bent, folded, and even twisted to mold the flow of CSPs.

Pronounced Photovoltaic Response from Multilayered Transition-Metal Dichalcogenides PN-Junctions.

Transition metal dichalcogenides (TMDs) are layered semiconductors with indirect band gaps comparable to Si. These compounds can be grown in large area, while their gap(s) can be tuned by changing their chemical composition or by applying a gate voltage. The experimental evidence collected so far points toward a strong interaction with light, which contrasts with the small photovoltaic efficiencies η ≤ 1% extracted from bulk crystals or exfoliated monolayers. Here, we evaluate the potential of these compounds by studying the photovoltaic response of electrostatically generated PN-junctions composed of approximately 10 atomic layers of MoSe2 stacked onto the dielectric h-BN. In addition to ideal diode-like response, we find that these junctions can yield, under AM-1.5 illumination, photovoltaic efficiencies η exceeding 14%, with fill factors of ~70%. Given the available strategies for increasing η such as gap tuning, improving the quality of the electrical contacts, or the fabrication of tandem cells, our study suggests a remarkable potential for photovoltaic applications based on TMDs.

Extraordinary exciton conductance induced by strong coupling.

We demonstrate that exciton conductance in organic materials can be enhanced by several orders of magnitude when the molecules are strongly coupled to an electromagnetic mode. Using a 1D model system, we show how the formation of a collective polaritonic mode allows excitons to bypass the disordered array of molecules and jump directly from one end of the structure to the other. This finding could have important implications in the fields of exciton transistors, heat transport, photosynthesis, and biological systems in which exciton transport plays a key role.