Direct Writing of Room Temperature Polariton Condensate Lattice.

Realizing lattices of exciton polariton condensates has been of much interest owing to the potential of such systems to realize analogue Hamiltonian simulators and physical computing architectures. Here, we report the realization of a room temperature polariton condensate lattice using a direct-write approach. Polariton condensation is achieved in a microcavity embedded with host-guest Frenkel excitons of an organic dye (rhodamine) in a small-molecule ionic isolation lattice (SMILES). The microcavity is patterned using focused ion beam etching to realize arbitrary lattice geometries, including defect sites on demand. The band structure of the lattice and the emergence of condensation are imaged using momentum-resolved spectroscopy. The introduction of defect sites is shown to lower the condensation threshold and result in the formation of a defect band in the condensation spectrum. The present approach allows us to study periodic, quasiperiodic, and disordered polariton condensate lattices at room temperature using a direct-write approach.

Addressing the Dark State Problem in Strongly Coupled Organic Exciton-Polariton Systems.

The manipulation of molecular excited state processes through strong coupling has attracted significant interest for its potential to provide precise control of photochemical phenomena. However, the key limiting factor for achieving this control has been the "dark-state problem", in which photoexcitation populates long-lived reservoir states with energies and dynamics similar to those of bare excitons. Here, we use a sensitive ultrafast transient reflection method with momentum and spectral resolution to achieve the selective excitation of organic exciton-polaritons in open photonic cavities. We show that the energy dispersions of these systems allow us to avoid the parasitic effect of the reservoir states. Under phase-matching conditions, we observe the direct population and decay of polaritons on time scales of less than 100 fs and find that momentum scattering processes occur on even faster time scales. We establish that it is possible to overcome the "dark state problem" through the careful design of strongly coupled systems.

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.

The Bulk van der Waals Layered Magnet CrSBr is a Quasi-1D Material.

Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for the study of fundamental interactions and excitations, such as Tomonaga-Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly for magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D material embedded in a magnetically ordered environment. The strong 1D electronic character originates from the Cr-S chains and the combination of weak interlayer hybridization and anisotropy in effective mass and dielectric screening, with an effective electron mass ratio of mXe/mYe ∼ 50. This extreme anisotropy experimentally manifests in strong electron-phonon and exciton-phonon interactions, a Peierls-like structural instability, and a Fano resonance from a van Hove singularity of similar strength to that of metallic carbon nanotubes. Moreover, because of the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D-correlated many-body physics in the presence of magnetic order.

Spin Dynamics of a Solid-State Qubit in Proximity to a Superconductor.

A broad effort is underway to understand and harness the interaction between superconductors and spin-active color centers with an eye on hybrid quantum devices and novel imaging modalities of superconducting materials. Most work, however, overlooks the interplay between either system and the environment created by the color center host. Here we use a diamond scanning probe to investigate the spin dynamics of a single nitrogen-vacancy (NV) center proximal to a superconducting film. We find that the presence of the superconductor increases the NV spin coherence lifetime, a phenomenon we tentatively rationalize as a change in the electric noise due to a superconductor-induced redistribution of charge carriers near induced redistribution of charge carriers near the NV. We then build on these findings to demonstrate transverse-relaxation-time-weighted imaging of the superconductor film. These results shed light on the dynamics governing the spin coherence of shallow NVs, and promise opportunities for new forms of noise spectroscopy and imaging of superconductors.

Sensing the Local Magnetic Environment through Optically Active Defects in a Layered Magnetic Semiconductor.

Atomic-level defects in van der Waals (vdW) materials are essential building blocks for quantum technologies and quantum sensing applications. The layered magnetic semiconductor CrSBr is an outstanding candidate for exploring optically active defects because of a direct gap, in addition to a rich magnetic phase diagram, including a recently hypothesized defect-induced magnetic order at low temperature. Here, we show optically active defects in CrSBr that are probes of the local magnetic environment. We observe a spectrally narrow (1 meV) defect emission in CrSBr that is correlated with both the bulk magnetic order and an additional low-temperature, defect-induced magnetic order. We elucidate the origin of this magnetic order in the context of local and nonlocal exchange coupling effects. Our work establishes vdW magnets like CrSBr as an exceptional platform to optically study defects that are correlated with the magnetic lattice. We anticipate that controlled defect creation allows for tailor-made complex magnetic textures and phases with direct optical access.

Highly nonlinear dipolar exciton-polaritons in bilayer MoS2.

Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in this context. However, the weak interaction between these quasiparticles has been a hurdle in this quest. Dipolar excitons provide an attractive strategy to overcome this limitation but are often hindered by their weak oscillator strength. The interlayer dipolar excitons in naturally occurring homobilayer MoS2 alleviates this issue owing to their formation via hybridization of interlayer charge transfer exciton with intralayer B exciton. Here we demonstrate the formation of dipolar exciton polaritons in bilayer MoS2 resulting in unprecedented nonlinear interaction strengths. A ten-fold increase in nonlinearity is observed for the interlayer dipolar excitons compared to the conventional A excitons. These highly nonlinear dipolar polaritons will likely be a frontrunner in the quest for solid-state quantum nonlinear devices.

Spin-correlated exciton-polaritons in a van der Waals magnet.

Strong coupling between light and elementary excitations is emerging as a powerful tool to engineer the properties of solid-state systems. Spin-correlated excitations that couple strongly to optical cavities promise control over collective quantum phenomena such as magnetic phase transitions, but their suitable electronic resonances are yet to be found. Here, we report strong light-matter coupling in NiPS3, a van der Waals antiferromagnet with highly correlated electronic degrees of freedom. A previously unobserved class of polaritonic quasiparticles emerges from the strong coupling between its spin-correlated excitons and the photons inside a microcavity. Detailed spectroscopic analysis in conjunction with a microscopic theory provides unique insights into the origin and interactions of these exotic magnetically coupled excitations. Our work introduces van der Waals magnets to the field of strong light-matter physics and provides a path towards the design and control of correlated electron systems via cavity quantum electrodynamics.

Thermalization of Fluorescent Protein Exciton-Polaritons at Room Temperature.

Fluorescent proteins (FPs) have recently emerged as a serious contender for realizing ultralow threshold room temperature exciton-polariton condensation and lasing. This contribution investigates the thermalization of FP microcavity exciton-polaritons upon optical pumping under ambient conditions. Polariton cooling is realized using a new FP molecule, called mScarlet, coupled strongly to the optical modes in a Fabry-Pérot cavity. Interestingly, at the threshold excitation energy (fluence) of ≈9 nJ per pulse (15.6 mJ cm-2 ), an effective temperature is observed, Teff  ≈ 350 ± 35 K close to the lattice temperature indicative of strongly thermalized exciton-polaritons at equilibrium. This efficient thermalization results from the interplay of radiative pumping facilitated by the energetics of the lower polariton branch and the cavity Q-factor. Direct evidence for dramatic switching from an equilibrium state into a metastable state is observed for the organic cavity polariton device at room temperature via deviation from the Maxwell-Boltzmann statistics at k‖  = 0 above the threshold. Thermalized polariton gases in organic systems at equilibrium hold substantial promise for designing room temperature polaritonic circuits, switches, and lattices for analog simulation.

Quasi-1D exciton channels in strain-engineered 2D materials.

Strain engineering is a powerful tool in designing artificial platforms for high-temperature excitonic quantum devices. Combining strong light-matter interaction with robust and mobile exciton quasiparticles, two-dimensional transition metal dichalcogenides (2D TMDCs) hold great promise in this endeavor. However, realizing complex excitonic architectures based on strain-induced electronic potentials alone has proven to be exceptionally difficult so far. Here, we demonstrate deterministic strain engineering of both single-particle electronic bandstructure and excitonic many-particle interactions. We create quasi-1D transport channels to confine excitons and simultaneously enhance their mobility through locally suppressed exciton-phonon scattering. Using ultrafast, all-optical injection and time-resolved readout, we realize highly directional exciton flow with up to 100% anisotropy both at cryogenic and room temperatures. The demonstrated fundamental modification of the exciton transport properties in a deterministically strained 2D material with effectively tunable dimensionality has broad implications for both basic solid-state science and emerging technologies.

Selective isomer emission via funneling of exciton polaritons.

Polaritons in organic systems has shown the potential to modify chemical properties and to mediate long-range energy transfer between individual chromophores, among other capabilities. Here, we demonstrate that strong coupling and formation of organic exciton-polaritons can be used to selectively tune the isomer emission of organic molecules. By taking advantage of their delocalized and hybrid character, polaritons emerging in the strong coupling regime open a new relaxation pathway that allows for an efficient funneling of the excitation between the molecular isomers. We implement this by strong coupling to trans-DCS (E-4-dimethylamino-4'cyanostilbene)molecules, which present two isomers in different amounts when immersed in a polymer matrix. Thanks to this new relaxation pathway, the photoexcitation that is first shared by the common polaritonic mode is then selectively funneled to the excited states of one of the isomers, recognizing pure emission from the isomeric states that do not contribute to emission under normal conditions.

Experimental observation of topological Z2 exciton-polaritons in transition metal dichalcogenide monolayers.

The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. Topological polaritons (TPs) offer an ideal platform in this context, with unique properties stemming from resilient topological states of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) as a promising platform for topological polaritonics. We show that the strong coupling between topological photonic modes of the metasurface and excitons in TMDs yields a topological polaritonic Z2 phase. We experimentally confirm the emergence of one-way spin-polarized edge TPs in metasurfaces integrating MoSe2 and WSe2. Combined with the valley polarization in TMD monolayers, the proposed system enables an approach to engage the photonic angular momentum and valley and spin of excitons, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics.

Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2.

Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe2) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼[Formula: see text] which is ∼4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.

Damage-Free Atomic Layer Etch of WSe2: A Platform for Fabricating Clean Two-Dimensional Devices.

The development of a controllable, selective, and repeatable etch process is crucial for controlling the layer thickness and patterning of two-dimensional (2D) materials. However, the atomically thin dimensions and high structural similarity of different 2D materials make it difficult to adapt conventional thin-film etch processes. In this work, we propose a selective, damage-free atomic layer etch (ALE) that enables layer-by-layer removal of monolayer WSe2 without altering the physical, optical, and electronic properties of the underlying layers. The etch uses a top-down approach where the topmost layer is oxidized in a self-limited manner and then removed using a selective etch. Using a comprehensive set of material, optical, and electrical characterization, we show that the quality of our ALE processed layers is comparable to that of pristine layers of similar thickness. The ALE processed WSe2 layers preserve their bright photoluminescence characteristics and possess high room-temperature hole mobilities of 515 cm2/V·s, essential for fabricating high-performance 2D devices. Further, using graphene as a testbed, we demonstrate the fabrication of ultra-clean 2D devices using a sacrificial monolayer WSe2 layer to protect the channel during processing, which is etched in the final process step in a technique we call sacrificial WSe2 with ALE processing (SWAP). The graphene transistors made using the SWAP technique demonstrate high room-temperature field-effect mobilities, up to 200,000 cm2/V·s, better than previously reported unencapsulated graphene devices.

Plasmonic enhancement of stability and brightness in organic light-emitting devices.

The field of plasmonics, which studies the resonant interactions of electromagnetic waves and free electrons in solid-state materials1, has yet to be put to large-scale commercial application2 owing to the large amount of loss that usually occurs in plasmonic materials3. Organic light-emitting devices (OLEDs)4-7 have been incorporated into billions of commercial products because of their good colour saturation, versatile form factor8 and low power consumption9, but could still be improved in terms of efficiency and stability. Although OLEDs incorporating organic phosphors achieve an internal charge-to-light conversion of unity10, their refractive index contrast reduces the observable fraction of photons outside the device to around 25 per cent11-13. Further, during OLED operation, a localized buildup of slow-decaying14 triplet excitons and charges15 gradually reduces the brightness of the device in a process called ageing16,17, which can result in 'burn-in' effects on the display. Simultaneously improving device efficiency and stability is of paramount importance for OLED technology. Here we demonstrate an OLED that uses the decay rate enhancement18 of a plasmonic system to increase device stability, while maintaining efficiency by incorporating a nanoparticle-based out-coupling scheme to extract energy from the plasmon mode. Using an archetypal phosphorescent emitter, we achieve a two-fold increase in operational stability at the same brightness as a reference conventional device while simultaneously extracting 16 per cent of the energy from the plasmon mode as light. Our approach to increasing OLED stability avoids material-specific designs19-22 and is applicable to all commercial OLEDs that are currently used for lighting panels, televisions and mobile displays.

Ultralong-Range Energy Transport in a Disordered Organic Semiconductor at Room Temperature Via Coherent Exciton-Polariton Propagation.

Amorphous molecular solids are inherently disordered, exhibiting strong exciton localization. Optical microcavities containing such disordered excitonic materials have been theoretically shown to support both propagating and localized exciton-polariton modes. Here, the ultrastrong coupling of a Bloch surface wave photon and molecular excitons in a disordered organic thin film at room temperature is demonstrated, where the major fraction of the polaritons are propagating states. The delocalized exciton-polariton has a group velocity as high as 3 × 107 m s-1 and a lifetime of 500 fs, leading to propagation distances of over 100 µm from the excitation source. The polariton intensity shows a halo-like pattern that is due to self-interference of the polariton mode, from which a coherence length of 20 µm is derived and is correlated with phase breaking by polariton scattering. The demonstration of ultralong-range exciton-polariton transport at room temperature promises new photonic and optoelectronic applications such as efficient energy transfer in disordered condensed matter systems.

A room-temperature polariton light-emitting diode based on monolayer WS2.

Exciton polaritons that arise through the strong coupling of excitons and cavity photons are used to demonstrate a wide array of fundamental phenomena and potential applications that range from Bose-Einstein-like condensation1-3 to analogue Hamiltonian simulators4,5 and chip-scale interferometers6. Recently, the two-dimensional (2D) transition metal dichalcogenides (TMDs), because of their large exciton binding energies, oscillator strength and valley degree of freedom, have emerged as a very attractive platform to realize exciton polaritons at elevated temperatures7. Achieving the electrical injection of polaritons is attractive both as a precursor to realizing electrically driven polariton lasers as well as for high speed light-emitting diodes (LEDs) for communication systems. Here, we demonstrate an electrically driven polariton LED that operates at room temperature using monolayer tungsten disulfide (WS2) as the emissive material. The extracted external quantum efficiency is ~0.1% and is comparable to recent demonstrations of bulk organic8 and carbon nanotube-based polariton electroluminescence (EL) devices9. The possibility to realize electrically driven polariton LEDs in atomically thin semiconductors at room temperature presents a promising step towards achieving an inversionless electrically driven laser in these systems as well as for ultrafast microcavity LEDs using van der Waals (vdW) materials.

Direct Observation of Gate-Tunable Dark Trions in Monolayer WSe2.

Spin-forbidden intravalley dark excitons in tungsten-based transition-metal dichalcogenides (TMDCs), because of their unique spin texture and long lifetime, have attracted intense research interest. Here, we show that we can control the dark exciton electrostatically by dressing it with one free electron or free hole, forming the dark trions. The existence of the dark trions is suggested by the unique magneto-photoluminescence spectroscopy pattern of the boron nitride (BN)-encapsulated monolayer WSe2 device at low temperature. The unambiguous evidence of the dark trions is further obtained by directly resolving the radiation pattern of the dark trions through back focal plane imaging. The dark trions possess a binding energy of ∼15 meV, and they inherit the long lifetime and large g-factor from the dark exciton. Interestingly, under the out-of-plane magnetic field, dressing the dark exciton with one free electron or hole results in distinctively different valley polarization of the emitted photon, as a result of the different intervalley scattering mechanism for the electron and hole. Finally, the lifetime of the positive dark trion can be further tuned from ∼50 ps to ∼215 ps by controlling the gate voltage. The gate-tunable dark trions usher in new opportunities for excitonic optoelectronics and valleytronics.

Guiding of visible photons at the ångström thickness limit.

Optical waveguides are vital components of data communication system technologies, but their scaling down to the nanoscale has remained challenging despite advances in nano-optics and nanomaterials. Recently, we theoretically predicted that the ultimate limit of visible photon guiding can be achieved in monolayer-thick transition metal dichalcogenides. Here, we present an experimental demonstration of light guiding in an atomically thick tungsten disulfide membrane patterned as a photonic crystal structure. In this scheme, two-dimensional tungsten disulfide excitonic photoluminescence couples into quasi-guided photonic crystal modes known as resonant-type Wood's anomalies. These modes propagate via total internal reflection with only a small portion of the light diffracted to the far field. Such light guiding at the ultimate limit provides more possibilities to miniaturize optoelectronic devices and to test fundamental physical concepts.