Solid-state cavity quantum electrodynamics is a rapidly advancing field, which explores the frontiers of light–matter coupling. Metal-based approaches are of particular interest in this field, as they carry the potential to squeeze optical modes to spaces significantly below the diffraction limit. Transition metal dichalcogenides are ideally suited as the active material in cavity quantum electrodynamics, as they interact strongly with light at the ultimate monolayer limit. Here, we implement a Tamm-plasmon-polariton structure and study the coupling to a monolayer of WSe2, hosting highly stable excitons. Exciton-polariton formation at room temperature is manifested in the characteristic energy–momentum dispersion relation studied in photoluminescence, featuring an anti-crossing between the exciton and photon modes with a Rabi-splitting of 23.5 meV. Creating polaritonic quasiparticles in monolithic, compact architectures with atomic monolayers under ambient conditions is a crucial step towards the exploration of nonlinearities, macroscopic coherence and advanced spinor physics with novel, low-mass bosons.
Spin-orbit coupling is a fundamental mechanism that connects the spin of a charge carrier with its momentum 1 . Likewise, in the optical domain, a synthetic spin-orbit coupling is accessible, for instance, by engineering optical anisotropies in photonic materials 2 . Both, akin, yield the possibility to create devices directly harnessing spin-and polarization as information carriers 3 . Atomically thin layers of transition metal dichalcogenides provide a new material platform which promises intrinsic spin-valley Hall features both for free carriers, two-particle excitations (excitons), as well as for photons 4 . In such materials, the spin of an exciton is closely linked to the high-symmetry point in reciprocal space it emerges from (K and K' valleys) 5,6 . Here, we demonstrate, that spin, and hence valley selective propagation is accessible in an atomically thin layer of MoSe2, which is strongly coupled to a microcavity photon mode. We engineer a wire-like device, where we can clearly trace the flow, and the helicity of exciton-polaritons expanding along a channel. By exciting a coherent superposition of K and K' tagged polaritons, we observe valley selective expansion of the polariton cloud without neither any applied external magnetic fields nor coherent Rayleigh scattering. Unlike the valley Hall effect for TMDC excitons 7 , the observed optical valley Hall effect (OVHE) 8 strikingly occurs on a macroscopic scale, and clearly reveals the potential for applications in spin-valley locked photonic devices.Spin-valley locking is a striking feature of free charge carriers and excitons emerging in monolayers of transition metal dichalcogenides (TMDCs) 6,9 . It originates form the strong spin-orbit interaction, which arises from the heavy transition metals in TMDCs and the broken inversion symmetry of the crystal lattice. This leads to inverted spin orientations at opposite K points at the corners of the hexagonal Brillouin zone, for both conduction band electrons and valence band holes. As a result, the K and K' valleys can be selectively addressed by σ + and σcircular polarized light 10,11 , which is referred to as valley-polarization. Likewise, coherent superpositions of both valleys can be excited by linear polarized light, which is referred to as valley coherence. The outstanding control of the valley pseudospin has attracted great interest in exploiting this degree of freedom to encode and process information by manipulating free charge carriers 12 and excitons 7,13,14 , which has led to the emerging field of valleytronics 4 . However, exciton spin-valley applications are strongly limited by the depolarization mechanisms due to the strong Coulomb exchange interaction of electrons and holes, as well as by the limited exciton diffusion and propagation lengths.
Bosonic condensation belongs to the most intriguing phenomena in physics, and was mostly reserved for experiments with ultra-cold quantum gases. More recently, it became accessible in exciton-based solid-state systems at elevated temperatures. Here, we demonstrate bosonic condensation driven by excitons hosted in an atomically thin layer of MoSe2, strongly coupled to light in a solid-state resonator. The structure is operated in the regime of collective strong coupling between a Tamm-plasmon resonance, GaAs quantum well excitons, and two-dimensional excitons confined in the monolayer crystal. Polariton condensation in a monolayer crystal manifests by a superlinear increase of emission intensity from the hybrid polariton mode, its density-dependent blueshift, and a dramatic collapse of the emission linewidth, a hallmark of temporal coherence. Importantly, we observe a significant spin-polarization in the injected polariton condensate, a fingerprint for spin-valley locking in monolayer excitons. Our results pave the way towards highly nonlinear, coherent valleytronic devices and light sources.
When the coupling between light and matter becomes comparable to the energy gap between different excited states they hybridize, leading to the appearance of a rich and complex phenomenology which attracted remarkable interest in recent years. While the mixing between states with different number of excitations, so-called ultrastrong coupling regime, has been observed in various implementations, the effect of the hybridization between different single excitation states, referred to as very strong coupling regime, has remained elusive. In semiconductor quantum wells such a regime is predicted to manifest as a photon-mediated electron-hole coupling leading to different excitonic wavefunctions for the two polaritonic branches when the ratio of the coupling strength to exciton binding energy ⁄ approaches unity. Here, we verify experimentally the existence of this regime in magneto-optical measurements on a microcavity with 28 GaAs quantum wells, characterized by ⁄ ≈ 0.64, showing that the average electron-hole separation of the upper polariton is significantly increased compared to the bare quantum well exciton Bohr radius. This manifests in a diamagnetic shift around zero detuning that exceeds the shift of the lower polariton by one order of magnitude and the bare quantum well exciton diamagnetic shift by a factor of two. The lower polariton exhibits a diamagnetic shift smaller than expected from the coupling of a rigid exciton to the cavity mode which suggests more tightly bound electron-hole pairs than in the bare quantum well.
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