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.
Atmospheric aerosols can undergo phase transitions including liquid−liquid phase separation (LLPS) while responding to changes in the ambient relative humidity (RH). Here, we report results of chemical imaging experiments using environmental scanning electron microscopy (ESEM) and scanning transmission X-ray microscopy (STXM) to investigate the LLPS of micrometer-sized particles undergoing a full hydration-dehydration cycle. Internally mixed particles composed of ammonium sulfate (AS) and either: limonene secondary organic carbon (LSOC), α, 4-dihydroxy-3-methoxybenzeneaceticacid (HMMA), or polyethylene glycol (PEG-400) were studied. Events of LLPS were observed for all samples with both techniques. Chemical imaging with STXM showed that both LSOC/AS and HMMA/AS particles were never homogeneously mixed for all measured RH's above the deliquescence point and that the majority of the organic component was located in the outer phase. The outer phase composition was estimated as 65:35 organic: inorganic in LSOC/AS and as 50:50 organic: inorganic for HMMA/AS. PEG-400/AS particles showed fully homogeneous mixtures at high RH and phase separated below 89−92% RH with an estimated 70:30% organic to inorganic mix in the outer phase. These two chemical imaging techniques are well suited for in situ analysis of the hygroscopic behavior, phase separation, and surface composition of collected ambient aerosol particles.
Monolayers of transition metal dichalcogenide materials emerged as a new material class to study excitonic effects in solid state, as they benefit from enormous Coulomb correlations between electrons and holes. Especially in WSe2, sharp emission features have been observed at cryogenic temperatures, which act as single photon sources. Tight exciton localization has been assumed to induce an anharmonic excitation spectrum; however, the evidence of the hypothesis, namely the demonstration of a localized biexciton, is elusive. Here we unambiguously demonstrate the existence of a localized biexciton in a monolayer of WSe2, which triggers an emission cascade of single photons. The biexciton is identified by its time-resolved photoluminescence, superlinearity and distinct polarization in micro-photoluminescence experiments. We evidence the cascaded nature of the emission process in a cross-correlation experiment, which yields a strong bunching behaviour. Our work paves the way to a new generation of quantum optics experiments with two-dimensional semiconductors.
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.
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