interaction that 2D materials have demonstrated has made them highly attractive for practical device applications. Graphene, the archetype 2D material was explored extensively for a wide array of photonic applications 1 . However, due to the lack of direct bandgap in graphene, considerable attention has shifted towards 2D materials known as layered transition metal dichalcogenides (TMDs) 2,3 . These TMDs are a group of naturally abundant material with a MX 2 stoichiometry, where M is a transition metal element from group VI (M = Mo, W); and X is a chalcogen (M = S, Se, Te). One of the most intriguing aspect of TMDs is the emergence of fundamentally distinct electronic and optoelectronic properties as the material transitions from bulk to the 2D limit (monolayer) [4][5][6][7][8] . For example, the TMDs evolve from indirect to direct bandgap semiconductors spanning the energy range of 1.1 to 1.9 eV in the 2D limit 4-6 .Among the TMDs, molybdenum disulphide (MoS 2 ) is one of the most widely studied systems used to demonstrate 2D light emitters 9 , transistors 10,11 , valleytronics 12-15 and photodetectors 16,17 . The novel excitonic properties of 2D MoS 2 that make it very interesting for both fundamental studies and applications include: (i) the enhanced direct band gap photoluminescence (PL) quantum yield of the monolayer compared with the bulk counterpart 7,8 , (ii) the small effective exciton Bohr radius (0.93 nm) and associated large exciton binding energy (0.897 eV) 18,19 providing the opportunity for excitonic devices that operate at room temperature (RT) and (iii) the 2D nature of the dipole orientation making the excitonic emission highly anisotropic 20 . 3The interaction of a dipole with light can be modified by altering the surrounding dielectric environment. The most widely studied and technologically relevant phenomenon in this context is the Purcell enhancement wherein the spontaneous emission rate of the dipole is enhanced using an optical cavity by altering the photon density of states. Here the coupling between the dipole and the cavity photon is defined to be in the weak coupling regime since the interaction strength is weaker than the dissipation rates of the dipole and the photon. This regime has been demonstrated in the 2D materials using photonic crystal cavities coupled to 2D layers of MoS 2 21 , and WSe 2 22 . It resulted in an enhancement of the spontaneous emission rate and highly directional photon emission.When the interaction between the dipole and the cavity photons occur at a rate that is faster than the average dissipation rates of the cavity photon and dipole, one enters the strong coupling regime resulting in the formation of new eigenstates that are half-light -half-matter bosonic quasiparticles called cavity polaritons. Since with the pioneering work of Weisbuch et al. 23 there have been numerous demonstrations of cavity polariton formation and associated exotic phenomena in solid state systems using microcavities and quantum wells that support quasi 2D excitons [24][25][26] . H...
Light-matter interactions can be controlled by manipulating the photonic environment. We uncovered an optical topological transition in strongly anisotropic metamaterials that results in a dramatic increase in the photon density of states-an effect that can be used to engineer this interaction. We describe a transition in the topology of the iso-frequency surface from a closed ellipsoid to an open hyperboloid by use of artificially nanostructured metamaterials. We show that this topological transition manifests itself in increased rates of spontaneous emission of emitters positioned near the metamaterial. Altering the topology of the iso-frequency surface by using metamaterials provides a fundamentally new route to manipulating light-matter interactions.
Transport of nanoscale energy in the form of excitons is at the core of photosynthesis and the operation of a wide range of nanostructured optoelectronic devices such as solar cells, lightemitting diodes and excitonic transistors. Of particular importance is the relationship between exciton transport and nanoscale disorder, the defining characteristic of molecular and nanostructured materials. Here we report a spatial, temporal and spectral visualization of exciton transport in molecular crystals and disordered thin films. Using tetracene as an archetype molecular crystal, the imaging reveals that exciton transport occurs by random walk diffusion, with a transition to subdiffusion as excitons become trapped. By controlling the morphology of the thin film, we show that this transition to subdiffusive transport occurs at earlier times as disorder is increased. Our findings demonstrate that the mechanism of exciton transport depends strongly on the nanoscale morphology, which has wide implications for the design of excitonic materials and devices.
Emerging quantum technologies for cryptography, computing and metrology exploit quantum mechanical effects for enhanced information processing and nanoscale sensing. Though different platform systems are currently being explored, light-based quantum technologies using single-photon emitters as the basic building block are among the frontrunners 1 . Several strategies have been used to realize deterministic single photon sources in the solid state 2 , including quantum dots 3 , single molecules 4 , and point defects in wide bandgap materials such as diamond and silicon carbide 5-9 . Single photon emitters in novel van der Waals materials have garnered recent attention due to their potential for integration with waveguides, microcavities, and other passive components typical in photonic devices. Example 2D systems hosting quantum emitters include WSe 2 and MoS 2 as well as other transition metal dichalcogenides (TMDs) 10-14 .Here we focus on hexagonal boron nitride (hBN), a wide bandgap semiconductor where defect emission has been shown to be tunable and robust at room temperature 15-22 and above 23 . We use confocal microscopy to investigate the photoluminescence (PL) of point defects within thin hBN flakes deposited on a lithographically patterned SiO 2 substrate. Due to Van der Waals forces the flake conforms to the surface topography thus accumulating significant local strain near protruding features. Using large structured arrays of different sizes and geometries we find nearly perfect correspondence between the strained areas of the flake and defect emission. Our modeling supports the notion of defect activation via charge trapping in deformation potential wells. The physics at play has some similarities with that governing the dynamics of excitons in WSe 2 monolayers subjected to comparable geometries, as reported recently 24,25 . Unlike TMDs, however, the wide bandgap of hBN can accommodate large potential modulations, sufficient to stabilize the defect charge at room temperature. In particular, we calculate deformation potential wells as deep as 500 meV confined to regions of tensile and compressive strain in the hBN flake that correlate well with the spatial localization of the emitters.For the first set of experiments we use an array of 155-nm-high nanopillars with diameters ranging from 200 to 700 nm fabricated via electron beam lithography over a large-area silica substrate (Figure 1a); the sample is a commercial, 20-nmthick flake of hBN grown via chemical vapor deposition (CVD). We follow a wet transfer protocol 26 to drape the flake on the patterned silica substrate (see Methods). This technique takes advantage of the Van der Waals forces to make the flake conform to the surface topography. As an illustration, Figure 1b shows an atomic force microscopy (AFM) image from an hBN fragment where the 20-nm-thick flake folds on itself: We identify single-and double-layer sections near the left and right areas, respectively; bare pillars -visible on the lower, right corner of the image -provide a direct view...
A comprehensive theory is presented to mechanistically elucidate the long-range energy transfer between molecules strongly coupled to electromagnetic fields.
Here, we present the optical equivalent of the Lifshitz transition in strongly anisotropic metamaterials. When one of the components of the dielectric permittivity tensor of such a composite changes sign, the corresponding isofrequency surface transforms from an ellipsoid to a hyperboloid. Since the photonic density of states can be related to the volume enclosed by the isofrequency surface, such a topological transition in a metamaterial leads to a dramatic change in the photonic density of states, with a resulting effect on every single physical parameter related to the metamaterial -from thermodynamic quantities such as its equilibrium electromagnetic energy to the nonlinear optical response to quantumelectrodynamic effects such as spontaneous emission. In the present paper, we demonstrate the modification of spontaneous light emission from quantum dots placed near the surface of the metamaterial undergoing the topological Lifshitz transition, and present the theoretical description of the effect.
Fluorescent defects recently observed under ambient conditions in hexagonal boron nitride (h-BN) promise to open novel opportunities for the implementation of on-chip photonic devices that rely on identical photons from single emitters. Here we report on the room-temperature photoluminescence dynamics of individual emitters in multilayer h-BN flakes exposed to blue laser light. Comparison of optical spectra recorded at successive times reveals considerable spectral diffusion, possibly the result of slowly fluctuating, trapped-carrier-induced Stark shifts. Large spectral jumpsreaching up to 100 nmfollowed by bleaching are observed in most cases upon prolonged exposure to blue light, an indication of one-directional photochemical changes possibly taking place on the flake surface. Remarkably, only a fraction of the observed emitters also fluoresce on green illumination, suggesting a more complex optical excitation dynamics than previously anticipated and raising questions on the physical nature of the crystal defect at play.
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