When electron-hole pairs are excited in a semiconductor, it is a priori not clear if they form a plasma of unbound fermionic particles or a gas of composite bosons called excitons. Usually, the exciton phase is associated with low temperatures. In atomically thin transition metal dichalcogenide semiconductors, excitons are particularly important even at room temperature due to strong Coulomb interaction and a large exciton density of states. Using state-of-the-art many-body theory, we show that the thermodynamic fission–fusion balance of excitons and electron-hole plasma can be efficiently tuned via the dielectric environment as well as charge carrier doping. We propose the observation of these effects by studying exciton satellites in photoemission and tunneling spectroscopy, which present direct solid-state counterparts of high-energy collider experiments on the induced fission of composite particles.
Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum photonic technologies. The ability to tailor quantum emitters via site-selective defect engineering is essential for realizing scalable architectures. However, a major difficulty is that defects need to be controllably positioned within the material. Here, we overcome this challenge by controllably irradiating monolayer MoS 2 using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion exposed MoS 2 flake with high-quality hBN reveals spectrally narrow emission lines that produce photons in the visible spectral range. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron–hole complexes at defect states generated by the local helium ion exposure. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and interacting exciton lattices that may allow the exploration of Hubbard physics.
In monolayer transition metal dichalcogenides, quantum emitters are associated with localized strain that can be deterministically applied to create designer nano-arrays of single photon sources. Despite an overwhelming empirical correlation with local strain, the nanoscale interplay between strain, excitons, defects and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopy of excitons in nanobubbles of localized strain in monolayer WSe2 with atomistic structural models to elucidate how strain induces nanoscale confinement potentials that give rise to highly localized exciton states in 2D semiconductors. Nano-optical imaging of nanobubbles in low-defect monolayers reveal localized excitons on length scales of ~10 nm at multiple sites along the periphery of individual nanobubbles, which is in stark contrast to predictions of continuum models of strain. These results agree with theoretical confinement potentials that are atomistically derived from measured topographies of existing nanobubbles. Our results provide one-of-a-kind experimental and theoretical insight of how strain-induced confinement-without crystalline defects-can efficiently localize excitons on length scales commensurate with exciton size, providing key nanoscale structure-property information for quantum emitter phenomena in monolayer WSe2.The intense light-matter interactions of two-dimensional (2D) monolayer transition metal dichalcogenides (1L-TMDs) are mediated by a diverse suite of excitonic phenomena that present a wealth of opportunities for novel optoelectronic functionalities in areas spanning from high- *
The electronic and optical properties of monolayer transition-metal dichalcogenides (TMDs) and van der Waals heterostructures are strongly subject to their dielectric environment. In each layer, the field lines of the Coulomb interaction are screened by the adjacent material, which reduces the single-particle band gap as well as exciton and trion binding energies. By combining an electrostatic model for a dielectric heteromultilayered environment with semiconductor many-particle methods, we demonstrate that the electronic and optical properties are sensitive to the interlayer distances on the atomic scale. An analytic treatment is used to provide further insight into how the interlayer gap influences different excitonic transitions. Spectroscopical measurements in combination with a direct solution of a three-particle Schrödinger equation reveal trion binding energies that correctly predict recently measured interlayer distances and shed light on the effect of temperature annealing.
The optical properties of atomically thin transition metal dichalcogenide (TMDC) semiconductors are shaped by the emergence of correlated many-body complexes due to strong Coulomb interaction. Exceptional electron-hole exchange predestines TMDCs to study fundamental and applied properties of Coulomb complexes such as valley depolarization of excitons and fine-structure splitting of trions. Biexcitons in these materials are less understood and it has been established only recently that they are spectrally located between exciton and trion.Here we show that biexcitons in monolayer TMDCs exhibit a distinct fine structure on the order of meV due to electron-hole exchange. Ultrafast pump-probe experiments on monolayer WSe2 reveal decisive biexciton signatures and a fine structure in excellent agreement with a microscopic theory. We provide a pathway to access biexciton spectra with unprecedented accuracy, which is valuable beyond the class of TMDCs, and to understand even higher Coulomb complexes under the influence of electron-hole exchange.The exchange interaction between electrons and holes in semiconductors has long been a major field of interest in both theory and experiment. It has been discussed in the context of longitudinal-transverse exciton splitting in bulk materials [1, 2] and of exciton fine-structure splitting in quantum dots, where it is a major limitation to the generation of entangled photons [3,4]. Biexcitons, also known as exciton molecules, are fundamental to the nonlinear optical response of semiconductors. Based on a many-body theory including biexcitonic effects, nonlinear pump-probe experiments in InGaAs quantum wells have been successfully described [5,6] without taking electron-hole exchange into account. On the other hand, several authors have recognized the relevance of electronhole exchange for biexcitons in materials like CuCl and CdS [7][8][9][10][11][12][13]. Although in some cases significant corrections of biexciton binding energies due to electron-hole exchange have been reported, a fine-structure splitting of biexcitons has not been discussed.Atomically thin TMDC semiconductors offer new possibilities for studying Coulomb correlation effects by introducing reciprocal-space valleys as a new degree of freedom selectively addressable by circularly polarized light. Electron-hole exchange has strong implications for the valley dynamics and is currently an object of intense research [14][15][16][17]. The theory of electron-hole exchange in TMDC semiconductors has been put on a microscopic basis by Qiu et al. [18], who discussed the resulting nonanalytic exciton dispersion and strong splitting between bright and dark excitons. Similarly strong effects are observed in the fine-structure splitting of inter-and intravalley trions in these materials [19][20][21]. It is worth speculating whether biexcitons could also have a fine structure with implications for nonlinear optical effects utilized in coherent control schemes [22] and for manipulation of exciton spin coherences [23]. However, even...
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