M. Zinkiewicz, T. Woźniak, T. Kazimierczuk, P. Kapuściński, K. Oreszczuk, M. Grzeszczyk, M. Bartos, K. Nogajewski, K. Watanabe, T. Taniguchi, C. Faugeras, P. Ko… 展开作者
M. Zinkiewicz, T. Woźniak, T. Kazimierczuk, P. Kapuściński, K. Oreszczuk, M. Grzeszczyk, M. Bartos, K. Nogajewski, K. Watanabe, T. Taniguchi, C. Faugeras, P. Kossacki, M. Potemski, A. Babiński, M. R. Molas
We investigate the origin of emission lines apparent in the low-temperature photoluminescence spectra of $n$-doped WS$_2$ monolayer embedded in hexagonal BN layers using external magnetic fields and first-principles calculations. Apart from the neutral A exciton line, all observed emission lines are related to the negatively charged excitons. Consequently, we identify emissions due to both the bright (singlet and triplet) and dark (spin- and momentum-forbidden) negative trions as well as the phonon replicas of the latter optically-inactive complexes. The semi-dark trions and negative biexcitons are distinguished. Based on their experimentally extracted and theoretically calculated $g$-factors, we identify three distinct families of emissions due to exciton complexes in WS$_2$: bright, intravalley and intervalley dark. The $g$-factors of the spin-split subbands in both the conduction and valence bands are also determined.
Recently, two-dimensional (2D) materials have opened a new paradigm for fundamental physics explorations and device applications. Unlike gapless graphene, monolayer transition metal dichalcogenide (TMDC) has new optical functionalities for next generation ultra-compact electronic and opto-electronic devices. When TMDC crystals are thinned down to monolayers, they undergo an indirect to direct bandgap transition, making it an outstanding 2D semiconductor. Unique electron valley degree of freedom, strong light matter interactions and excitonic effects were observed. Enhancement of spontaneous em…
The magneto-optical response of monolayer transition metal dichalcogenides (TMDs), including excitonic effects, is studied using a nanoribbon geometry. We compute the diagonal optical conductivity and the Hall conductivity. Comparing the excitonic optical Hall conductivity to results obtained in the independent particle approximation, we find an increase in the amplitude corresponding to one order of magnitude when excitonic effects are included. The Hall conductivities are used to calculate Faraday rotation spectra for MoS2 and WSe2. Finally, we have also calculated the diamagnetic shift of t…
The recent advent of two-dimensional monolayer materials with tunable optoelectronic properties and high carrier mobility offers renewed opportunities for efficient, ultra-thin excitonic solar cells alternative to those based on conjugated polymer and small molecule donors. Using first-principles density functional theory and many-body calculations, we demonstrate that monolayers of hexagonal BN and graphene (CBN) combined with commonly used acceptors such as PCBM fullerene or semiconducting carbon nanotubes can provide excitonic solar cells with tunable absorber gap, donor-acceptor interface …
Light emission in atomically thin heterostructures is known to depend on the type of materials, number and stacking sequence of the constituent layers. Here we show that the thickness of a two-dimensional substrate can be crucial in modulating the light emission. We study the layer-dependent charge transfer in vertical heterostructures built from monolayer tungsten disulphide (WS2) on one- and two-layer epitaxial graphene, unravelling the effect that the interlayer electronic coupling has on the excitonic properties of such heterostructures. We bring evidence that the excitonic properties of W…
We investigate Landau-quantized excitonic absorption and luminescence of monolayer WSe$_2$ under magnetic field. We observe gate-dependent quantum oscillations in the bright exciton and trions (or exciton-polarons) as well as the dark trions and their phonon replicas. Our results reveal spin- and valley-polarized Landau levels (LLs) with filling factors $n = +0, +1$ in the bottom conduction band and $n = -0$ to $-6$ in the top valence band, including the Berry-curvature-induced $n = \pm0$ LLs of massive Dirac fermions. The LL filling produces periodic plateaus in the exciton energy shift accom…
Exciton intervalley scattering, annihilation and relaxation dynamics, and diffusive transport in a monolayer transition metal dichalcogenides are central to the functionality of devices based on them. This motivated us to investigate these properties in exfoliated high-quality monolayer MoSe2 using heterodyned nonlinear four-wave-mixing transient grating spectroscopy. While free exciton excitations are found to be long-lived (~230 ps), an extremely fast intervalley scattering ( less than 120 fs) is observed leading to a negligible valley polarization, consistent with steady state photoluminesc…
Strong Coulomb interaction in 2D materials provides unprecedented opportunities for studying many key issues of condensed matter physics, such as co-existence and mutual conversions of excitonic complexes, fundamental optical processes associated with their conversions, and their roles in the celebrated Mott transition. Recent lasing demonstrations in 2D materials raise important questions about the existence and origin of optical gain and possible roles of excitonic complexes. While lasing occurred at extremely low densities dominated by various excitonic complexes, optical gain was observed …
The reduced dielectric screening in atomically thin transition metal dichalcogenides allows to study the hydrogen-like series of higher exciton states in optical spectra even at room temperature. The width of excitonic peaks provides information about the radiative decay and phonon-assisted scattering channels limiting the lifetime of these quasi-particles. While linewidth studies so far have been limited to the exciton ground state, encapsulation with hBN has recently enabled quantitative measurements of the broadening of excited exciton resonances. Here, we present a joint experiment-theory …
We investigate the excitonic spectrum of MoS$_2$ monolayers and calculate its optical absorption properties over a wide range of energies. Our approach takes into account the anomalous screening in two dimensions and the presence of a substrate, both cast by a suitable effective Keldysh potential. We solve the Bethe-Salpeter equation using as a basis a Slater-Koster tight-binding model parameterized to fit ab initio MoS$_2$ band structure calculations. The resulting optical conductivity is in good quantitative agreement with existing measurements up to ultraviolet energies. We establish that t…
Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such d…
Transition metal dichalcogenides (TMDs) are known to support complex excitonic states. Revealing the differences in relaxation dynamics among different excitonic species and elucidating the transition dynamics between them may provide important guidelines for designing TMD-based excitonic devices. Combining photoluminescence (PL) and reflectance contrast measurements with ultrafast pump-probe spectroscopy under cryogenic temperatures, we herein study the relaxation dynamics of neutral and charged excitons in a back-gate-controlled monolayer device. Pump-probe results reveal quite different rel…
We theoretically investigate excitons in MoS$_2$ monolayers in an applied in-plane electric field. Tight-binding and Bethe-Salpeter equation calculations predict a quadratic Stark shift, of the order of a few meV for fields of 10 V/$μ$m, in the linear absorption spectra. The spectral weight of the main exciton peaks decreases by a few percent with an increasing electric field due to the exciton field ionization into free carriers as reflected in the exciton wave functions. Subpicosecond exciton decay lifetimes at fields of a few tens of V/$μ$m could be utilized in solar energy harvesting and p…
Novel 2D material CrI3 reveals unique combination of 2D ferromagnetism and robust excitonic response. We demonstrate that the possibility of the formation of magnetic topological defects, such as Neel skyrmions, together with large excitonic Zeeman splitting, leads to giant scattering asymmetry, which is the necessary prerequisite for the excitonic anomalous Hall effect. In addition, the diamagnetic effect breaks the inversion symmetry, and in certain cases can result in exciton localization on the skyrmion. This enables the formation of magnetoexcitonic quantum dots with tunable parameters.
Motivated by the recent synthesis of two-dimensional monolayer AlSb, we theoretically investigate its ground state and electronic properties using the first-principles calculations coupled with Bethe-Salpeter equation. An excitonic instability is revealed as a result of larger exciton binding energy than the corresponding one-electron energy gap by $\sim$0.1 eV, which is an indicative of a many-body ground state accompanied by spontaneous exciton generation. Including the spin-orbit coupling is proven to be a must to correctly predict the ground state. At room temperature, the two-dimensional …
The effect of anisotropy in the energy spectrum on the binding energy and structural properties of excitons, trions, and biexcitons is investigated. To this end we employ the stochastic variational method with a correlated Gaussian basis. We present results for the binding energy of different excitonic complexes in black phosphorus (bP) and TiS$_3$ and compare them with recent results in the literature when available, for which we find good agreement. The binding energies of excitonic complexes in bP are larger than those in TiS$_3$. We calculate the different average interparticle distances i…
We analyze the dielectric-function spectra of low dimensional transition metal dichalcogenides (TMDCs) using a fully analytical model of the complex dielectric function that is applicable in fractional dimensional space. We extract the dimensionalities of the $A$ and $B$ excitons as well as their Lorentzian broadening widths by fitting the model to experimental data in the spectral range of photon energies (1.5 - 3 eV). Our results show the significant contribution of the lowest ground exciton state to the dielectric properties of exemplary monolayer materials (MoS$_2$, MoSe$_2$ and WSe$_2$). …
Uniform Narrow Excitonic Spectrum in Large-Area Suspended WSe2 Monolayers
NTT Basic Research Laboratories, NTT, Inc.(NTT基础研究所);Department of Materials Science, Graduate School of Engineering, Tohoku University(东北大学大学院工学研究科材料科学系);Center for Science and Innovation in Spintronics, Tohoku University(东北大学自旋电子学科学与创新中心);Quantum Materials and Applications Research Center, National Institutes for Quantum Science and Technology(量子科学技术研究院量子材料与应用研究中心)
Confined excitonic complexes in two dimensions, consisting of N_e electrons and N_h holes, are studied by means of Bethe-Goldstone equations. Systems with up to twelve pairs, and asymmetric configurations with N_e \ne N_h are considered. The weak confinement regime gives indication of weak binding or even unbinding in the triexciton and the four-exciton system, and binding in the higher complexes.
Strong Coulomb interactions in atomically thin semiconductors like monolayer WSe$_2$ induce not only tightly bound excitons, but also make their optical properties very sensible to doping. By utilizing a microscopic theory based on the excitonic Heisenberg equations of motion, we systematically determine the influence of doping on the excitonic linewidth, lineshift, and oscillator strength. We calculate trion resonances and demonstrate that the Coulomb coupling of excitons to the trionic continuum generates a non-Markovian interference, which, due to a time retardation, builds up a phase respo…
WSe$_2$ monolayers with variable doping are an ideal system to study two-dimensional excitonic complexes. Here, we find that the strongest photoluminescence from bright neutral excitons occurs at moderate $p$-doping levels, owing to a rapid decrease of signal from positive dark trions and a slow increase of signal from positive bright trions with growing $p$-concentrations. We explain our observations with a qualitative model, in which the scattering rate of bright excitons into dark complexes is enhanced by exciton localization, while the scattering rate into positive bright trions increases …
Atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDCs) are attractive materials for next generation nanoscale optoelectronic applications. Understanding nanoscale optical behavior of the edges and grain boundaries of synthetically grown TMDCs is vital for optimizing their optoelectronic properties. Elucidating the nanoscale optical properties of 2D materials through far-field optical microscopy requires a diffraction-limited optical beam diameter sub-micron in size. Here we present our experimental work on spatial photoluminescence (PL) scanning of large size ( $\geq 50$…
The formation and various possible decay processes of neutral and charged excitonic complexes in electronic integral and fractional quantum Hall systems are discussed. The excitonic complexes are bound states of a small number of the relevant negatively and positively charged quasiparticles (e.g., conduction electrons and valence holes, reversed-spin electrons and spin holes, Laughlin quasielectrons and quasiholes, composite fermions) that occur in an electron system under specific conditions (e.g., electron density, well width, electric and magnetic fields, or hydrostatic pressure). The examp…
Excitonic complexes in type-II quantum-ring heterostructures may be considered as artificial atoms due to the confinement of only one charge-carrier type in an artificial nucleus. Binding energies of excitons, trions, and biexcitons in these nanostructures are then effectively ionization energies of these artificial atoms. The binding energies reported here are calculated within the effective-mass approximation using the diffusion quantum Monte Carlo method and realistic geometries for gallium antimonide rings in gallium arsenide. The electrons form a halo outside the ring, with very little ch…
Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such ground state interactions is generally not sufficient to reach the regime of quantum nonlinear optics and strong single…
We predict a phase transition in freestanding monolayer Xenes from the semiconducting phase to the excitonic insulating (EI) phase can be induced by reducing an external electric field below some critical value which is unique to each material. The splitting of the conduction and valence bands due to spin-orbit coupling at non-zero electric fields leads to the formation of $A$ and $B$ excitons in the larger or smaller band gap, with correspondingly larger or smaller binding energies. Our calculations show the coexistence of the semiconducting phase of $A$ excitons with the EI phase of $B$ exci…
Monolayer transition metal dichalcogenide semiconductors host strongly bound two-dimensional excitonic complexes, and form an excellent platform for probing many-body physics through manipulation of Coulomb interaction. Quantum confined Stark effect is one of the routes to dynamically tune the emission line of these excitonic complexes. In this work, using a high quality graphene/hBN/WS$_2$/hBN/Au vertical heterojunction, we demonstrate for the first time, an out-of-plane electric field driven change in the sign of the Stark shift from blue to red for four different excitonic species, namely, …
We report many-body perturbation theory calculations of excited-state properties of distorted 1-T diamond-chain monolayer rhenium disulfide (ReS2) and diselenide (ReSe2). Electronic self-energy substantially enhances their quasiparticle band gaps and, surprisingly, converts monolayer ReSe2 to a direct-gap semiconductor, which was, however, regarded to be an indirect one by density-functional-theory calculations. Their optical absorption spectra are dictated by strongly bound excitons. Unlike hexagonal structures, the lowest-energy bright exciton of distorted 1-T ReS2 exhibits a perfect figure-…
We report a combined theoretical/experimental study of dynamic screening of excitons in media with frequency-dependent dielectric functions. We develop an analytical model showing that interparticle interactions in an exciton are screened in the range of frequencies from zero to the characteristic binding energy depending on the symmetries and transition energies of that exciton. The problem of the dynamic screening is then reduced to simply solving the Schrodinger equation with an effectively frequency-independent potential. Quantitative predictions of the model are experimentally verified us…
Light-emitting diodes are of importance for lighting, displays, optical interconnects, logic and sensors. Hence the development of new systems that allow improvements in their efficiency, spectral properties, compactness and integrability could have significant ramifications. Monolayer transition metal dichalcogenides have recently emerged as interesting candidates for optoelectronic applications due to their unique optical properties. Electroluminescence has already been observed from monolayer MoS2 devices. However, the electroluminescence efficiency was low and the linewidth broad due both …
We develop a theory of the excitonic phase recently proposed as the zero-field insulating state observed near charge neutrality in monolayer WTe$_2$. Using a Hartree-Fock approximation, we numerically identify two distinct gapped excitonic phases: a spin density wave state for weak non-zero interaction strength and spin spiral order at stronger interactions, separated by a narrow window of non-excitonic quantum spin Hall insulator. We introduce a simplified model capturing key features of the WTe$_2$ band structure, in which these phases appear as distinct valley ferromagnetic orders. We link …
Monolayers of transition metal dichalcogenides (TMDCs) have emerged as new optoelectronic materials in the two dimensional (2D) limit, exhibiting rich spin-valley interplays, tunable excitonic effects, and strong light-matter interactions. An essential yet undeveloped ingredient for many photonic applications is the manipulation of its light emission. Here we demonstrate the control of excitonic light emission from monolayer tungsten diselenide (WSe2) in an integrated photonic structure, achieved by transferring one monolayer onto a photonic crystal (PhC) with a cavity. In addition to the obse…
Quantifying and controlling the coherent dynamics and couplings of optically active excitations in solids is of paramount importance in fundamental research in condensed matter optics and for their prospective optoelectronic applications in quantum technologies. Here, we perform ultrafast coherent nonlinear spectroscopy of a charge-tunable MoSe$_2$ monolayer. The experiments show that the homogeneous and inhomogeneous line width and the population decay of exciton complexes hosted by this material can be directly tuned by an applied gate bias, which governs the Fermi level and therefore the fr…
Hereby, we present a comprehensive experimental and theoretical study of the electronic structure and optical properties of excitonic complexes in strain-engineered InGaAs/GaAs quantum dots (QDs) grown by metal-organic chemical vapour deposition and emitting at the 1300 nm telecommunication window. Single QD properties have been determined experimentally for a number of nanostructures by means of excitation-power-dependent and polarization-resolved microphotoluminescence and further compared with the results of confined states calculations employing the 8-band kp theory combined with the confi…
The results of magneto-optical spectroscopy investigations of excitons in a CVD grown monolayer of WSe2 encapsulated in hexagonal boron nitride are presented. The emission linewidth for the 1s state is of 4:7 meV, close to the narrowest emissions observed in monolayers exfoliated from bulk material. The 2s excitonic state is also observed at higher energies in the photoluminescence spectrum. Magneto-optical spectroscopy allows for the determination of the g-factors and of the spatial extent of the excitonic wave functions associated with these emissions. Our work establishes CVD grown monolaye…
We present optical spectroscopy (photoluminescence and reflectance) studies of thin layers of the transition metal dichalcogenide WSe2, with thickness ranging from mono- to tetra-layer and in the bulk limit. The investigated spectra show the evolution of excitonic resonances as a function of layer thickness, due to changes in the band structure and, importantly, due to modifications of the strength of Coulomb interaction as well. The observed temperature-activated energy shift and broadening of the fundamental direct exciton are well accounted for by standard formalisms used for conventional s…
Exciton enhanced nonlinear optical responses in monolayer h-BN and MoS2: Insight from first-principles exciton-state coupling formalism and calculations
University of California at Berkeley(加州大学伯克利分校);Lawrence Berkeley National Laboratory(劳伦斯伯克利国家实验室);National Center of Theoretical Physics(国家理论物理中心);Institute of Atomic and Molecular Sciences, Academia Sinica(中央研究院原子与分子科学研究所)
A configuration space approach is developed to uncover generic stability peculiarities for the lowest energy neutral and charged exciton complexes (biexciton and trion) in quasi-one-dimensional semiconductors. Trions are shown to be more stable than biexcitons in strongly confined structures with small reduced electron-hole masses. Biexcitons are more stable in less confined structures with large reduced electron-hole masses. In semiconducting carbon nanotubes, in particular, the trion binding energy is shown to be greater than that of the biexciton by a factor ~1.4 decreasing with diameter, t…
We present a comprehensive optical study of the excitonic Zeeman effects in transition metal dichalcogenide monolayers, which are discussed comparatively for selected materials: MoSe$_2$, WSe$_2$ and WS$_2$. We introduce a simple semi-phenomenological description of the magnetic field evolution of individual electronic states in fundamental sub-bands by considering three additive components: valley, spin and orbital terms. We corroborate the validity of the proposed description by inspecting the Zeeman-like splitting of neutral and charged excitonic resonances in absorption-type spectra. The v…
Despite 2D materials holding great promise for a broad range of applications, the proliferation of devices and their fulfillment of real-life demands are still far from being realized. Experimentally obtainable samples commonly experience a wide range of perturbations (ripples and wrinkles, point and line defects, grain boundaries, strain field, doping, water intercalation, oxidation, edge reconstructions) significantly deviating the properties from idealistic models. These perturbations, in general, can be entangled or occur in groups with each group forming a complex perturbation making the …
Due to degeneracies arising from crystal symmetries, it is possible for electron states at band edges ("valleys") to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseudospins, analogous to that routinely implemented using true spin, in the quest for quantum technologies. Here we show for the first time that SU(2) valley coherence can indeed be generated and detected. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley e…
Monolayer transition metal dichalcogenides in the T' phase promise to realize the quantum spin Hall (QSH) effect at room temperature, because they exhibit a prominent spin-orbit gap between inverted bands in the bulk. Here we show that the binding energy of electron-hole pairs excited through this gap is larger than the gap itself in MoS2, a paradigmatic material that we investigate from first principles by many-body perturbation theory (MBPT). This paradoxical result hints at the instability of the T' phase against the spontaneous generation of excitons, and indeed we find that it gives rise …
Monolayer transition metal dichalcogenides feature tightly bound bright excitons at the degenerate valleys, where electron-hole Coulomb exchange interaction strongly couples the valley pseudospin to the momentum of exciton. Placed on periodically structured dielectric substrate, the spatial modulation of the Coulomb interaction leads to the formation of exciton Bloch states with real-space valley pseudospin texture displayed in a mesoscopic supercell. We find this spatial valley texture in the exciton Bloch function is pattern-locked to the propagation direction, enabling nano-optical excitati…
Recently, quantum oscillation of the resistance in insulating monolayer WTe$_2$ was reported. An explanation in terms of gap modulation in the hybridized Landau levels of an excitonic insulator was also proposed by one of us. However, the previous picture of gap modulation in the Landau levels spectrum was built on a pair of well nested electron and hole Fermi surfaces, while the monolayer WTe$_2$ has one hole and two electron Fermi pockets with relative anisotropy. Here we demonstrate that for system like monolayer WTe$_2$, the excitonic insulating state arising from the coupled one hole and …
Second-harmonic generation (SHG) is a well-known nonlinear spectroscopy method to probe electronic structure, specifically, in transition metal dichalcogenide (TMDC) monolayers. This work investigates the nonlinear dynamics of a strongly excited TMDC monolayer by solving the time evolution equations for the density matrix. It is shown that the presence of excitons qualitatively changes the nonlinear dynamics leading, in particular, to a huge enhancement of the nonlinear signal as a function of the dielectric environment. It is also shown that the SHG polarization angular diagram and its depend…
The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (> 6 $μ$s) and…
Screening due to surrounding dielectric medium reshapes the electron-hole interaction potential and plays a pivotal role in deciding the binding energies of strongly bound exciton complexes in quantum confined monolayers of transition metal dichalcogenides (TMDs). However, owing to strong quasi-particle bandgap renormalization in such systems, a direct quantification of estimated shifts in binding energy in different dielectric media remains elusive using optical studies. In this work, by changing the dielectric environment, we show a conspicuous photoluminescence (PL) peak shift at low temper…
Excitonic optical absorption in strained monolayer CrSBr
Universidad Autónoma de Madrid(马德里自治大学);École Polytechnique Fédérale de Lausanne (EPFL)(洛桑联邦理工学院);Universitat de València(瓦伦西亚大学);Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)(马德里材料科学研究所)
Transition-metal dichalcogenides can be easily produced as atomically thin sheets, exhibiting the possibility to optically polarize and read out the valley pseudospin of extremely stable excitonic quasiparticles present in these 2D semiconductors. Here, we investigate a monolayer of tungsten disulphide in high magnetic fields up to 30\,T via photoluminescence spectroscopy at low temperatures. The valley degeneracy is lifted for all optical features, particularly for excitons, singlet and triplet trions, for which we determine the g factor separately. While the observation of a diamagnetic shif…
Monolayer transition metal dichalcogenide (TMDC) semiconductors exhibit strong excitonic optical resonances which serve as a microscopic, non-invasive probe into their fundamental properties. Like the hydrogen atom, such excitons can exhibit an entire Rydberg series of resonances. Excitons have been extensively studied in most TMDCs (MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$), but detailed exploration of excitonic phenomena has been lacking in the important TMDC material molybdenum ditelluride (MoTe$_2$). Here, we report an experimental investigation of excitonic luminescence properties of monolay…
The interplay between topology and correlations can generate a variety of quantum phases, many of which remain to be explored. Recent advances have identified monolayer WTe2 as a promising material for doing so in a highly tunable fashion. The ground state of this two-dimensional (2D) crystal can be electrostatically tuned from a quantum spin Hall insulator (QSHI) to a superconductor. However, much remains unknown about the gap-opening mechanism of the insulating state. Here we report evidence that the QSHI is also an excitonic insulator (EI), arising from the spontaneous formation of electron…