We propose a state of excitonic solid for double layer two dimensional electron hole systems in transition metal dicalcogenides stacked on opposite sides of thin layers of BN. Properties of the exciton lattice such as its Lindemann ratio and possible supersolid behaviour are studied. We found that the solid can be stabilized relative to the fluid by the potential due to the BN.
In this paper, we employ a fully microscopic approach to the study of interlayer excitons in hetero-bilayers. We use Fowler's and Karplus' method to access the dynamical polarizability of non--interacting interlayer excitons in a $\mathrm{WSe}_{2}/\mathrm{WS}_{2}$--based van der Waals heterostructure. Following from the calculation of the linear polarizability, we consider Svendsen's variational method to the calculation of the dynamic third--order polarizability. With this variational method, we study both two--photon absorption and third--harmonic generation processes for interlayer excitons…
An ordered state of electrons in solids in which excitons condense was proposed many years ago as a theoretical possibility but has, until recently, never been observed. We review recent studies of semiconductor bilayer systems that provide clear evidence for this phenomenon and explain why exciton condensation in the quantum Hall regime, where these experiments were performed, is as likely to occur in electron-electron bilayers as in electron-hole bilayers. In current quantum Hall exciton condensates, disorder induces mobile vortices that flow in response to a supercurrent and limit the extre…
In ordinary semiconductor bilayers, exciton condensates appear at total Landau level filling factor $ν_{T}=1$. We predict that similar states will occur in Bernal stacked graphene bilayers at many non-zero integer filling factors. For $ν_{T} = -3,1$ we find that the superfluid density of the exciton condensate vanishes and that a finite-temperature fluctuation induced first order isotropic-smectic phase transition occurs when the layer densities are not balanced. These anomalous properties of bilayer graphene exciton condensates are due to the degeneracy of Landau levels with $n=0$ and $n=1$ o…
Exciton superfluid is a macroscopic quantum phenomenon in which large quantities of excitons undergo the Bose-Einstein condensation. Recently, exciton superfluid has been widely studied in various bilayer systems. However, experimental measurements only provide indirect evidence for the existence of exciton superfluid. In this article, by viewing the exciton in a bilayer system as an electric dipole, we provide a general theory for the electric dipole superconductivity, and derive the London-type and Ginzburg-Landau-type equations for the electric dipole superconductors. By using these equatio…
In this paper we discuss the optical response due to the excitonic effect of two types of hBN bilayers: AB and AA'. Understanding the properties of these bilayers is of great utility to the study of twisted bilayers at arbitrary angles, since these two configurations correspond to the limit cases of 0 and 60 degree rotation. To obtain the excitonic response we present a method to solve a four-band Bethe-Salpeter equation, by casting it into a 1D problem, thus greatly reducing the numerical burden of the calculation when compared with strictly 2D methods. We find results in good agreement with …
We have studied the excitonic gap formation in the Bernal Stacked, bilayer graphene (BLG) structures at half-filling. Considering the local Coulomb interaction between the layers, we calculate the excitonic gap parameter and we discuss the role of the interlayer and intralayer Coulomb interactions and the interlayer hopping on the excitonic pair formation in the BLG. Particularly, we predict the origin of excitonic gap formation and condensation, in relation to the farthermost interband optical transition spectrum. The general diagram of excitonic phase transition is given, explaining differen…
We report the direct observation of intervalley exciton between the Q conduction valley and $Γ$ valence valley in bilayer WSe$_2$ by photoluminescence. The Q$Γ$ exciton lies at ~18 meV below the QK exciton and dominates the luminescence of bilayer WSe$_2$. By measuring the exciton spectra at gate-tunable electric field, we reveal different interlayer electric dipole moments and Stark shifts between Q$Γ$ and QK excitons. Notably, we can use the electric field to switch the energy order and dominant luminescence between Q$Γ$ and QK excitons. Both Q$Γ$ and QK excitons exhibit pronounced phonon re…
Interlayer valley excitons in bilayer MoS2 feature concurrently large oscillator strength and long lifetime, and hence represent an advantageous scenario for valleytronic applications. However, control of valley pseudospin of interlayer excitons in pristine bilayer MoS2, which lies at the heart of valleytronics, has remained elusive. Here we report the observation of highly circularly polarized photoluminescence from interlayer excitons of bilayer MoS2 with both optical and magnetic addressability. Under excitation of circularly polarized light near exciton resonance, interlayer excitons of bi…
Electron interactions in undoped bilayer graphene lead to instability of the gapless state, `which-layer' symmetry breaking, and energy gap opening at the Dirac point. In contrast to single layer graphene, the bilayer system exhibits instability even for arbitrarily weak interaction. A controlled theory of this instability for realistic dynamically screened Coulomb interactions is developed, with full acount of dynamically generated ultraviolet cutoff. This leads to an energy gap that scales as a power law of the interaction strength, making the excitonic instability readily observable.
Bilayer quantum Hall systems at ν=1 support an excitonic ground state. In addition to the usual charged quasiparticles, this system possesses a condensate degree of freedom: exciton transport. Detection of this neutral transport mode is facilitated by the use of the Corbino multiply-connected geometry in which charge transport is suppressed. We here summarize our recent experiments on Corbino devices which directly demonstrate exciton transport across the bulk of the incompressible ν=1 quantum Hall state.
Biased bilayer graphene, with its easily tunable band gap, presents itself as the ideal system to explore the excitonic effect in graphene based systems. In this paper we study the excitonic optical response of such a system by combining a tight binding model with the solution of the Bethe-Salpeter equation, the latter being solved in a semi-analytical manner, requiring a single numerical quadrature, thus allowing for a transparent calculation. With our approach we start by analytically obtaining the optical selection rules, followed by the computation of the absorption spectrum for the case o…
The large surface-to-volume ratio in atomically thin 2D materials allows to efficiently tune their properties through modifications of their environment. Artificial stacking of two monolayers into a bilayer leads to an overlap of layer-localized wave functions giving rise to a twist angle-dependent hybridization of excitonic states. In this joint theory-experiment study, we demonstrate the impact of interlayer hybridization on bright and momentum-dark excitons in twisted WSe$_2$ bilayers. In particular, we show that the strong hybridization of electrons at the $Λ$ point leads to a drastic reds…
We analyze the lineshape of the quasiparticle photoluminescence of monolayer and bilayer molybdenum ditelluride in temperature- and excitation intensity-dependent experiments. We confirm the existence of a negatively charged trion in the bilayer based on its emission characteristics and find hints for a coexistence of intra- and interlayer trions with a few meV splitting in energy. From the lineshape analysis of exciton and trion emission we extract values for exciton and trion deformation potentials as well as acoustical and optical phonon-limited mobilities in MoTe2, with the mobilities show…
We study the kinetics of 2D Bose gas cooling provided Bose particles interact with 3D phonons. At low temperatures phonon emission is prohibited by the energy and the momentum conservation. We show that both particle-particle scattering and impurity scattering assist the Bose gas cooling.
Experiments aimed at demonstrating Bose-Einstein condensation of excitons in two types of experiments with bilayer structures (coupled quantum wells) are reviewed, with an emphasis on the basic effects. Bose-Einstein condensation implies the existence of a macroscopic coherence, also known as off-diagonal long-range order, and proposed tests and past claims for coherence in these excitonic systems are discussed.
Bilayer electron-hole systems with unequal electron and hole densities are expected to have exciton condensate ground states with spontaneous spin-polarization in both conduction and valence bands. In the absence of spin-orbit and electron-hole exchange interactions there is no coupling between the spin-orientations in the two quantum wells. In this article we show that Rashba spin-orbit interactions lead to unconventional magnetic anisotropies, whose strength we estimate, and to ordered states with unusual quasiparticle spectra.
Spatially indirect excitons with displaced wavefunctions of electrons and holes play a pivotal role in a large portfolio of fascinating physical phenomena and emerging optoelectronic applications, such as valleytronics, exciton spin Hall effect, excitonic integrated circuit and high-temperature superfluidity. Here, we uncover three types of spatially indirect excitons (including their phonon replicas) and their quantum-confined Stark effects in hexagonal boron nitride encapsulated bilayer WSe2, by performing electric field-tunable photoluminescence measurements. Because of different out-of-pla…
We develop a theory of interlayer tunneling in the exciton condensate of bilayer quantum Hall systems, which predicts strongly enhanced, but finite, tunneling conductance peaks near zero bias even at zero temperature. It is emphasized that, though this strongly enhanced tunneling originates from spontaneous interlayer phase coherence, it is fundamentally not the Josephson effect. Because of strong interlayer correlation, the bilayer system behaves as a single system so that conventional tunneling theories treating two layers as independent systems are not applicable. Based on our theory, we co…
We investigate a bilayer system of critical HgTe quantum wells each featuring a spin-degenerate pair of massless Dirac fermions. In the presence of an electrostatic inter-layer Coulomb coupling, we determine the exciton condensate order parameter of the system self-consistently. Calculating the bulk topological $\mathbb Z_2$ invariant of the resulting mean field Hamiltonian, we discover a novel time reversal symmetric topological exciton condensate state coined the helical topological exciton condensate. We argue that this phase can exist for experimentally relevant parameters. Interestingly, …
Understanding the dynamics of excitons in two dimensional semiconductors requires a theory that incorporates the essential physics distinct from their three-dimensional counterparts. In addition to the modified dielectric environment, single-particle states with strongly non-parabolic dispersion appear in many two-dimensional band structures, so that "effective mass" is ill-defined. Focusing on electrostatically-biased bilayer graphene as an example where quartic (and higher) dispersion terms are necessary, we present a semi-analytic theory used to investigate the properties of ground and exci…
Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in this context. However, the weak interaction between these quasiparticles has been a hurdle in this quest. Dipolar excitons provide an attractive strategy to overcome this limitation but are often hindered by their weak oscillator strength. The interlayer dipolar excitons in naturally occurring homobilayer MoS$_2$ alleviates this issue owing to …
The interaction of intralayer and interlayer excitons is studied in a two-dimensional semiconductor, homobilayer MoS$_2$. It is shown that the measured optical susceptibility reveals both the magnitude and the sign of the coupling constants. The interlayer exciton interacts capacitively with the intralayer B-exciton (positive coupling constant) consistent with hole tunnelling from one monolayer to the other. Conversely, the interlayer exciton interacts inductively with the intralayer A-exciton (negative coupling constant). First-principles many-body calculations show that this coupling arises …
While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster time scale in MoSe$_2$ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the $K$ va…
We show how the excitonic features of biaxial MoS2 flakes are very sensitive to biaxial strain. We find a lower bound for the gauge factors of the A exciton and B exciton of (-41 +- 2) meV/% and (-45 +- 2) meV/% respectively, which are larger than those found for single-layer MoS2. Interestingly, the interlayer exciton feature also shifts upon biaxial strain but with a gauge factor that is systematically larger than that found for the A exciton, (-48 +- 4) meV/%. We attribute this larger gauge factor for the interlayer exciton to the strain tunable van der Waals interaction due to the Poisson …
Tunneling spectroscopy reveals evidence for interlayer electron-hole correlations in quantum Hall bilayer two-dimensional electron systems at layer separations near, but above, the transition to the incompressible exciton condensate at total Landau level filling $ν_T=1$. These correlations are manifested by a non-linear suppression of the Coulomb pseudogap which inhibits low energy interlayer tunneling in weakly-coupled bilayers. The pseudogap suppression is strongest at $ν_T=1$ and grows rapidly as the critical layer separation for exciton condensation is approached from above.
The quantum Hall state at total filling factor $ν_T=1$ in bilayer systems realizes an exciton condensate and exhibits a zero-bias tunneling anomaly, similar to the Josephson effect in the presence of fluctuations. In contrast to conventional Josephson junctions, no Fraunhofer diffraction pattern has been observed, due to disorder induced topological defects, so-called merons. We consider interlayer tunneling in the presence of microwave radiation, and find Shapiro steps in the tunneling current-voltage characteristic despite the presence of merons. Moreover, the Josephson oscillations can also…
This tutorial paper reviews some of the physics of quantum Hall bilayers with a focus on the case where there is low or zero tunnelling between the two layers. We describe the interlayer coherent states at filling factors nu=1 and nu=2 as exciton condensates and discuss some of the theory associated with these states.
Spontaneous Polarization Suppression of Exciton-Exciton Annihilation in 3R-Stacked MoS$_2$ Bilayers
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory(橡树岭国家实验室纳米相材料科学中心);Honda Research Institute USA Inc.(本田美国研究院);University of Tennessee at Knoxville(田纳西大学诺克斯维尔分校)
The optical properties of monolayer and bilayer transition metal dichalcogenide semiconductors are governed by excitons in different spin and valley configurations, providing versatile aspects for van der Waals heterostructures and devices. We present experimental and theoretical studies of exciton energy splittings in external magnetic field in neutral and charged WSe$_2$ monolayer and bilayer crystals embedded in a field effect device for active doping control. We develop theoretical methods to calculate the exciton $g$-factors from first principles and tight-binding for all possible spin-va…
The condensation of excitons, bound electron-hole pairs in a solid, into a coherent collective electronic state was predicted over 50 years ago. Perhaps surprisingly, the phenomenon was first observed in a system consisting of two closely-spaced parallel two-dimensional electron gases in a semiconductor double quantum well. At an appropriate high magnetic field and low temperature, the bilayer electron system condenses into a state resembling a superconductor, only with the Cooper pairs replaced by excitons comprised of electrons in one layer bound to holes in the other. In spite of being char…
We demonstrate that counterflowing electrical currents can move through the bulk of the excitonic quantized Hall phase found in bilayer two-dimensional electron systems (2DES) even as charged excitations cannot. These counterflowing currents are transported by neutral excitons which are emitted and absorbed at the inner and outer boundaries of an annular 2DES sample via an Andreev reflection process.
We consider the excitonic effects on the thermal properties in the AB-stacked bilayer graphene. The calculations are based on the bilayer generalization of the usual Hubbard model at the half-filling. The full interaction bandwidth is used without any low-energy assumption. We obtain the unusually high values for the electronic figure of merit even at the room-temperatures which is very promising for the thermoelectric applications of the AB-bilayer structure. We discuss the effects of the interlayer Coulomb interaction and temperature on different thermal parameters in the bilayer graphene an…
Motivated by recent studies that reported the successful synthesis of monolayer Mg(OH)$_{2}$ [Suslu \textit{et al.}, Sci. Rep. \textbf{6}, 20525 (2016)] and hexagonal (\textit{h}-)AlN [Tsipas \textit{et al}., Appl. Phys. Lett. \textbf{103}, 251605 (2013)], we investigate structural, electronic, and optical properties of vertically stacked $h$-AlN and Mg(OH)$_{2}$, through \textit{ab initio} density-functional theory (DFT), many-body quasi-particle calculations within the GW approximation, and the Bethe-Salpeter equation (BSE). It is obtained that the bilayer heterostructure prefers the $AB^{\p…
We study the exciton condensate in zero temperature limit in a special class of electron-hole bilayer systems adjacent to insulating ferromagnetic films. With the self-consistent mean-field approximation, we find that the Rashba spin-orbit interaction in the electron and hole layers can induce the p \pm ip or p pairing states depending on the different magnetization of the overlapped ferromagnetic films. Correspondingly, the topologically nontrivial or trivial phases emerge. Furthermore, in the topologically nontrivial phase, the quasiparticle excitations of the U(1) vortex are attached to fra…
Interaction induced topological states remain one of the fascinating phases in condensed matter physics. The exciton condensate has recently sparked renewed interest due to the discovery of new candidate materials and its driving force to realize exotic topological states. In this work, we explore the exciton orders induced high-order topology in the bilayer quantum spin Hall insulators and find that the topological excitonic corner states can be realized by tuning the gate and magnetic field. When an in-plane Zeeman field is applied to the system, two or four excitonic boundary-obstructed cor…
Several recent experiments have reported an anomalous temperature dependence of the Coulomb drag effect in electron-hole bilayers. Motivated by these puzzling data, we study theoretically a low-density electron-hole bilayer, where electrons and holes avoid quantum degeneracy by forming excitonic molecules. We describe the ionization-recombination crossover between the electron-hole plasma and exciton gas and calculate both the intralayer and drag resistivity as a function of temperature. The latter exhibits a minimum followed by a sharp upturn at low temperatures in a qualitative agreement wit…
Excitons in bilayer transition metal dichalcogenides (2L-TMDs) are Coulomb-bound electron/hole pairs that can be viewed as broadly tunable analogs of atomic or molecular systems. Here, we study the properties of 2L-TMD excitons under strong electric field. To overcome the field limit, reached in previous experiments, we developed a new organic/inorganic molecular gating technique. Our approach allows reaching the field > 0.27 V nm-1, about twice higher than previously available. Under this field inter and intra-layer excitonic are brought into an energetic resonance, allowing us to discover ne…
Nonreciprocal perfect Coulomb drag in electron-hole bilayers: coherent exciton superflow as a diode
Tsung-Dao Lee Institute & School of Physics and Astronomy, Shanghai Jiao Tong University(上海交大李政道研究所与物理与天文学院);Shanghai Branch, Hefei National Laboratory(合肥国家实验室上海分部)
We report an experimental study of temperature-dependent spectral lineshapes of phonon side-band emission stemming from dark excitons in monolayer and bilayer WSe$_{2}$. Using photoluminescence spectroscopy in the range from 4 to 100K, we observe a pronounced asymmetry in the phonon-assisted luminescence from momentum-indirect exciton reservoirs. We demonstrate that the corresponding spectral profiles are distinct from those of bright excitons with direct radiative decay pathways. The lineshape asymmetry reflects thermal distribution of exciton states with finite center-of-mass momenta, charac…
Bilayer electron-hole systems, where carriers in one layer are electrons and carriers in the other are holes, have been actively investigated in recent years with the focus on Bose-Einstein condensation of excitons. This condensation is expected to occur when the layer separation d is much smaller than the interparticle distance r_sa_B within each layer. In this Brief Report, we argue for the existence of a state, Wigner supersolid, in which excitons are phase-coherent but form a Wigner crystal due to dipolar repulsion. We present the qualitative phase diagram of a bilayer system, and discuss …
When two sheets of graphene stack in a twisted bilayer graphene (tBLG) configuration, the resulting constrained overlap between interplanar 2p orbitals produce angle-tunable electronic absorption resonances. Using a novel combination of multiphoton transient absorption (TA) microscopy and TEM, we resolve the resonant electronic structure, and ensuing electronic relaxation inside single tBLG domains. Strikingly, we find that the transient electronic population in resonantly excited tBLG domains is enhanced many fold, forming a major electronic relaxation bottleneck. 2-photon TA microscopy shows…
The ground state of two-dimensional (2D) electron systems with equal low densities of electrons and holes in nearby layers is an exciton fluid. We show that a reservoir for excitons can be established by contacting the two layers separately and maintaining the chemical potential difference at a value less than the spatially indirect band gap. Equilibration between the exciton fluid and the contacts proceeds via a process involving virtual intermediate states in which an unpaired electron or hole occupies a free carrier state in one of the 2D layers. We derive an approximate relationship betwee…
We introduce a design of electrically isolated floating bilayer GaAs quantum wells (QW) in which application of a large gating voltage controllably and highly reproducibly induces charges that remain trapped in the bilayer after removal of the gating voltage. At smaller gate voltages, the bilayer is fully electrically isolated from external electrodes by thick insulating barriers. This design permits full control of the total and differential densities of two coupled 2D electron systems. The floating bilayer design provides a unique approach for studying systems inaccessible by simple transpor…
Twist angle modifies the band alignment, screening, and interlayer (IL) coupling in twisted bilayers (tBLs) of transition metal dichalcogenides. Intermediate misorientation (twist angles > 15 degrees) bilayers (BLs) offer a unique opportunity to tune excitonic behavior within these concurrent physical mechanisms but are seldom studied. In this paper, we measure many-body excitonic complexes in monolayer (ML), natural BL, and tBL WSe2. Neutral biexciton (XX) is observed in tBL, while being undetected in nonencapsulated ML and BL, demonstrating unique effects of disorder screening in tBLs. The X…
We have considered the AB-stacked bilayer graphene Josephson junction. The bilayers are supposed to be in the charge equilibrium states and at the half-filling in each of the electronic layers of the construction and at each value of the external gate. By considering the interacting bilayers in both sides of the junction and by taking into account both intralayer and interlayer Coulomb interaction effects, we have calculated the normal and excitonic tunnel currents through the junction. The electronic band renormalizations have been taken into account, due to the excitonic pairing effects and …
Double-layer electron systems in the quantum Hall regime have excitonic condensate ground states when the layers are close together and the total Landau level filling factor is close to an odd integer. In this paper we discuss the microscopic physics of these states and recent progress toward building a theory of the anomalous collective transport effects that occur in separately contacted bilayers when the condensate is present.
We study the electronic properties of AA-stacked bilayer graphene in a transverse electric field. The strong on-site Coulomb repulsion stabilizes the antiferromagnetic order in such a system. The antiferromagnetic order is suppressed by the transverse bias voltage, at least partially. The inter-plane Coulomb repulsion and non-zero voltage stabilize an exciton order parameter. The exciton order parameter coexists with the antiferromagnetism and can be as large as several tens of meV for realistic values of the bias voltage and interaction constants. The application of a transverse bias voltage …
Interlayer excitons are bound states of electrons and holes confined in separate two-dimensional layers. Due to their repulsive dipolar interaction, interlayer excitons can form a correlated liquid. If another electron-hole bilayer is present, excitons from different bilayers can exhibit mutual attraction. We study such a quadrilayer system by a hypernetted chain formalism. We compute ground state energies, pair correlation functions, and collective mode velocities as functions of the exciton densities. We estimate the critical density for the transition to a paired biexciton phase. For a stro…