Indirect Excitons Research Articles

Tuning moiré excitons in Janus heterobilayers for high-temperature Bose-Einstein condensation.

Using first-principles calculations, we predict that moiré excitons in twisted Janus heterobilayers could realize tunable and high-temperature Bose-Einstein condensation (BEC). The electric dipole in the Janus heterobilayers leads to charge-transfer interlayer and intralayer moiré excitons with exceptionally long lifetimes, in the absence of spacer layers. The electric dipole is also expected to enhance exciton-exciton repulsions at high exciton densities and can modulate moiré potentials that trap excitons for their condensation. The key parameters for exciton condensation, including exciton Bohr radius, binding energy, effective mass, and critical Mott density, are examined as a function of the twist angle. Last, exciton phase diagrams for the Janus heterobilayers are constructed from which one can estimate the BEC (>100 K) and superfluid (~30 K) transition temperatures. In addition to indirect interlayer excitons, we find that direct intralayer excitons can also condense at high temperatures, consistent with experiments.

Temperature behavior of the near band edge luminescence in CsPbBr3 single crystal and nanoparticle ensemble

The temperature dependences of the luminescence spectra for CsPbBr3 single crystal and nanoparticle ensemble are presented. The emission bands of single crystal are interpreted in terms of the direct and indirect exciton transitions. An attempt to estimate the contribution of the direct and indirect transitions for wide luminescence band inherent for CsPbBr3 nanoparticles is made. The temperature dependence of the luminescence band position is analyzed by the taking into account the thermal expansion and exciton-phonon interaction. For both the single crystal and the ensemble of nanoparticles, main contribution to the shift of the luminescence bands of the direct and indirect excitons to the low-energy region was revealed to be caused by the interaction with optical phonons. This interaction is predominant for the indirect excitons and can be used as a sign of Rashba nature of the exciton.

A Pair of 2D Quantum Liquids: Investigating the Phase Behavior of Indirect Excitons.

Long-lived indirect excitons (IXs) exhibit a rich phase diagram, including a Bose–Einstein condensate (BEC), a Wigner crystal, and other exotic phases. Recent experiments have hinted at a “classical” liquid of IXs above the BEC transition. To uncover the nature of this phase, we use a broad range of theoretical tools and find no evidence of a driving force toward classical condensation. Instead, we attribute the condensed phase to a quantum electron–hole liquid (EHL), first proposed by Keldysh for direct excitons. Taking into account the association of free carriers into bound excitons, we study the phase equilibrium between a gas of excitons, a gas of free carriers, and an EHL for a wide range of electron–hole separations, temperatures, densities, and mass ratios. Our results agree reasonably well with recent measurements of GaAs/AlGaAs coupled quantum wells.

Excitonic Tonks-Girardeau and charge density wave phases in monolayer semiconductors

Excitons in two-dimensional semiconductors provide a novel platform for fundamental studies of many-body interactions. In particular, dipolar interactions between spatially indirect excitons may give rise to strongly correlated phases of matter that so far have been out of reach of experiments. Here, we show that excitonic few-body systems in atomically thin transition-metal dichalcogenides undergo a crossover from a Tonks-Girardeau to a charge-density-wave regime. To this end, we take into account realistic system parameters and predict the effective exciton-exciton interaction potential. We find that the pair correlation function contains key signatures of the many-body crossover already at small exciton numbers and show that photoluminescence spectra provide readily accessible experimental fingerprints of these strongly correlated quantum many-body states.

Superfluid drag between excitonic polaritons and superconducting electron gas

The Andreev-Bashkin effect, or superfluid drag, is predicted in a system of Bose-condensed excitonic polaritons in optical microcavity coupled by electron-exciton interaction with a superconducting layer. Two possible setups with spatially indirect dipole excitons or direct excitons are considered. The drag density characterizing a magnitude of this effect is found by many-body calculations with taking into account dynamical screening of electron-exciton interaction. For the superconducting electronic layer, we assume the recently proposed polaritonic mechanism of Cooper pairing, although the preexisting thin-film superconductor should also demonstrate the effect. According to our calculations, the drag density can reach considerable values in realistic conditions, with excitonic and electronic layers made from GaAs-based quantum wells or two-dimensional transition metal dichalcogenides. The predicted nondissipative drag could be strong enough to be observable as induction of a supercurrent in the electronic layer by a flow of polariton Bose condensate.

Intervalley electron-hole exchange interaction and impurity-assisted recombination of indirect excitons in WS2 and WSe2 monolayers

The variety of excitonic states in tungsten-based dichalcogenide monolayers stems from unique interplay between the spin and valley degrees of freedom. One of the exciton species is the indirect exciton (momentum or valley dark), which is responsible for a series of resonances when the monolayer is charge neutral. We investigate the short-range electron-hole exchange interaction of the indirect exciton, as well as its recombination mechanism mediated by impurities. The analysis provides thorough understanding of the energy and polarization of the zero-phonon indirect exciton resonance in the emission spectrum.

Strain-Induced Exciton Hybridization in WS2 Monolayers Unveiled by Zeeman-Splitting Measurements

Mechanical deformations and ensuing strain are routinely exploited to tune the band gap energy and to enhance the functionalities of two-dimensional crystals. In this Letter, we show that strain leads also to a strong modification of the exciton magnetic moment in WS_{2} monolayers. Zeeman-splitting measurements under magnetic fields up to 28.5 T were performed on single, one-layer-thick WS_{2} microbubbles. The strain of the bubbles causes a hybridization of k-space direct and indirect excitons resulting in a sizable decrease in the modulus of the g factor of the ground-state exciton. These findings indicate that strain may have major effects on the way the valley number of excitons can be used to process binary information in two-dimensional crystals.

Effect of electric bias on trapping and release of excitons in GaN/(Al,Ga)N quantum wells

A giant built-in electric field in the growth direction makes excitons in wide GaN/(Al, Ga)N quantum wells spatially indirect even in the absence of any external bias. Significant densities of indirect excitons can accumulate in electrostatic traps imprinted in the quantum well plane by a thin metal layer deposited on top of the heterostructure. By jointly measuring spatially resolved photoluminescence and photo-induced current, we demonstrate that exciton density in the trap can be controlled via an external electric bias, which is capable of altering the trap depth. Application of a negative bias deepens the trapping potential, but does not lead to any additional accumulation of excitons in the trap. This is due to exciton dissociation instigated by the lateral electric field at the electrode edges. The resulting carrier losses are detected as an increased photocurrent and reduced photoluminescence intensity. By contrast, application of a positive bias washes out the electrode-induced trapping potential. Thus, excitons get released from the trap and recover free propagation in the plane that we reveal by spatially resolved photoluminescence.

Collective interlayer pairing and pair superfluidity in vertically stacked layers of dipolar excitons

Layered bosonic dipolar fluids have been suggested to host a condensate of interlayer molecular bound states. However, experimental observation has remained elusive. Motivated by two recent experimental works [C. Hubert et al., Phys. Rev. X9, 021026 (2019) and D. J. Choksy et al., Phys. Rev. B 103, 045126 (2021)], we theoretically study, using numerically exact quantum Monte Carlo calculations, the experimental signatures of collective interlayer pairing in vertically stacked indirect exciton (IX) layers. We find that IX energy shifts associated with each layer evolve nontrivially as a function of density imbalance following a nonmonotonic trend with a jump discontinuity at density balance, identified with the interlayer IX molecule gap. This behavior discriminates between the superfluidity of interlayer bound pairs and independent dipole condensation in distinct layers. Considering finite temperature and finite density imbalance conditions, we find a cascade of Berezinskii-Kosterlitz-Thouless (BKT) transitions, initially into a pair superfluid and only then, at lower temperatures, into complete superfluidity of both layers. Our results may provide a theoretical interpretation of existing experimental observations in GaAs double quantum well (DQW) bilayer structures. Furthermore, to optimize the visibility of pairing dynamics in future studies, we present an analysis suggesting realistic experimental settings in GaAs and transition metal dichalcogenide (TMD) bilayer DQW heterostructures where collective interlayer pairing and pair superfluidity can be clearly observed.

Phonon-assisted broadening in Bernal boron nitride: A comparison between indirect and direct excitons

We study the deep-ultraviolet emission in Bernal boron nitride as a function of temperature. The quasidegeneracy of indirect and direct excitons in Bernal boron nitride leads to their simultaneous recombination, allowing a comparison of phonon-assisted broadening in the two cases. Temperature-dependent measurements reveal that below 200 K, the efficiency of phonon-assisted broadening is one order of magnitude lower for the direct transition at 6.035 eV than for the phonon replicas of the indirect exciton. This striking effect results from the inhibition of quasielastic acoustic phonon scattering in the strong-coupling regime of the light-matter interaction, where the density of final states is reduced by the curvature of the polaritonic dispersion.

Anisotropic magnetoexcitons in two-dimensional transition metal trichalcogenide semiconductors

Direct and indirect excitons in Rydberg states in transition metal trichalcogenide (TMTC) monolayers, bilayers, and van der Waals (vdW) heterostructures in an external magnetic field are studied within the framework of the effective mass approximation. Binding energies of magnetoexcitons are calculated using the Rytova-Keldysh potential for direct magnetoexcitons and both the Rytova-Keldysh and Coulomb potentials for indirect magnetoexcitons. We report the magnetic field energy contribution to the binding energies and diamagnetic coefficients for magnetoexcitons that depend strongly on the effective mass anisotropy of electrons and holes. The comparative study of TMTCs and phosphorene is given. In ${\mathrm{TiS}}_{3}$, ${\mathrm{TiSe}}_{3}$, and ${\mathrm{ZrSe}}_{3}$ the excitonic binding energies and diamagnetic coefficients demonstrate the same kind of anisotropy as in phosphorene. In contrast, ${\mathrm{ZrS}}_{3}$ has the opposite anisotropy to phosphorene. The tunability of the binding energy of direct and indirect magnetoexcitons by the external magnetic field and the possibility to control the binding energy of magnetoexcitons in vdW heterostructures by manipulation of numbers of hBN monolayers are shown.

Spatially indirect excitons and exciton quasimolecules in nanosystems with double quantum dots

In mini-review, deals with the theory of exciton quasimolecules in a nanosystem consisting of double quantum dots of germanium synthesized in a silicon matrix. An exciton quasimolecule was formed as a result of the interaction of two spatially indirect excitons. It is shown that, depending on the distance D between the surfaces of the quantum dots, spatially indirect excitons and of exciton quasimolecules was formed in the nanosystem. The binding energy of the singlet ground state of the exciton quasimolecule has been gigantic exceeding the binding energy of the biexciton in a silicon single crystal by almost two orders of magnitude. The emergence of a band of localized electron states in the band gap of the silicon matrix was found. This band of localized electron states appeared as a result of the splitting of electron levels in the chain of germanium quantum dots.

Recombination dynamics of indirect excitons in hexagonal BN epilayers containing polytypic segments grown by chemical vapor deposition using carbon-free precursors

Hexagonal (h) BN is a semiconductor that crystallizes in layers of a two-dimensional honeycomb structure. Since hBN exhibits high quantum efficiency (QE) near-band edge emission at around 5.8 eV in spite of the indirect bandgap, hBN has a potential for the use in deep-ultraviolet light emitters. For elucidating the emission dynamics of indirect excitons (iXs) in hBN, spatially and temporally resolved luminescence measurements were carried out on hBN epilayers grown using carbon-free precursors. In addition to major μm-side flat-topped (0001) hBN columnar grains, sub-μm-scale polytypic segments were identified, which were likely formed by certain growth instabilities. The hBN domains exhibited predominant emissions of phonon-assisted fundamental iXs at 5.7–5.9 eV and a less-pronounced 4.0-eV emission band. The photoluminescence lifetime (τPL) for the iX emissions was 54 ps, which most likely represents the midgap recombination lifetime (τMGR) for an iX reservoir. Because τPL did not change while the cathodoluminescence (CL) intensity increased with temperature above 100 K, both the immobile character of iXs and strong exciton–phonon interaction seem significant for procreating the high QE. The CL intensity and τPL of the 5.5 eV band monotonically decreased with temperature, indicating that τPL represents τMGR, most probably a nonradiative lifetime, around the real states. Equally significant emissions at 6.035 eV at 12 K and 6.0–6.1 eV at 300 K were observed from the polytypic segments, most probably graphitic bernal BN, which also exhibited negligible thermal quenching property.

Transient surface photovoltage spectroscopy of diamond

Contactless and highly sensitive probing of electronic transitions in diamond over a wide spectral range from near infrared to deep ultraviolet is still challenging. Surface photovoltage (SPV) signals depend on electronic transitions and transport phenomena leading to charge separation in space and allow for a contactless study of electronic transitions. Here, transient SPV spectroscopy in an arrangement with a charge amplifier and a laser tunable over a wide range was applied to study an undoped diamond single crystal between 0.8 and 5.9 eV at room temperature in ambient air. SPV transients were measured without and with weak visible bias light, which allowed for suppression of possible parasitic contributions in SPV signals not related to diamond and distinction of processes of charge separation that were independent of band bending. Transitions at 1.0 and 3.1 eV led to preferential separation of photogenerated holes toward the surface. In contrast, a transition at 1.8 eV caused preferential separation of photogenerated electrons toward the surface. Transitions near the indirect bandgap of diamond were observed at 5.27, 5.32, 5.48, and 5.53 eV and could be assigned to absorption assisted (i) by an indirect exciton and absorption of longitudinal optical and acoustic phonons, (ii) by absorption of transverse acoustic phonons, (iii) by emission of transverse acoustic phonons, and (iv) by emission of longitudinal optical and acoustic phonons, respectively. Charge separation under excitation at 5.27 eV was caused by directed charge transfer at/near the diamond surface after exciton diffusion followed by exciton dissociation.

Properties of Spatially Indirect Excitons in Nanowire Arrays

This paper deals with the excitons formed by electrons and holes located in different, closely placed semiconducting nanowires (spatially indirect excitons). We calculated the charge densities and the binding energies of the excitons for different nanowire diameters D and distances h between the nanowires. Together with the estimated exciton lifetimes, these results suggest that at certain h and D, the spatially indirect excitons in the nanowire arrays may have the potential to serve as information-processing units. Possible ways of exciton generation in the nanowire arrays are discussed.

Interlayer Coupling and Pressure Engineering in Bilayer MoS2

Controlling the interlayer coupling by tuning lattice parameters through pressure engineering is an important route for tailoring the optoelectronic properties of two-dimensional materials. In this work, we report a pressure-dependent study on the exciton transitions of bilayer MoS2 exfoliated on a diamond anvil surface. The applied hydrostatic pressure changes from ambient pressure up to 11.05 GPa using a diamond anvil cell device. Raman, photoluminescence, and reflectivity spectra at room temperature are analyzed to characterize the interlayer coupling of this bilayer system. With the increase of pressure, the indirect exciton emission disappears completely at about 5 GPa. Importantly, we clearly observed the interlayer exciton from the reflectivity spectra, which becomes invisible at a low pressure around 1.26 GPa. This indicates that the interlayer exciton is very sensitive to the hydrostatic pressure due to the oscillator strength transfer from the direct transition to the indirect one.

Excitonic effects in graphene-like C3N

Monolayer ${\mathrm{C}}_{3}\mathrm{N}$ is an emerging two-dimensional indirect band gap semiconductor with interesting mechanical, thermal, and electronic properties. In this paper we present a description of ${\mathrm{C}}_{3}\mathrm{N}$ electronic and dielectric properties, focusing on the so-called momentum-resolved exciton band structure. Excitation energies and oscillator strengths are computed in order to characterize bright and dark states, and discussed also with respect to the crystal symmetry. Activation of excitonic states is observed for finite transferred momenta: Indeed, we find an active indirect exciton at $\ensuremath{\sim}$ 0.9 eV, significantly lower than the direct optical gap of 1.96 eV, with excitonic binding energies in the range 0.6--0.9 eV for the lowest states. As for other 2D materials, we find a quasilinear excitonic dispersion close to $\mathrm{\ensuremath{\Gamma}}$, which however shows a downward convexity related to the indirect band gap of ${\mathrm{C}}_{3}\mathrm{N}$ as well as to the dark nature of the involved excitons.

Two-dimensional confinement of excitons at the interface in nonpolar MgZnO/ZnO heterostructures

We report on the polarity-dependent excitonic emission at the interface in MgZnO/ZnO heterostructures grown on both polar and nonpolar ZnO single-crystal substrates. Structural and morphological analyses confirm that the heterostructures grow homoepitaxially on nonpolar $m$-plane and $a$-plane crystal substrates. The nonpolar heterostructures are investigated by depth-resolved cathodoluminescence spectroscopy revealing an excitonic interface emission centered at 3.12 eV, identified as the $H$-band signature of indirect excitons. These results reveal the formation of robust indirect excitons confined at the MgZnO/ZnO interface due to the presence of an epitaxially strained interfacial layer near the interface in the MgZnO, which is confirmed by high-order x-ray diffraction. It is also found that the $H$-band emission originates from the self-absorption of the ZnO free exciton emission in the proximity of the interface. Temperature-dependent studies of the $H$ band yields a thermal activation energy of 47 meV for the indirect exciton in the nonpolar heterojunctions. This activation energy is the largest among all free and bound excitons in ZnO and is much higher than the values found in AlGaN/GaN and MgZnO/ZnO/sapphire hetrostructures. Our findings indicate that the optical properties of nonpolar heterostructures are strongly influenced by the piezoelectric effect.

Magnetoexcitons in phosphorene monolayers, bilayers, and van der Waals heterostructures

We study direct and indirect excitons in Rydberg states in phosphorene monolayers, bilayers, and van der Waals (vdW) heterostructure in an external magnetic field within the framework of the effective-mass approximation. The magnetic field is applied perpendicular to the monolayer or heterostructure and is varied between 0 and 60 T. Binding energies of magnetoexcitons are calculated by numerical integration of the Schr\"odinger equation using the Rytova-Keldysh potential for direct magnetoexcitons and both the Rytova-Keldysh and Coulomb potentials for indirect magnetoexcitons. The latter aids in the understanding of the role of screening in phosphorene. We report the magnetic field energy contribution to the binding energies and diamagnetic coefficients (DMCs) for magnetoexcitons, which depend strongly on the effective anisotropic masses of electrons and holes and can be tuned by the external magnetic field. We demonstrate that the vdW phosphorene heterostructure is a novel category of two-dimensional semiconductors with magnetoexcitonic binding energies tunable by means of the external magnetic field. The binding energies and DMCs are controlled by the number of hexagonal boron nitride layers separating two phosphorene sheets. Such tunability is potentially useful for the device design.

Strain-induced quantum Hall phenomena of excitons in graphene

We study direct and indirect pseudomagnetoexcitons, formed by an electron and a hole in the layers of gapped graphene under strain-induced gauge pseudomagnetic field. Since the strain-induced pseudomagnetic field acts on electrons and holes the same way, it occurs that the properties of single pseudomagnetoexcitons, their collective effects and phase diagram are cardinally different from those of magnetoexcitons in a real magnetic field. We have derived wave functions and energy spectrum of direct in a monolayer and indirect pseudomagnetoexcitons in a double layer of gapped graphene. The quantum Hall effect for direct and indirect excitons was predicted in the monolayers and double layers of gapped graphene under strain-induced gauge pseudomagnetic field, correspondingly.