We examine the impact of quantum confinement on the interaction potential between two charges in two-dimensional semiconductor nanosheets in solution. The resulting effective potential depends on two length scales, namely the thickness $d$ and an emergent length scale $d^* \equiv εd / ε_{\text{sol}}$, where $ε$ is the permittivity of the nanosheet and $ε_{\text{sol}}$ is the permittivity of the solvent. In particular, quantum confinement, and not electrostatics, is responsible for the logarithmic behavior of the effective potential for separations smaller than $d$, instead of the one-over-distance bulk Coulomb interaction. Finally, we corroborate that the exciton binding energy also depends on the two-dimensional exciton Bohr radius $a_0$ in addition to the length scales $d$ and $d^*$ and analyze the consequences of this dependence.
The combined effect of finite potential barriers and dielectric mismatch between dot and matrix on excitonic properties of semiconductor quantum dots has been studied. To avoid the unphysical divergence in the self-polarization energy which arises for the simplest and profusely adopted step-like model of the dielectric interface, we proposed a realistic (finite size) smooth profile for the dielectric interface. We have found that the excitonic binding energy can be either higher than the corresponding one to complete confinement by infinite barriers or essentially zero for a wide range of dot …
In monolayers of the semiconducting transition metal dichalcogenides, the electron-hole exchange interaction splits the exciton dispersion into a massive transverse branch, and a longitudinal branch that has very light or even zero mass depending on the form of screened Coulomb interaction. The group velocity of the longitudinal branch is sensitive to the strength of electron-hole exchange, which can be engineered through the dielectric environment. Here we show that dielectric patterning of the substrate can be exploited to realize waveguide of the exciton in the longitudinal branch in a homo…
In order to fully exploit the potential of transition metal dichalcogenide monolayers (TMD-MLs), the well-controlled creation of atomically sharp lateral heterojunctions within these materials is highly desirable. A promising approach to create such heterojunctions is the local modulation of the electronic structure of an intrinsic TMD-ML via dielectric screening induced by its surrounding materials. For the realization of this non-invasive approach, an in-depth understanding of such dielectric effects is required. We report on the modulations of excitonic transitions in TMD-MLs through the ef…
Excitons, trions, biexcitons, and exciton-trion complexes in two-dimensional transition metal dichalcogenide sheets of MoS$_2$, MoSe$_2$, MoTe$_2$, WS$_2$ and WSe$_2$ are studied by means of density functional theory and path integral Monte Carlo method in order to accurately account for the particle-particle correlations. In addition, the effect of dielectric environment on the properties of these exciton complexes is studied by modifying the effective interaction potential between particles. Calculated exciton and trion binding energies are consistent with previous experimental and computati…
We theoretically study the effect of the dielectric environment on the exciton ground state of CdSe and CdTe/CdSe/CdTe nanorods. We show that insulating environments enhance the exciton recombination rate and blueshift the emission peak by tens of meV. These effects are particularly pronounced for type-II nanorods. In these structures, the dielectric confinement may even modify the spatial distribution of electron and hole charges. A critical electric field is required to separate electrons from holes, whose value increases with the insulating strength of the surroundings.
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…
Exciton-exciton annihilation (EEA) and Auger recombination are detrimental processes occurring in semiconductor optoelectronic devices at high carrier densities. Despite constituting one of the main obstacles for realizing lasing in semiconductor nanocrystals (NCs), the dependencies on NC size are not fully understood, especially for those with both weakly and strongly confined dimensions. Here, we use differential transmission spectroscopy to investigate the dependence of EEA on the physical dimensions of thickness-controlled 2D halide perovskite nanoplatelets (NPls). We find the EEA lifetime…
Dielectric screening is greatly important to an accurate calculation of the exciton binding energies in two-dimensional materials. In this work, we calculate the dielectric function and 2D polarizability of multilayer (up to three) phosphorene sheets using Density Functional Theory. The 2D polarizabilities are then used in the dielectric screening of the excitonic interaction in multilayer phosphorene quantum dots. In the limit of large quantum dots, excitonic gaps are shown to exhibit very good agreement with state-of-the-art measurements of the optical gaps of multilayer phosphorene sheets d…
Using semi-analytical models we calculate the energy, effective Bohr radius and radiative lifetime of neutral excitons confined in CdSe colloidal nanoplatelets (NPLs). The excitonic properties are largely governed by the electron-hole in-plane correlation, which in NPLs is enhanced by the quasi-two-dimensional motion and the dielectric mismatch with the organic environment. In NPLs with lateral size $L \gtrsim 20$ nm the exciton behavior is essentially that in a quantum well, with superradiance leading to exciton lifetimes of 1 ps or less, only limited by the NPL area. However, for $L < 20$ nm…
In this work, we present a comprehensive theoretical and computational investigation of exciton fine structures of WSe$_2$-monolayers, one of the best known two-dimensional (2D) transition-metal dichalcogenides (TMD's), in various dielectric-layer environments by solving the first-principles-based Bethe-Salpeter equation. While the physical and electronic properties of atomically thin nano-materials are normally sensitive to the variation of surrounding environment, our studies reveal that the influence of dielectric environment on the exciton fine structures of TMD-ML's is surprisingly limite…
The screened Coulomb potential plays a crucial role in the binding energies of excitons in a thin dielectric slab. The asymptotic behavior of this potential is studied when the thickness of the slab is very small as compared to the exciton Bohr radius. A regularized expression is given and the exact effective 2D potential is derived. These expressions may be useful for the computation of the exciton binding energy in 2D or quasi-2D materials.
The optoelectronic and transport properties of two-dimensional transition metal dichalcogenide semiconductors (2D TMDs) are highly susceptible to external perturbation, enabling precise tailoring of material function through post-synthetic modifications. Here we show that nanoscale inhomogeneities known as nanobubbles can be used for both strain and, less invasively, dielectric tuning of exciton transport in bilayer tungsten disulfide (WSe2). We use ultrasensitive spatiotemporally resolved optical scattering microscopy to directly image exciton transport, revealing that dielectric nanobubbles …
Reduced electron screening in two-dimension plays a fundamental role in determining exciton properties, which dictates optoelectronic and photonic device performances. Considering the explicit electron-hole interaction within the $GW-$Bethe-Salpeter formalism, we first study the excitonic properties of pristine phosphorene and investigate the effects of strain and impurity coverage. The calculations reveal strongly bound exciton in these systems with anisotropic spatial delocalization. Further, we present a simplified hydrogenic model with anisotropic exciton mass and effective electron screen…
Theoretical description of the charge transfer (CT) exciton across the donor-acceptor interface without the use of a completely localized hole (or electron) is a challenge in the field of organic solar cells. We calculate the total wavefunction of the CT exciton by solving an effective two-particle Schrodinger equation for the inhomogeneous dielectric interface. We formulate the magnitude of the CT and construct a minimal model of the CT exciton under the breakdown of inversion symmetry. We demonstrate that both a light hole mass and a hole localization along the normal to the dielectric inter…
Based on extensive first principle calculations, we explore the thickness dependent effective di- electric constant and slab polarizability of few layer black phosphorene. We find that the dielectric constant in ultra-thin phosphorene is thickness dependent and it can be further tuned by applying an out of plane electric field. The decreasing dielectric constant with reducing number of layers of phosphorene, is a direct consequence of the lower permittivity of the surface layers and the in- creasing surface to volume ratio. We also show that the slab polarizability depends linearly on the numb…
The exciton and biexciton binding energy have been studied for a ZnSe/ZnS core/shell quantum dot using WKB (Wentzel-Kramers-Brillouin) approximation. The exciton binding energy increases for small shell thickness and for large thickness, the binding energy again starts decreasing. A similar result is obtained for biexcitons where for thicker shells, the biexciton attains antibonding.
Excitons in atomically-thin semiconductors necessarily lie close to a surface, and therefore their properties are expected to be strongly influenced by the surrounding dielectric environment. However, systematic studies exploring this role are challenging, in part because the most readily accessible exciton parameter -- the exciton's optical transition energy -- is largely \textit{un}affected by the surrounding medium. Here we show that the role of the dielectric environment is revealed through its systematic influence on the \textit{size} of the exciton, which can be directly measured via the…
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$_2$). …
Starting from the single-particle Dirac Hamiltonian for charge carriers in monolayer transition metal dichalcogenides (TMDs), we construct a four-band Hamiltonian describing interlayer excitons consisting of an electron in one TMD layer and a hole in the other TMD layer. An expression for the electron-hole interaction potential is derived, taking into account the effect of the dielectric environment above, below, and between the two TMD layers as well as polarization effects in the transition metal layer and in the chalcogen layers of the TMD layers. We calculate the interlayer exciton binding…
There is an ever increasing interest in the development of plasmonic 2D nanomaterials, with widespread applications in optoelectronics, high resolution microscopy, imaging and sensing, among others. With the current ability of ultrathin noble metal film deposition down to a few monolayers in thickness, there is a need for an analytical expression of the thickness dependent complex dielectric function for predicting optical properties for arbitrary thicknesses. The free and bound electron contributions to the dielectric function are dealt with independently, since their influences affect separa…
We demonstrate that, in monolayers (MLs) of semiconducting transition metal dichalcogenides, the $s$-type Rydberg series of excitonic states follows a simple energy ladder: $ε_n=-Ry^*/(n+δ)^2$, $n$=1,2,\ldots, in which $Ry^*$ is very close to the Rydberg energy scaled by the dielectric constant of the medium surrounding the ML and by the reduced effective electron-hole mass, whereas the ML polarizability is only accounted for by $δ$. This is justified by the analysis of experimental data on excitonic resonances, as extracted from magneto-optical measurements of a high-quality WSe$_2$ ML encaps…
The dielectric environment of atomically-thin monolayer (ML) of semiconducting transition metal dichalcogenides affects both the electronic band gap and the excitonic binding energy in the ML. We investigate the effect of the environment on the in-plane magnetic field brightening of neutral and charged dark exciton emissions in the WSe$_2$ ML. The monolayers placed in three dielectric environments are studied, in particular, the ML encapsulated in hexagonal BN (hBN) flakes, the ML deposited on a hBN layer, and the ML embedded between the hBN flake and SiO$_2$/Si substrate. We observe that the …
Establishing the role of thickness in LaOBr; an alternative gate dielectric for vdW heterostructures
Quantum and Nanotechnologies Research Centre, National Research Council Canada（加拿大国家研究委员会量子与纳米技术研究中心）；Department of Physics, University of Ottawa（渥太华大学物理系）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（日本物质材料研究机构材料纳米架构研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（日本物质材料研究机构电子与光学材料研究中心）；Department of Inorganic Chemistry, University of Chemistry and Technology Prague（布拉格化工大学无机化学系）
For atomic thin layer insulating materials we provide an exact analytic form of the two-dimensional screened potential. In contrast to three-dimensional systems where the macroscopic screening can be described by a static dielectric constant in 2D systems the macroscopic screening is non local (q-dependent) showing a logarithmic divergence for small distances and reaching the unscreened Coulomb potential for large distances. The cross-over of these two regimes is dictated by 2D layer polarizability that can be easily computed by standard first-principles techniques. The present results have st…
We report absorption and photoluminescence spectra of Si and SnO$_2$ polycrystalline nanofilms in the UV-Vis-NIR range, featuring discrete bands resulting from transverse quantum confinement. The film thickness ranged 3.9 nm to 12.2 nm, depending on the material. The results are interpreted within the particle-in-a-box model, with the box width equal to the layer mass thickness. The energy levels and transitions scale as the inverse square of the film thickness. The calculated values of the effective electron mass are independent on the film thickness and equal to 0.17m$_o$ (Si) and 0.21m$_o$ …
The multi-quantum well (MQW) organic-inorganic perovskite offer an approach of tuning the exciton binding energy based on the well-barrier dielectric mismatch effect, which called the image charge effect. The exfoliation from MQW organic-inorganic perovskite forms a twodimensional (2D) nano-sheet. As with other 2D materials, like graphene or transition metal dichalcogenides (TMDs), the ultra-thin perovskites layers are highly sensitive to the dielectric environment. We investigate the ultrathin crystalline 2D van-der-Waals (vdW) layers of organic-inorganic perovskite crystals close to a surfac…
Atomically thin semiconductors such as monolayer MoS2 and WS2 exhibit nonlinear exciton-exciton annihilation at notably low excitation densities (below ~10 excitons/um2 in MoS2). Here, we show that the density threshold at which annihilation occurs can be tuned by changing the underlying substrate. When the supporting substrate is changed from SiO2 to Al2O3 or SrTiO3, the rate constant for second-order exciton-exciton annihilation, k_XX [cm2/s], is reduced by one or two orders of magnitude, respectively. Using transient photoluminescence microscopy, we measure the effective room-temperature ex…
Recent advances in emerging atomically thin transition metal dichalcogenide semiconductors with strong light-matter interactions and tunable optical properties provide novel approaches for realizing new material functionalities. Coupling two-dimensional semiconductors with all-dielectric resonant nanostructures represents an especially attractive opportunity for manipulating optical properties in both the near-field and far-field regimes. Here, by integrating single-layer WSe2 and titanium oxide (TiO2) dielectric metasurfaces with toroidal resonances, we realized robust exciton emission enhanc…
We propose a scheme for the spatial exciton energy control and exciton routing in a transition metal dichalcogenide (TMD) monolayer which lies on a quantum paraelectric substrate. It relies on the ultrasensitive response of the substrate dielectric permittivity to temperature changes, allowing for spatially inhomogeneous screening of Coulomb interaction in a monolayer. As an example, we consider the heterostructure of TMD and strontium titanate oxide SrTiO$_3$, where large dielectric screening can be attained. We study the impact of substrate temperature on the characteristic electronic featur…
Atomically thin materials are exceedingly susceptible to their dielectric environment. For transition metal dichalcogenides, sample placement on a substrate or encapsulation in hexagonal boron nitride (hBN) are frequently used. In this paper we show that the dielectric response due to optical phonons of adjacent materials influences excitons in 2d crystals. We provide an analytic model for the coupling of 2d charge carriers to optical substrate phonons, which causes polaron effects similar to that of intrinsic 2d phonons. We apply the model to hBN-encapsulated WSe2, finding a significant reduc…
The effects of substrate on electronic and optical properties of triangular and hexagonal graphene nanoflakes with armchair edges are investigated by using a configuration interaction approach beyond double excitation scheme. The quasiparticle correction to the energy gap and exciton binding energy are found to be dominated by the long-range Coulomb interactions and exhibit similar dependence on the dielectric constant of the substrate, which leads to a cancellation of their contributions to the optical gap. As a result, the optical gaps are shown to be insensitive to the dielectric environmen…
We systematically measure the dielectric function of atomically thin MoS2 films with different layer numbers and demonstrate that excitonic effects play a dominant role in the dielectric function when the films are less than 5-7 layers thick. The dielectric function shows an anomalous dependence on the layer number. It decreases with the layer number increasing when the films are less than 5-7 layers thick but turns to increase with the layer number for thicker films. We show that this is because the excitonic effect is very strong in the thin MoS2 films and its contribution to the dielectric …
Monolayer fluctuations in the thickness of a semiconductor quantum well (QW) lead to three types of excitons, located in the narrower, average and thicker regions of the QW, which are clearly resolved in optical spectra. Whether or not these excitons are coherently coupled via Coulomb interactions is a long-standing debate. We demonstrate that different types of disorder in QWs distinctly affects the coherent coupling and that the coupling strength can be quantitatively measured using optical two-dimensional Fourier transform spectroscopy. We prove experimentally and theoretically that in narr…
In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial --tens of teslas or more-- due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS$_2$, MoSe$_2$, MoTe$_2$, and WS$_2$ in very high magnetic fields to 91~T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton's $1s$ ground state but also …
Interlayer excitons, or bound electron-hole pairs whose constituent quasiparticles are located in distinct stacked semiconducting layers, are being intensively studied in heterobilayers of two dimensional semiconductors. They owe their existence to an intrinsic type-II band alignment between both layers that convert these into p-n junctions. Here, we unveil a pronounced interlayer exciton (IX) in heterobilayers of metal monochalcogenides, namely gamma-InSe on epsilon-GaSe, whose pronounced emission is adjustable just by varying their thicknesses given their number of layers dependent direct ba…
Mostly, optical spectroscopies are used to investigate the physics of excitons, whereas their electrical evidences are hardly explored. Here, we examined a forward bias activated differential capacitance response of GaInP-AlGaInP based multi-quantum well laser diodes to trace the presence of excitons using electrical measurements. Occurrence of negative activation energy after light emission is understood as thermodynamical signature of steady state excitonic population under intermediate range of carrier injections. Similar corroborative results are also observed in an InGaAs-GaAs quantum dot…
We study the eigenenergies and optical properties of both direct excitons in a phosphorene monolayer in different dielectric environments, and indirect excitons in heterostructures of phosphorene with hexagonal boron nitride. For these systems, we solve the 2D Schrödinger equation using the Rytova-Keldysh (RK) potential for direct, and both the RK and Coulomb potentials for indirect excitons. The results show that excitons formed from charge carriers with anisotropic effective mass exhibit enhanced (suppressed) optical absorption, compared to their 2D isotropic counterparts, under linearly pol…
The existence of strongly bound excitons is one of the hallmarks of the newly discovered atomically thin semi-conductors. While it is understood that the large binding energy is mainly due to the weak dielectric screening in two dimensions (2D), a systematic investigation of the role of screening on 2D excitons is still lacking. Here we provide a critical assessment of a widely used 2D hydrogenic exciton model which assumes a dielectric function of the form ε(q) = 1 + 2παq, and we develop a quasi-2D model with a much broader applicability. Within the quasi-2D picture, electrons and holes are d…
We investigate the carrier mobility in mono- and bi-layer graphene with a top HfO2 dielectric, as a function of the HfO2 film thickness and temperature. The results show that the carrier mobility decreases during the deposition of the first 2-4 nm of top dielectric and remains constant for thicker layers. The carrier mobility shows a relatively weak dependence on temperature indicating that phonon scattering does not play a dominant role in controlling the carrier mobility. The data strongly suggest that fixed charged impurities located in close proximity to the graphene are responsible for th…
We develop a non-local dielectric response theory to describe the temperature dependence of exciton lifetime in metal-semiconductor heterostructures. Coupling between excitons and surface plasmons results in a strongly nonmonotonous behaviour of exciton radiative decay rate versus temperature. Tuning the plasmon frequency one can control the efficiency of exciton emission of light.
We theoretically analyse the hybrid Mie-exciton optical modes arising from the strong coupling of excitons in organic dyes or transition-metal dichalcogenides with the Mie resonances of high-index dielectric nanoparticles. Detailed analytic calculations show that silicon--exciton core--shell nanoparticles are characterised by a richness of optical modes which can be tuned through nanoparticle dimensions to produce large anticrossings in the visible or near infrared, comparable to those obtained in plexcitonics. The complex magnetic-excitonic nature of these modes is understood through spectral…
A self-consistent scheme for the calculations of the interacting groundstate and the near bandgap optical spectra of mono- and multilayer transition-metal-dichalcogenide systems is presented. The approach combines a dielectric model for the Coulomb interaction potential in a multilayer environment, gap equations for the renormalized groundstate, and the Dirac-Wannier-equation to determine the excitonic properties. To account for the extension of the individual monolayers perpendicular to their basic plane, an effective thickness parameter in the Coulomb interaction potential is introduced. Num…
The problem of a size quantization for charge carriers in a planar quantum well consisting of different monolayers of transition metal dichalcogenides is solved using the Dirac model and the four-band model. For excitons, bound states of electrons and holes at the size quantization levels in such a quantum well, the energy spectrum was found in two cases: the Bohr radius is much smaller than the width of the quantum well (dielectric permeability of a substrate is relatively small) and the Bohr radius is much larger than it (the case of a strong dielectric screening). It is shown that the energ…
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…
We study the size-dependent exciton fine structure in monolayer black phosphorus quantum dots (BPQDs) deposited on different substrates (isolated, Si and SiO$_2$) using a combination of tight-binding method to calculate the single-particle states, and the configuration interaction formalism to determine the excitonic spectrum. We demonstrate that the substrate plays a dramatic role on the excitonic gaps and excitonic spectrum of the QDs. For reasonably high dielectric constants ($\varepsilon_{sub} \sim \varepsilon_{Si} = 11.7 \varepsilon_0$), the excitonic gap can be described by a single powe…
The formation of pulses of surface electromagnetic waves in a metal/dielectric interface is considered in the process of cooperative decay of excitons of quantum dots distributed near a metal surface in a dielectric layer. It is shown that the efficiency of exciton energy transfer to excited plasmons can be increased by selecting the dielectric material with specified values of the complex permittivity. It is found that in the mean field approximation the semiclassical model of formation of plasmon pulses in the system under study is reduced to the pendulum equation with the additional term of…
The excitonic behavior of anisotropic two-dimensional crystals is investigated using numerical methods. We employ a screened potential arising due to the system polarizability to solve the central-potential problem using the Numerov approach. The dependence of the exciton energies on the interaction strength and mass anisotropy is demonstrated. We use our results to obtain the exciton binding energy in phosphorene as a function of the substrate dielectric constant.
