We analyze the many-particle correlations that affect the optical properties of two-dimensional semiconductors. These correlations manifest themselves through the specific optical resonances such as excitons, trions, etc. Starting from the generic electron-hole Hamiltonian and employing the microscopic Heisenberg equation of motion the infinite hierarchy of differential equations can be obtained. In order to decouple the system we address the cluster expansion technique which provides a regular procedure of consistent accounting of many-particle correlation contributions into the interband polarization dynamics. In particular, the partially taken into account three-particle correlations modify the behavior of absorption spectra with the emergence of a trion-like peak additional to excitonic ones. In contrast to many other approaches, the proposed one allows us to model the optical response of 2d semiconductors in the regime when the Fermi energies are of the order of the exciton and trion binding energies, thus allowing us to rigorously model the onset of the excitonic Mott transition, the regime being recently studied in various 2d semiconductors, such as transition metal dichalcogenides.
Mostly optical spectroscopies are used to investigate existence of excitons, Mott transitions and other exquisite excitonic condensed phases of matter. On the other hand, electrical signatures of excitons are hardly explored. Here we examine steady state, small signal, electrical response of AlGaInP based multi-quantum well laser diodes to identify and investigate the presence of excitons in electroluminescence. This frequency dependent response shows bias activated capacitance following a phenomenological rate equation. Dynamic dependence of this response on frequency reverses after light emi…
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 …
Excitonic properties in the Kagome lattice system, which is produced by quantum wires on semiconductor surfaces, are investigated by using the exact diagonalization of a tight binding model. It is shown that due to the existence of flat bands the binding energy of exciton becomes remarkably large in the two-dimensional Kagome lattice compared to that in one-dimensional lattice, and the exciton Bohr radius is quite small as large as a lattice constant. We also discuss the magnetic field effects on the exciton binding energy and the stability of exciton against the creation of charged exciton an…
Some basic radiative and non-radiative processes taking place in semiconductor nanocrystals are discussed, and rates of these processes are calculated. In particular, in the present review we explore both intra-crystallite processes, such as the photon emission, Auger recombination, phonon-assisted exciton relaxation, capture on surface defects, multi-exciton generation, and inter-crystallite processes realized through the exciton migration in ensembles of nanocrystals. Exciton transitions, creation, and annihilation accompanied by the photon and (or) phonon emission or absorption are consider…
We present a scheme to realize the chiral topological excitonic insulator in semiconductor heterostructures which can be experimentally fabricated with a coupled quantum well adjacent to twoferromagnetic insulating films. The different mean-field chiral topological orders, which are due to the change in the directions of the magnetization of the ferromagnetic films, can be characterized by the TKNN numbers in the bulk system as well as by the winding numbers of the gapless states in the edged system. Furthermore, we propose an experimental scheme to detect the emergence of the chiral gapless e…
We present a comprehensive theoretical description of quantum well exciton-polaritons imbedded in a planar semiconductor microcavity. The exact non-local dielectric response of the quantum well exciton is treated in detail. The 4-spinor structure of the hole subband in the quantum well is considered, including the pronounced band mixing effect. The scheme is self-contained and can be used to treat different semiclassical aspects of the microcavity properties. As an example, we analyze the "selection" rules for the exciton-cavity mode coupling for different excitons.
One of the most striking features of novel 2D semiconductors (e.g., transition metal dichalcogenide monolayers or phosphorene) is a strong Coulomb interaction between charge carriers resulting in large excitonic effects. In particular, this leads to the formation of multi-carrier bound states upon photoexcitation (e.g., excitons, trions and biexcitons), which could remain stable at near-room temperatures and contribute significantly to optical properties of such materials. In the present work we have used the Path Integral Monte Carlo methodology to numerically study properties of multi-carrie…
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…
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 use a configuration interaction approach within the envelope function approximation to study the nature of the excitonic resonance in nano-hybrids, composite nanoparticles (NPs) combining a semiconducting and a metallic segment in contact. With reference to recent experimental reports, we specifically study CdS-based nanorods with metallic NPs deposited at the tips (matchstick) or metallic coatings (core-shell). The excitonic states are computed taking into account both the renormalization of the electron-hole interaction and self-energy effects induced by the the metallic segment on the el…
A microscopic approach is developed to compute the excitonic properties and the corresponding terahertz response for semiconductors characterized by anisotropic effective masses. The approach is illustrated for the example of germanium where it is shown that the anisotropic electron mass in the L-valley leads to two distinct terahertz absorption resonances separated by 0.8 meV.
The interaction of optically excited excitons in atomically thin semiconductors with residual doping densities leads to many-body effects which are continuously tunable by external gate voltages. Here, we develop a fully microscopic theory to describe the doping-dependent manipulation of the excitonic properties in atomically thin transition metal dichalcogenides. In particular, we establish a diagonalization approach for the Schrödinger equation which characterizes the interaction of a virtual exciton with the Fermi sea of dopants. Solving this many-body Schrödinger equation provides access t…
The use of ultrafast gating techniques allows us to resolve both spectrally and temporally the emission from short-lived neutral and negatively charged biexcitons in ultrasmall (sub-10 nm) CdSe nanocrystals (nanocrystal quantum dots). Because of forced overlap of electronic wave functions and reduced dielectric screening, these states are characterized by giant interaction energies of tens (neutral biexcitons) to hundreds (charged biexcitons) of meV. Both types of biexcitons show extremely short lifetimes (from sub-100 picoseconds to sub-picosecond time scales) that rapidly shorten with decrea…
We present a new exciton-based formalism for calculating the coherent response of asymmetric semiconductor multiple quantum well structures to ultra-short optical pulses valid to infinite order in the optical field and including the self-generated intraband fields. We use these equations to calculate and explain the oscillations with time delay of peaks in the spectrally-resolved degenerate four wave mixing signals from biased semiconductor superlattices, obtaining good agreement with experiment.
Strain engineering is a powerful tool for tuning physical properties of 2D materials, including monolayer transition metal dichalcogenides (TMD) -- direct bandgap semiconductors with strong excitonic response. Here, we demonstrate an approach for local characterization of strain-induced modification of excitonic photoluminescence in TMD-based materials. We reversibly stress a monolayer of MoSe$_2$ with an AFM tip and perform spatio-spectral mapping of the excitonic photoluminescence in the vicinity of the indentation point. To fully reproduce the experimental data, we introduce the linear depe…
We present quantum yield measurements of single layer $\textrm{WSe}_2$ (1L-$\textrm{WSe}_2$) integrated with high-Q ($Q>10^6$) optical microdisk cavities, using an efficient ($η>$90%) near-field coupling scheme based on a tapered optical fiber. Coupling of the excitonic emission is achieved by placing 1L-WSe$_2$ to the evanescent cavity field. This preserves the microresonator high intrinsic quality factor ($Q>10^6$) below the bandgap of 1L-WSe$_2$. The nonlinear excitation power dependence of the cavity quantum yield is in agreement with an exciton-exciton annihilation model. The cavity quant…
Excitonic contributions to absorption and photocurrent generation in semiconductor nanostructures are described theoretically and simulated numerically using steady-state non-equilibrium Green's function theory. In a first approach, the coherent interband polarization including Coulomb corrections is determined from a Bethe-Salpeter-type equation for the equal time interband single-particle charge carrier Green's function. The effects of excitonic absorption on photocurrent generation are considered on the same level of approximation via the derivation of the corresponding corrections to the e…
Time-resolved soft-X-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe$_2$. We present a many-body approximation for the Green's function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels reveals a delayed core-hole renormalization due to screening by excited quasi-free carriers, revealing an excitonic Mott transition. These findings establish time-resolved core-level photoelectron spectr…
This letter assigns the Faraday rotation in photoexcited semiconductors to ``Pauli interactions'', \emph{i}. \emph{e}., carrier exchanges, between the real excitons present in the sample and the virtual excitons coupled to the $σ_{\pm}$ parts of a linearly polarized light. While \emph{direct Coulomb} interactions scatter bright excitons into bright excitons, whatever their spins are, \emph{Pauli} interactions do it for bright excitons \emph{with same spin only}. This makes these Pauli interactions entirely responsible for the refractive index difference, which comes from processes in which the…
The exciton states in strained (In,Ga)As nanorings embedded in a GaAs matrix are computed. The strain distribution is extracted from the continuum mechanical model, and the exact diagonalization approach is employed to compute the exciton states. Weak oscillations of the ground exciton state energy with the magnetic field normal to the ring are an expression of the excitonic Aharonov-Bohm effect. Those oscillations arise from anticrossings between the ground and the second exciton state and can be enhanced by increasing the ring width. Simultaneously, the oscillator strength for exciton recomb…
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…
A fully microscopic theory for the spontaneous emission from semiconductors is discussed. The theory is evaluated for a quantum-well system and the role of excitonic and unbound electron-hole-pair contributions to the emission is analyzed. Simplifying aproximations to the full theory and their range of validity are discussed. Numerical solutions are presented for experimentally relevant situations and it is shown that a detailed analysis of measured spectra requires the knowledge of both absorption and emission under identical conditions.
Two-dimensional (2D) transition metal dichalcogenides (TMDs) exhibit novel electrical and optical properties and are emerging as a new platform for exploring 2D semiconductor physics. Reduced screening in 2D results in dramatically enhanced electron-electron interactions, which have been predicted to generate giant bandgap renormalization and excitonic effects. Currently, however, there is little direct experimental confirmation of such many-body effects in these materials. Here we present an experimental observation of extraordinarily large exciton binding energy in a 2D semiconducting TMD. W…
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…
Monolayer transition metal dichalcogenides (TMDs) possess superior optical properties, including the valley degree of freedom that can be accessed through the excitation light of certain helicity. While WS2 and WSe2 are known for their excellent valley polarization due to the strong spin-orbit coupling, the optical bandgap is limited by the ability to choose from only these two materials. This limitation can be overcome through the monolayer alloy semiconductor, WS2xSe2(1-x), which promises an atomically thin semiconductor with tunable bandgap. In this work, we show that the high-quality BN en…
We show that electron-hole correlation can be used to tune interband and intraband optical transition rates in semiconductor nanostructures with at least one weakly confined direction. The valence-to-conduction band transition rate can be enhanced by a factor $(L/a_B)^{N}$ -- with $L$ the length of the weakly confined direction, $a_B$ the exciton Bohr radius and $N$ the dimensionality of the nanostructure -- while the rate of intraband and inter-valence-band transitions can be slowed down by the inverse factor, $(a_B/L)^{N}$. Adding a hitherto underexplored degree of freedom to engineer excito…
When monolayers of two-dimensional (2D) materials are stacked into van der Waals structures, interlayer electronic coupling can introduce entirely new properties, as exemplified by recent discoveries of moiré bands that host highly correlated electronic states and quantum dot-like interlayer exciton lattices. Here we show the magnetic control of interlayer electronic coupling, as manifested in tunable excitonic transitions, in an A-type antiferromagnetic 2D semiconductor CrSBr. Excitonic transitions in bilayer and above can be drastically changed when the magnetic order is switched from layere…
Excitonic insulators conduct neither electrons nor holes but bound electron-hole pairs, excitons. Unfortunately, it is not possible to inject and detect the electron and hole currents independently within a single semiconducting layer. However, interlayer excitonic insulators provide a spatial separation of electrons and holes enabling exciton current measurements. The problem is that the spatial separation weakens electron-hole pairing and may lead to interlayer exciton disassociation. Here we develop an explicitly solvable model to determine an interlayer separation that is strong enough to …
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 …
We study theoretically the effect of the fermion and boson densities on the superconductivity transition critical temperature $(T_c)$ of a two dimensional electron gas (2DEG), where superconductivity is mediated by a Bose-Einstein condensate of exciton-polaritons. The critical temperature is found to increase with the boson density, but surprisingly it decreases with the 2DEG density increase. This makes doped semiconductor structures with shallow Fermi energies better adapted for observation of the exciton-induced superconductivity than metallic layers. For the realistic GaAs-based microcavit…
The Mott relation between the electrical and thermoelectric transport coefficients normally holds for phenomena involving scattering. However, the anomalous Hall effect (AHE) in ferromagnets may arise from intrinsic spin-orbit interaction. In this work, we have simultaneously measured AHE and the anomalous Nernst effect (ANE) in Ga1-xMnxAs ferromagnetic semiconductor films, and observed an exceptionally large ANE at zero magnetic field. We further show that AHE and ANE share a common origin and demonstrate the validity of the Mott relation for the anomalous transport phenomena.
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 …
The Mott transition from a dipolar excitonic liquid to an electron-hole plasma is demonstrated in a wide GaN/(Al,Ga)N quantum well at $T=7$K by means of spatially-resolved magneto-photoluminescence spectroscopy. Increasing optical excitation density we drive the system from the excitonic state, characterized by a diamagnetic behavior and thus a quadratic energy dependence on the magnetic field, to the unbound electron-hole state, characterized by a linear shift of the emission energy with the magnetic field. The complexity of the system requires to take into account both the density-dependence…
Exciton-polaritons are quasiparticles consisting of a linear superposition of photonic and excitonic states, offering potential for nonlinear optical devices. The excitonic component of the polariton provides a finite Coulomb scattering cross section, such that the different types of exciton found in organic materials (Frenkel) and inorganic materials (Wannier-Mott) produce polaritons with different interparticle interaction strength. A hybrid polariton state with distinct excitons provides a potential technological route towards in-situ control of nonlinear behaviour. Here we demonstrate a de…
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, …
Exciton Mott transition in Si is investigated by using terahertz time-domain spectroscopy. The excitonic correlation as manifested by the 1s-2p resonance is observed above the Mott density. The scattering rate of charge carriers is prominently enhanced at the proximity of Mott density, which is attributed to the non-vanishing exciton correlation in the metallic electron-hole plasma. Concomitantly, the signature of plasmon-exciton coupling is observed in the loss function spectra.
Excitonic effects play a particularly important role in the optoelectronic behavior of two-dimensional semiconductors. To facilitate the interpretation of experimental photoabsorption and photoluminescence spectra we provide (i) statistically exact diffusion quantum Monte Carlo binding-energy data for a Mott-Wannier model of (donor/acceptor-bound) excitons, trions, and biexcitons in two-dimensional semiconductors in which charges interact via the Keldysh potential, (ii) contact pair-distribution functions to allow a perturbative description of contact interactions between charge carriers, and …
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…
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…
We describe exciton-polariton modes formed by the interaction between excitons in a 2D layer of a transition metal dichalcogenide embedded in a cylindrical microcavity and the microcavity photons. For this, an expression for the excitonic susceptibility of a semiconductor disk placed in the symmetry plane perpendicular to the axis of the microcavity is derived. Semiclassical theory provides dispersion relations for the polariton modes, while the quantum-mechanical treatment of a simplified model yields the Hopfield coefficients, measuring the degree of exciton-photon mixing in the coupled mode…
The optical absorption of a single spherical semiconductor quantum dot in an electrical field is studied taking into account the nonlocal coupling between the field of the light and the polarizability of the semiconductor. These nonlocal effects lead to a small size anf field dependent shift and broadening of the excitonic resonance which may be of interest in future high precision experiments.
We report on a theoretical study of the fine structure of excited excitonic levels in semiconductor quantum disks. A particular attention is paid to the effect of electron-hole long-range exchange interaction. We demonstrate that, even in the axisymmetric quantum disks, the exciton P-shell is split into three sublevels. The analytical results are obtained in the limiting cases of strong and weak confinement. A possibility of exciton spin relaxation due to the resonant LO-phonon-assisted coupling between the P and S shells is discussed.
