This theoretical paper offers an explicit expression for the binding energy of excitons in a two-dimensional semiconductor with a flat valence band. The formula has been derived quasiclassically assuming that the exciton is tightly bound; i.e., its ground-state radius is determined by the intrinsic polarizability of the semiconductor rather than by the dielectric properties of the environment. The model is relevant to a few two-dimensional semiconductors discovered recently, including distorted 1T-TiSe$_2$, with a supposedly unstable electronic ground state. The valence band flatness reduces the exciton binding energy, which also may have an effect on the phase transition to an excitonic insulator.
The localization length of a low energy tightly bound electron-hole pair (excitons) is calculated by exact diagonalization for small interacting disordered systems. The exciton localization length (which corresponds to the thermal electronic conductance) is strongly enhanced by electron-electron interactions, while the localization length (pertaining to the charge conductance) is only slightly enhanced. This shows that the two particle delocalization mechanism widely discussed for the electron pair case is more efficient close to the Fermi energy for an electron-hole pair. The relevance to exp…
Exciton binding energy and excited states in monolayers of tungsten diselenide (WSe2) are investigated using the combined linear absorption and two-photon photoluminescence excitation spectroscopy. The exciton binding energy is determined to be 0.37eV, which is about an order of magnitude larger than that in III-V semiconductor quantum wells and renders the exciton excited states observable even at room temperature. The exciton excitation spectrum with both experimentally determined one- and two-photon active states is distinct from the simple two-dimensional (2D) hydrogenic model. This result…
The circularly-polarized and angular-resolved magneto-photoluminescence spectroscopy was carried out to study the free A exciton 1S state in wurtzite ZnO at 5 K.
If the Zeeman energy is small, the lowest energy excitations of a two dimensional electron gas at filling factor nu=1 are spin waves (spin flip excitations). At nu slightly larger (smaller) than unity, reversed spin electrons (spin holes) can form bound states with K spin waves that are known as skyrmions, S_K^- (antiskyrmions, S_K^+). It is suggested in this work that a valence hole can also bind K spin waves to form an excitonic complex X_K^+, analogous to the S_K^+. One spin hole of the S_K^+ is simply replaced by the valence hole. At nu<=1, a small number of S_K^+'s are present before intr…
Nesting in a semimetal can lead to an excitonic insulator state with spontaneous coherence between conduction and valence bands and a gap for charged excitations. In this paper we present a theory of the ferromagnetic state that occurs when the density of electrons in the conduction band and holes in the valence band differ. We find an unexpectedly rich doping-field phase diagram and an unusual collective excitation spectrum that includes two gapless collective modes. We predict regions of doping and external field in which phase-separated condensates of electrons and holes with parallel spins…
Electric-field-driven magnetic switching and tightly bound interlayer excitons in bilayer CrSBr
Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology（华中科技大学物理学院）；School of Physics and Technology, Wuhan University（武汉大学物理科学与技术学院）；National Institute for Material Science（日本国立材料研究所）
We present a method to calculate the exciton spectra of all direct semiconductors with a complex valence band structure. The Schrödinger equation is solved using a complete basis set with Coulomb Sturmian functions. This method also allows for the computation of oscillator strengths. Here we apply this method to investigate the impact of the valence band structure of cuprous oxide $\left(\mathrm{Cu_{2}O}\right)$ on the yellow exciton spectrum. Results differ from those in [Phys. Rev. Lett. 115, 027402 (2015)]; the differences are discussed and explained. The difference between the second and t…
We study dipole interseries transitions between the yellow and green exciton series in cuprous oxide including the complex valence band structure. To this end, we extend previous studies of the spectrum of complex green exciton resonances [Phys. Rev. B 101, 075208 (2020)] to optical transitions between different exciton states in addition to transitions from the crystal ground state. This allows us to augment the calculations on interseries transitions using a hydrogen-like model [Phys. Rev. B 100, 085201 (2019)] by a more comprehensive treatment of the valence band structure.
The photoluminescence (PL) of a two-dimensional electron gas (2DEG) in a high magnetic field is studied as a function of the filling factor and the separation d between the electron layer and the valence hole. Depending on the magnitude of d relative to the magnetic length lambda, two distinct regimes in the response of the 2DEG to the valence hole occur, with different elementary emission processes contributing to the PL spectrum. At d<lambda ("strong coupling" regime), the hole binds one or two electrons to form an exciton (X) or one of three possible charged exciton (X-) states, a spin-sing…
The energy spectrum of a two-dimensional electron gas (2DEG) in the fractional quantum Hall regime interacting with an optically injected valence band hole is studied as a function of the filling factor $ν$ and the separation $d$ between the electron and hole layers. The response of the 2DEG to the hole changes abruptly at $d$ of the order of the magnetic length $λ$. At $d<λ$, the hole binds electrons to form neutral ($X$) or charged ($X^-$) excitons, and the photoluminescence (PL) spectrum probes the lifetimes and binding energies of these states rather than the original correlations of the 2…
The energy spectrum of a two-dimensional electron gas (2DEG) interacting with a valence-band hole is studied in the high magnetic field limit as a function of the filling factor nu and the separation d between the electron and hole layers. For d smaller than the magnetic length lambda, the hole binds one or more electrons to form neutral (X) or charged (X-) excitons. The low-lying states can be understood in terms of Laughlin-like correlations among the constituent charged fermions (electrons and X-). For d comparable to lambda, the electron-hole interaction is not strong enough to bind a full…
In order to discuss the exciton fine-structure of transition-metal dichalcogenides mono-layers, excitons are first defined in the subspace of electron- and hole states, including the lowest conduction band (LCB) and the uppermost valence band (UVB). Both bands are spin degenerate at the Gamma-point. All other states are neglected. The resulting exciton states are analyzed in the framework of an invariant expansion of a model Hamiltonian: The spin-orbit coupling in the conduction- and valence band is simulated by introducing a fictive magnetic field, giving rise to a splitting of the electron- …
We reconsider a key point in semiconductor physics, the splitting of the valence band states induced by the spin-orbit interaction, through a novel approach which uses neither the group theory formalism, nor the usual $\textbf{L}\cdot\textbf{S}$ formulation valid for atoms but conceptually incorrect for periodic lattices, the angular momenta $\textbf{L}$ and $\textbf{J}$ having no meaning due to the absence of spherical symmetry. We show that for zinc-blende structures, the valence band eigenstates resulting from spin-orbit coupling are uniquely determined by: (i) the equivalence of the ($x,y,…
Excitonic quasi-particles, excitons/trions/bi-excitons, and their coupling with phonons and charge carriers play a crucial role in controlling the optical properties of atomically thin semiconducting 2D materials. In this work, we unravelled the dynamics of excitons/trions and their coupling with phonons and charge carriers in a few layers vertically and horizontally aligned MoS2. We observed trion signature up to the highest recorded temperature (330 K) in both systems and have shown that the dynamics of excitons/trions and their coupling with phonons and electrons are more affected in vertic…
We point out at the possible relationship between the two many-body phenomena: Friedel oscillations and Mahan exciton/Fermi edge singularity in a recombination process of a localized valence band hole with a degenerate electron system. It is qualitatively described that the oscillating electron density around the screened potential of a neutral acceptor can modify the wavefunction of the valence band hole and thus promote its recombination with electrons near Fermi-surface. The role of a finite hole mass for the net balance of the two hole energies: the kinetic energy and Coulomb attraction to…
Electron, hole, and exciton states of multishell CdS/HgS/CdS quantum-dot quantum well nanocrystals are determined by use of a multiband theory that includes valence-band mixing, modeled with a 6-band Luttinger-Kohn Hamiltonian, and nonparabolicity of the conduction band. The multiband theory correctly describes the recently observed dark-exciton ground state and the lowest, optically active, bright-exciton states. Charge separation in pair states is identified. Previous single-band theories could not describe these states or account for charge separation.
We uncover topological features of neutral particle-hole pair excitations of correlated quantum anomalous Hall (QAH) insulators whose approximately flat conduction and valence bands have equal and opposite non-zero Chern number. Using an exactly solvable model we show that the underlying band topology affects both the center-of-mass and relative motion of particle-hole bound states. This leads to the formation of topological exciton bands whose features are robust to nonuniformity of both the dispersion and the Berry curvature. We apply these ideas to recently-reported broken-symmetry spontane…
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…
Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe$_2$/WSe$_2$ heterostructures, strong hybridization occurs between the holes in the spin-split valence band of WSe$_2$ and in the top valence band of MoSe$_2$, especi…
I present a systematic study of self-assembled InAs/InP and InAs/GaAs quantum dots single particle and many body properties as a function of quantum dot-surrounding matrix valence band offset. I use an atomistic, empirical tight-binding approach and perform numerically demanding calculations for half-million atom nanosystems. I demonstrate that the overall confinement in quantum dots is a nontrivial interplay of two key factors: strain effects and the valence band offset. I show that strain effects determine both the peculiar structure of confined hole states of lens type InAs/GaAs quantum dot…
Time- and angle-resolved photoemission spectroscopy (trARPES) is a powerful spectroscopic method to measure the ultrafast electron dynamics directly in momentum-space. However, band gap materials with exceptional strong Coulomb interaction such as monolayer transition metal dichlacogenides (TMDC) exhibit tightly bound excitons, which dominate their optical properties. This rises the question whether excitons, in particular their formation and relaxation dynamics, can be detected in photoemission. Here, we develope a fully microscopic theory of the temporal dynamics of excitonic time- and angle…
Enhanced Coulomb interactions in monolayer transition metal dichalcogenides cause tightly bound electron-hole pairs (excitons) which dominate their linear and nonlinear optical response. The latter includes bleaching, energy renormalizations, and higher-order Coulomb correlation effects like biexcitons and excitation-induced dephasing (EID). While the first three are extensively studied, no theoretical footing for EID in exciton dominated semiconductors is available so far. In this study, we present microscopic calculations based on excitonic Heisenberg equations of motion and identify the cou…
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…
Purely electronic model for exciton-polaron formation in moiré heterostructures
Technical University of Munich（慕尼黑工业大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Joint Quantum Institute, University of Maryland（马里兰大学联合量子研究所）
Semiconducting transition metal dichalcogenides (STMDC) are two-dimensional (2D) crystals characterized by electron volt size band gaps, spin-orbit coupling (SOC), and d-orbital character of its valence and conduction bands. We show that these materials carry unique exciton quasiparticles (electron-hole bound states) with energy within the gap but which can ``collapse'' in the strong coupling regime by merging into the band structure continuum. The exciton collapse seems to be a generic effect in these 2D crystals.
We present a theoretical description of excitons and positively and negatively charged trions in "giant" CdSe/CdS core-shell nanocrystals (NCs). The developed theory provides the parameters describing the fine structure of excitons in CdSe/CdS core/thick shell NCs as a function of the CdSe/CdS conduction band offset and the CdSe core radius. We have also developed a general theory describing the fine structure of positively charged trions created in semiconductor NCs with a degenerate valence band. The calculations take into account the complex structure of the CdSe valence band and inter-part…
The excitonic spectra of single layer GeS and GeSe are predicted by ab initio GW-Bethe Salpeter equation calculations. G 0 W 0 calculations for the band structures find a fundamental band gap of 2.85 eV for GeS and 1.70 eV for GeSe monolayer. However, excitons are tightly bound, specially in GeS at the Γ point, where the quasi-particle interactions are so strong that they shift the Γ exciton peak energy into the visible range and below the off-Γ exciton peak. The lowest energy excitons in both materials are excited by light along the zigzag direction and have exciton binding energies of 1.05 e…
Transition metal dichalcogenides (TMDs) are layered materials that have a semiconducting phase with many advantageous optoelectronic properties, including tightly bound excitons and spin-valley locking. In Tungsten-based TMDs, spin and momentum forbidden transitions give rise to dark excitons that typically are optically inaccessible but represent the lowest excitonic states of the system. Dark excitons can deeply affect transport, dynamics and coherence of bright excitons, hampering device performance. Therefore, it is crucial to create conditions in which these excitonic states can be visual…
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…
We derive analytically the change of exciton fine structure splitting (FSS) under the external stresses in the self-assembled InAs/GaAs quantum dots using the Bir-Pikus model. We find that the FSS change is mainly due to the strain induced valence bands mixing and valence-conduction band coupling. The exciton polarization angle under strain are determined by the argument of the electron-hole off-diagonal exchange integrals. The theory agrees well with the empirical pseudopotential calculations.
Semiconductor microresonators embedding quantum wells can host tightly confined and mutually interacting excitonic, optical and mechanical modes at once. We theoretically investigate the case where the system operates in the strong exciton-photon coupling regime, while the optical and excitonic resonances are parametrically modulated by the interaction with a mechanical mode. Owing to the large exciton-phonon coupling at play in semiconductors, we predict an enhancement of polariton-phonon interactions by two orders of magnitude with respect to mere optomechanical coupling: a near-unity single…
The electronic and structural properties of excitons and trions in monolayer transition metal dichalcogenides are investigated using both a multiband and a single-band model. In the multiband model we construct the excitonic Hamiltonian in the product base of the single-particle states at the conduction and valence band edges. We decouple the corresponding energy eigenvalue equation and solve the resulting differential equation self-consistently, using the finite element method (FEM), to determine the energy eigenvalues and the wave functions. As a comparison, we also consider the simple singl…
We present numerical investigations based on the Luttinger-Kohn four-band $k \cdot p$ theory and, accordingly, establish a quantitatively valid model of the excitonic fine structures of droplet epitaxial GaAs/AlGaAs quantum dots under uni-axial stress control. In the formalisms, stressing a photo-excited quantum dot is equivalent creating a pseudo-magnetic field that is directly coupled to the pseudo-spin of the exciton doublet and tunable to tailor the polarized fine structure of exciton. The latter feature is associated with the valence-band-mixing of exciton that is especially sensitive to …
We predict a phase transition in freestanding monolayer Xenes from the semiconducting phase to the excitonic insulating (EI) phase can be induced by reducing an external electric field below some critical value which is unique to each material. The splitting of the conduction and valence bands due to spin-orbit coupling at non-zero electric fields leads to the formation of $A$ and $B$ excitons in the larger or smaller band gap, with correspondingly larger or smaller binding energies. Our calculations show the coexistence of the semiconducting phase of $A$ excitons with the EI phase of $B$ exci…
Two-dimensional group-VI transition metal dichalcogenide semiconductors, such as MoS2, WSe2 and others, exhibit strong light-matter coupling and possess direct band gaps in the infrared and visible spectral regimes, making them potentially interesting candidates for various applications in optics and optoelectronics. Here, we review their optical and optoelectronic properties with emphasis on exciton physics and devices. As excitons are tightly bound in these materials and dominate the optical response even at room-temperature, their properties are examined in depth in the first part of this a…
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…
We investigate excitons in stacked transition metal dichalcogenide (TMDC) layers under perpendicularly applied electric field, herein MoSe$_2$/WSe$_2$ van der Waals heterostructures. Band structures are obtained with density functional theory calculations, along with the electron and hole wave functions in conduction and valence bands, respectively. Although the type-II nature of the heterostructure leads to fully charge separated inter-layer excitons, charge carriers distribution among the layers is shown to be easily tunable by external field. Our results show that moderate values of electri…
For composite complexes -- quasi-two-dimensional (2D) charged magneto-excitons X- -- we propose a new exact classification of states, which is based on magnetic translations. We consider implications of this symmetry for magneto-optical transitions. It is shown, in particular, that in a translationally-invariant system with a simple valence band, the ground triplet X- state is dark in interband transitions at finite magnetic fields B. This exact result calls for the re-interpretation of several previous theoretical studies. We consider the symmetry-breaking effects of spatial lateral confineme…
Two-dimensional (2D) magnetic semiconductors feature both tightly-bound excitons with large oscillator strength and potentially long-lived coherent magnons due to the presence of bandgap and spatial confinement. While magnons and excitons are energetically mismatched by orders of magnitude, their coupling can lead to efficient optical access to spin information. Here we report strong magnon-exciton coupling in the 2D van der Waals (vdW) antiferromagnetic (AFM) semiconductor CrSBr. Coherent magnons launched by above-gap excitation modulate the interlayer hybridization, which leads to dynamic mo…
Atomically thin semiconductors provide an excellent platform to study intriguing many-particle physics of tightly-bound excitons. In particular, the properties of tungsten-based transition metal dichalcogenides are determined by a complex manifold of bright and dark exciton states. While dark excitons are known to dominate the relaxation dynamics and low-temperature photoluminescence, their impact on the spatial propagation of excitons has remained elusive. In our joint theory-experiment study, we address this intriguing regime of dark state transport by resolving the spatio-temporal exciton d…
Single and multi-band (Burt-Foreman) k.p Hamiltonians for GaAs crystal phase quantum dots are developed and used to assess ongoing experimental activity on the role of such factors as quantum confinement, spontaneous polarization, valence band mixing and exciton Coulomb interaction. Spontaneous polarization is found to be a dominating term. Together with the control of dot thickness [Vainorious Nano Lett. 15, 2652 (2015)] it enables wide exciton wavelength and lifetime tunability. Several new phenomena are predicted for small diameter dots [Loitsch et al. Adv. Mater. 27, 2195 (2015)], includin…
Excitons, composite electron-hole quasiparticles, are known to play an important role in optoelectronic phenomena in many semiconducting materials. Recent experiments and theory indicate that the band-gap optics of the newly discovered monolayer transition-metal dichalcogenides (TMDs) is dominated by tightly bound valley excitons. The strong interaction of excitons with long-range electromagnetic fields in these 2D systems can significantly affect their intrinsic properties. Here, we develop a semi-classical framework for intrinsic exciton-polaritons in monolayer TMDs that treats their dispers…
We perform a $\mathbf{k \cdot p}$ theory analysis of the spectra of the lowest energy and excited states of the excitons in few-layer atomically thin films of InSe taking into account in-plane electric polarizability of the film and the influence of the encapsulation environment. For the thinner films, the lowest-energy state of the exciton is weakly indirect in momentum space, with its dispersion showing minima at a layer-number-dependent wave number, due to an inverted edge of a relatively flat topmost valence band branch of the InSe film spectrum and we compute the activation energy from th…
The photoluminescence (PL) spectrum of a two-dimensional electron gas (2DEG) in the fractional quantum Hall regime is studied. The response of the 2DEG to an optically injected valence hole depends on the separation d between the electron and hole layers. At d smaller than the magnetic length lambda, the PL spectrum shows recombination of neutral (X) and charged (X-) excitons. At d>lambda, the hole binds one or two Laughlin quasielectrons (QE) of the 2DEG to form fractionally charged excitons (FCX), hQE or hQE2. Different FCX states have different optical properties, and their stability depend…
The properties of energy spectrum of excitons in monolayer transition metal dichalcogenides are investigated using a multiband model. In the multiband model we use the excitonic Hamiltonian in the product base of the Dirac single-particle states at the conduction and valence band edges. Following the separation of variables we decouple the corresponding energy eigenvalue system of the first order ODE radial equations rigorously and solve the resulting the second order ODE self-consistently, using the finite difference method, thus we determine the energy eigenvalues of the discrete excitonic s…
Excitons - the particle-hole bound states - composed of localized electron-hole states in semiconducting systems are crucial to explaining the optical spectrum. Spectroscopic measurements can contain signatures of these two particle bound states and can be particularly useful in determining the characteristics of these excitons. We formulate an expression for evaluating the angle-resolved photoemission spectrum arising from the ionization of excitons given their steady-state distribution in a semiconductor. We show that the spectrum contains information about the direct/indirect band gap natur…
Magnetic-field driven hybridization of heavy- and light-hole Rydberg excitons in GaAs quantum wells
Universidad Autónoma de Madrid（马德里自治大学）；Condensed Matter Physics Center (IFIMAC)（凝聚态物理中心（IFIMAC））；CNR Nanotec, Institute of Nanotechnology（意大利国家研究委员会纳米技术研究所）；School of Physics and Astronomy, Monash University（莫纳什大学物理与天文学院）
