Biexciton Binding Energy Research Articles

Electrically driven uniaxial stress device for tuning in situ semiconductor quantum dot symmetry and exciton emission in cryostat

Uniaxial stress is a powerful tool for tuning exciton emitting wavelength, polarization, fine-structure splitting (FSS), and the symmetry of quantum dots (QDs). Here, we present a technique for applying uniaxial stress, which enables us in situ to tune exciton optical properties at low temperature down to 15 K with high tuning precision. The design and operation of the device are described in detail. This technique provides a simple and convenient approach to tune QD structural symmetry, exciton energy and biexciton binding energy. It can be utilized for generating entangled and indistinguishable photons. Moreover, this device can be employed for tuning optical properties of thin film materials at low temperature.

From strong to weak temperature dependence of the two-photon entanglement resulting from the biexciton cascade inside a cavity

We investigate the degree of entanglement quantified by the concurrence of photon pairs that are simultaneously emitted in the biexciton-exciton cascade from a quantum dot in a cavity. Four dot-cavity configurations are compared that differ with respect to the detuning between the cavity modes and the quantum dot transitions, corresponding to different relative weights of direct two-photon and sequential single-photon processes. The dependence of the entanglement on the exciton fine-structure splitting $\delta$ is found to be significantly different for each of the four configurations. For a finite splitting and low temperatures, the highest entanglement is found when the cavity modes are in resonance with the two-photon transition between the biexciton and the ground state and, in addition, the biexciton has a finite binding energy of a few meV. However, this widely used configuration is rather strongly affected by phonons such that other dot-cavity configurations, that are commonly regarded as less suited for obtaining high degrees of entanglement, become more favorable already at temperatures on the order of 10 K and above. If the cavity modes are kept in resonance with one of the exciton-to-ground-state transitions and the biexciton binding energy is finite, the entanglement drastically drops for positive $\delta$ with rising temperatures when $T$ is below $\simeq$ 4 K, but is virtually independent of the temperature for higher $T$.

Nonlinear optical dynamics of a 2D semiconductor quantum dot super-crystal: Emerging multistability, self-oscillations and chaos

We conduct a theoretical study of the nonlinear optical dynamics of a 2D super-crystal comprising regularly spaced identical semiconductor quantum dots (SQDs), subjected to a resonant continuous wave excitation. A single SQD is considered as three-level ladder-like systems involving the ground, one-exciton and bi-exction states. We show that the super - crystal reveals a rich nonlinear dynamics, exhibiting multistability, self-oscillations and chaos. The behaviour is driven by the retarded SQD-SQD interactions and bi-exciton binding energy.

Binding energies of excitonic complexes in type-II quantum rings from diffusion quantum Monte Carlo calculations

Excitonic complexes in type-II quantum-ring heterostructures may be considered as artificial atoms due to the confinement of only one charge-carrier type in an artificial nucleus. Binding energies of excitons, trions, and biexcitons in these nanostructures are then effectively ionization energies of these artificial atoms. The binding energies reported here are calculated within the effective-mass approximation using the diffusion quantum Monte Carlo method and realistic geometries for gallium antimonide rings in gallium arsenide. The electrons form a halo outside the ring, with very little charge density inside the central cavity of the ring. The de-excitonization and binding energies of the complexes are relatively independent of the precise shape of the ring.

Trions and biexcitons in ZnO/ZnMgO, CdSe/ZnS and CdSe/CdS core/shell nanowires

A study of the trion and biexciton in a nanowire (NW) in the framework of the effective-mass model is presented. We consider the formation of trions and biexcitons under the action of both the lateral confinement and the localization potential. The analytical expressions for the binding energy and eigenfunctions of the trion and biexciton are obtained and expressed by means of matrix elements of the effective one-dimensional cusp-type Coulomb potentials whose parameters are determined self-consistently by employing eigenfunctions of the confined electron and hole states. Our calculations for the ZnO/ZnMgO, CdSe/ZnS and CdSe/CdS core/shell cylindrical shaped NWs show that the trion and biexciton binding energy in NWs are size-dependent and for the same input parameters the biexciton binding energy in NWs is always larger than the binding energy of the trion. The trion and biexciton remain stable in CdSe/ZnS NW with the increase of the dielectric shell, while in ZnO/ZnMgO NW they become unstable when the surrounding dielectric shell exceeds 2.5 nm and 2 nm for each, respectively. The associative ionization of biexciton antibonding states into trion bonding states that leads to the formation of trions is studied. Based on the results for size dependence of biexciton binding energy and probability associative ionization an optimal radius for optoelectronic application NW is suggested.

Excitonic complexes in anisotropic atomically thin two-dimensional materials: Black phosphorus and TiS3

The effect of anisotropy in the energy spectrum on the binding energy and structural properties of excitons, trions, and biexcitons is investigated. To this end we employ the stochastic variational method with a correlated Gaussian basis. We present results for the binding energy of different excitonic complexes in black phosphorus (bP) and TiS$_3$ and compare them with recent results in the literature when available, for which we find good agreement. The binding energies of excitonic complexes in bP are larger than those in TiS$_3$. We calculate the different average interparticle distances in bP and TiS$_3$ and show that excitonic complexes in bP are strongly anisotropic whereas in TiS$_3$ they are almost isotropic, even though the constituent particles have an anisotropic energy spectrum. This is also confirmed by the correlation functions.

Ultrafast time-resolved investigations of excitons and biexcitons at room temperature in layered WS2

Strong light-matter interactions in layered transition metal dichalcogenides (TMDs) open up vivid possibilities for novel excitonic quasiparticle-based devices. The optical properties of TMDs are dominated mostly by the tightly bound excitons and more complex quasiparticles, the biexcitons. Instead of physically exfoliated monolayers, the solvent-mediated chemical exfoliation of these 2D crystals is a cost-effective, large-scale production method suitable for substantial practical implications. Here, we explore the ultrafast excitonic phenomena in layered WS2 (mono-to-quad) dispersion using broadband (350–750 nm) femtosecond pump-probe spectroscopy at room temperature (300 K) which are inaccessible to the steady-state absorption or emission spectroscopy. The transient absorption spectra (TAS) suggest that the mono-to-quad layered dispersion of WS2 has similar spectral features as monolayer WS2 in terms of saturation absorptions (SA) and excited state absorptions (ESA). Similar to monolayer TMDs, we are able to identify excitons and biexcitons in multi-layered 2D stratum of WS2 as well as calculate the biexciton binding energies ( 69 meV and 66 meV), which are in excellent agreement with earlier theoretical predictions. Furthermore, using many-body physics, we demonstrate that the excitons in layered WS2 behave like Wannier–Mott excitons and explain their origins via first-principles calculations. Our detailed time-resolved investigation provides ultrafast radiative and non-radiative lifetimes of the excitons and biexcitons in layered WS2. Indeed, our results unravel the complex optical response of layered TMDs, which should lead to numerous technological applications for developing excitonic quasiparticle-based valleytronic devices and ultrafast biexciton lasers at room temperature.

Vanishing biexciton binding energy from stacked, MOVPE grown, site-controlled pyramidal quantum dots for twin photon generation

We characterized stacked double-pyramidal quantum dots which showed biexciton binding energies close to zero by means of photoluminescence and cross-correlation measurements. It was possible to obtain a sequence of two photons with (nearly) the same energy from the biexciton-exciton-ground state cascade, as corroborated by a basic rate-equation model. This type of two-photon emission is both of relevance for fundamental quantum information theory studies as well as for more exotic applicative fields such as quantum biology.

Vertical Cavity Biexciton Lasing in 2D Dodecylammonium Lead Iodide Perovskites

AbstractLayered Ruddlesden‐Popper‐type (2D) metal‐halide perovskites exhibit markedly increased exciton binding energies, exceeding 150 meV, compared to their 3D counterparts. Many‐body physics, enabled by Coulomb interactions, plays a strong role and raises the biexciton binding energy to 50 meV. Here, photoluminescence at a range of temperatures and carrier concentrations in thin films of the layered perovskite material (C12H25NH3)2PbI4 is reported. Biexcitons are directly observed up to a sample temperature of 225 K. An optical microcavity (comprising a distributed Bragg reflector and a metal mirror), with photonic resonances tuned near to the biexciton energy, is constructed. Optically‐pumped biexciton lasing up to 125 K, with a threshold peak excitation density of 5.6 × 1018 cm−3, is observed. The demonstration of biexciton lasing above liquid nitrogen temperatures is a crucial step for the application of layered perovskites in photonic applications.

Comparison of different concurrences characterizing photon pairs generated in the biexciton cascade in quantum dots coupled to microcavities

We compare three different notions of concurrence to measure the polarization entanglement of two-photon states generated by the biexciton cascade in a quantum dot embedded in a microcavity. We focus on the often-discussed situation of a dot with finite biexciton binding energy in a cavity tuned to the two-photon resonance. Apart from the time-dependent concurrence, which can be assigned to the two-photon density matrix at any point in time, we study single- and double-time integrated concurrences commonly used in the literature that are based on different quantum state reconstruction schemes. We argue that the single-time integrated concurrence can be thought of as the concurrence of photons simultaneously emitted from the cavity without resolving the common emission time, while the more widely studied double-time integrated concurrence refers to photons that are neither filtered with respect to the emission time of the first photon nor with respect to the delay time between the two emitted photons. Analytic and numerical calculations reveal that the single-time integrated concurrence indeed agrees well with the typical value of the time-dependent concurrence at long times, even in the presence of phonons. Thus, the more easily measurable single-time integrated concurrence gives access to the physical information represented by the time-dependent concurrence. However, the double-time integrated concurrence shows a different behavior with respect to changes in the exciton fine structure splitting and even displays a completely different trend when the ratio between the cavity loss rate and the fine structure splitting is varied while keeping their product constant. This implies the non-equivalence of the physical information contained in the time-dependent and single-time integrated concurrence on the one hand and the double-time integrated concurrence on the other hand.

Two-Photon Absorption and Two-Photon-Induced Gain in Perovskite Quantum Dots.

Perovskite quantum dots (PQDs) emerged as a promising class of material for applications in lighting devices, including light emitting diodes and lasers. In this work, we explore nonlinear absorption properties of PQDs showing the spectral signatures and the size dependence of their two-photon absorption (2PA) cross-section, which can reach values higher than 106 GM. The large 2PA cross section allows for low threshold two-photon induced amplified spontaneous emission (ASE), which can be as low as 1.6 mJ/cm2. We also show that the ASE properties are strongly dependent on the nanomaterial size, and that the ASE threshold, in terms of the average number of excitons, decreases for smaller PQDs. Investigating the PQDs biexciton binding energy, we observe strong correlation between the increasing on the biexciton binding energy and the decreasing on the ASE threshold, suggesting that ASE in PQDs is a biexciton-assisted process.

Evidence of exciton complexes in non polar ZnO/(Zn,Mg)O A-plane quantum well

Excitons complexes in ZnO/(Zn, Mg)O non-polar quantum well have been studied by using continuous-wave photoluminescence according to temperature and to the density of excitation. The spectrum of photoluminescence of the quantum well consists of three different lines. The ratio between the intensities of these lines depends of the temperature but also of the density of excitation. The lines are attributed to the free exciton, the negatively charged trion and the biexciton. The binding energy of trion and biexciton are found to be respectively 19.5 ± 2 meV and 45 ± 5 meV.

Two-Photon Rabi Splitting in a Coupled System of a Nanocavity and Exciton Complexes.

Two-photon Rabi splitting in a cavity-dot system provides a basis for multiqubit coherent control in a quantum photonic network. Here we report on two-photon Rabi splitting in a strongly coupled cavity-dot system. The quantum dot was grown intentionally large in size for a large oscillation strength and small biexciton binding energy. Both exciton and biexciton transitions couple to a high-quality-factor photonic crystal cavity with large coupling strengths over 130 μeV. Furthermore, the small binding energy enables the cavity to simultaneously couple with two exciton states. Thereby, two-photon Rabi splitting between the biexciton and cavity is achieved, which can be well reproduced by theoretical calculations with quantum master equations.

Excitons, trions, and biexcitons in transition-metal dichalcogenides: Magnetic-field dependence

The influence of a perpendicular magnetic field on the binding energy and structural properties of excitons, trions, and biexcitons in monolayers of semiconducting transition metal dichalcogenides (TMDs) is investigated. The stochastic variational method (SVM) with a correlated Gaussian basis is used to calculate the different properties of these few-particle systems. In addition, we present a simplified variational approach which supports the SVM results for excitons as a function of magnetic field. The exciton diamagnetic shift is compared with recent experimental results and we extend this concept to trions and biexcitons. The effect of a local potential fluctuation, which we model by a circular potential well, on the binding energy of trions and biexcitons is investigated and found to significantly increase the binding of those excitonic complexes.

Telecom wavelength single quantum dots with very small excitonic fine-structure splitting

We report on molecular beam epitaxy growth of symmetric InAs/InP quantum dots (QDs) emitting at a telecom C-band (1.55 μm) with an ultra-small excitonic fine-structure splitting of ∼2 μeV. The QDs are grown on a distributed Bragg reflector (DBR) and systematically characterized by micro-photoluminescence (μ-PL) measurements. One order of magnitude of QD PL intensity enhancement is observed in comparison to the samples without DBR. A combination of power-dependent and polarization-resolved measurements reveals background-free exciton, biexciton, and dark exciton emission with a resolution-limited linewidth below 35 μeV and a biexciton binding energy of ∼1 meV. The results are confirmed by statistical measurements of about 20 QDs.

Biexciton Binding Energy in Spherical Quantum Dots with Γ8 Valence Band

The biexciton binding energy in spherical CdSe/ZnSe quantum dots is calculated variationally in the framework of kp-perturbation theory. Smooth and abrupt confining potentials with the same localization area of carriers are compared for two limiting cases of light hole to heavy hole mass ratio β = m lh /m hh : β = 1 and β = 0. Accounting for correlations between carriers results in their polarized configuration and significantly increases the biexciton binding energy in comparison with the first order perturbation theory. For β = 0 in smooth confining potentials there are three nearby biexciton states separated by small energy gap between 1S3/2 and 1P3/2 hole states.

Complexes of dipolar excitons in layered quasi-two-dimensional nanostructures

We discuss neutral and charged complexes (biexciton and trion) formed by indirect excitons in layered quasi-two-dimensional semiconductor heterostructures. Indirect excitons -- long-lived neutral Coulomb-bound pairs of electrons and holes of different layers -- have been known for semiconductor coupled quantum wells and are recently reported for van der Waals heterostructures such as bilayer graphene and transition metal dichalcogenides. Using the configuration space approach, we derive the analytical expressions for the trion and biexciton binding energies as functions of the interlayer distance. The method captures essential kinematics of complex formation to reveal significant binding energies, up to a few tens of meV for typical interlayer distances ~3-5 A, with the trion binding energy always being greater than that of the biexciton. Our results can contribute to the understanding of more complex many-body phenomena such as exciton Bose-Einstein condensation and Wigner-like electron-hole crystallization in layered semiconductor heterostructures.

Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder

With strongly bound and stable excitons at room temperature, single-layer, two-dimensional organic-inorganic hybrid perovskites are viable semiconductors for light-emitting quantum optoelectronics applications. In such a technological context, it is imperative to comprehensively explore all the factors --- chemical, electronic and structural --- that govern strong multi-exciton correlations. Here, by means of two-dimensional coherent spectroscopy, we examine excitonic many-body effects in pure, single-layer (PEA)$_2$PbI$_4$ (PEA = phenylethylammonium). We determine the binding energy of biexcitons --- correlated two-electron, two-hole quasiparticles --- to be $44 \pm 5$\,meV at room temperature. The extraordinarily high values are similar to those reported in other strongly excitonic two-dimensional materials such as transition-metal dichalchogenides. Importantly, we show that this binding energy increases by $\sim25$\% upon cooling to 5\,K. Our work highlights the importance of multi-exciton correlations in this class of technologically promising, solution-processable materials, in spite of the strong effects of lattice fluctuations and dynamic disorder.

Stability of trions in coupled quantum wells modeled by two-dimensional bilayers

We report variational and diffusion quantum Monte Carlo calculations of the binding energies of indirect trions and biexcitons in ideal two-dimensional bilayer systems within the effective-mass approximation, and with a Coulomb $1/r$ interaction between charge carriers. The critical layer separation at which trions become unbound has been studied for various electron-hole mass ratios, and found to be over an order of magnitude larger than the critical layer separation for biexcitons.

Biexciton binding energy in spherical quantum dots with Gamma-=SUB=-8-=/SUB=- valence band

AbstractThe biexciton binding energy in spherical CdSe/ZnSe quantum dots is calculated variationally in the framework of kp-perturbation theory. Smooth and abrupt confining potentials with the same localization area of carriers are compared for two limiting cases of light hole to heavy hole mass ratio β = m_ lh /m_ hh : β = 1 and β = 0. Accounting for correlations between carriers results in their polarized configuration and significantly increases the biexciton binding energy in comparison with the first order perturbation theory. For β = 0 in smooth confining potentials there are three nearby biexciton states separated by small energy gap between 1 S _3/2 and 1 P _3/2 hole states.