Biexciton Emission Research Articles

Observation of biexciton emission from single semiconductor nanoplatelets

Quasi-two-dimensional semiconductor nanoplatelets (NPLs) are intriguing systems for studying the influence of Auger recombination processes on the multiexciton emission efficiencies in the weak in-plane confinement regime. We investigate CdSe/CdS core/shell NPLs using cryogenic temperature single particle spectroscopy and observe bright biexciton emission at high excitation powers. The average binding energy of the biexcitons is determined to be 16.5 meV. The observed switching between the biexciton and trion states indicates charging-decharging dynamics of the NPLs mediated by the Auger ionization process. These findings are highly relevant for harvesting efficient biexciton emission for energy, lighting, and quantum applications.

Enhancing Dielectric Screening for Auger Suppression in CdSe/CdS Quantum Dots by Epitaxial Growth of ZnS Shell.

Auger recombination is the main nonradiative process in multicarrier states of high-quality quantum dots (QDs). For the most-studied CdSe/CdS core/shell QDs, we effectively reduce the biexciton Auger rate by enhancing dielectric screening of band-edge carriers via epitaxial growth of additional ZnS shells. Super volume scaling of negative-trion Auger lifetime for CdSe/CdS core/shell QDs is achieved with the outermost ZnS shells. The volume of CdSe/CdS/ZnS QDs can be less than half that of CdSe/CdS QDs with the same negative-trion Auger lifetime. Auger suppression by the ZnS shells is more pronounced for QDs with wave functions of band-edge carriers spreading close to the inorganic-organic interface, such as CdSe/CdS QDs with small cores. A maximum drop of biexciton Auger rate of ∼50% and a maximum enhancement of biexciton emission quantum yield of 75% are achieved. Auger engineering by dielectric screening opens up new opportunities to improve the emission properties of multicarrier states in QDs.

Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides.

The capability of quantum dots to generate both single and multiexcitons can be harnessed for a wide variety of applications, including those that require high optical gain. Here, we use time-correlated photoluminescence (PL) spectroscopy to demonstrate that the isolation of single CdSeTe/ZnS core-shell, nanocrystal quantum dots (QDs) in Zero Mode Waveguides (ZMWs) leads to a significant modification in PL intensity, blinking dynamics, and biexciton behavior. QDs in aluminum ZMWs (AlZMWs) exhibited a 15-fold increase in biexciton emission, indicating a preferential enhancement of the biexciton radiative decay rate as compared to the single exciton rate. The increase in biexciton behavior was accompanied by a decrease in blinking events due to a shortening in the dark state residence time. These results indicate that plasmon mediated enhanced decay rates of QDs in AlZMWs lead to substantial changes in the photophysical properties of single quantum dots, including an increase in biexciton behavior.

Identification of Excitons and Biexcitons in Sb2Se3 under High Photoluminescence Excitation Density

AbstractThe near‐band‐edge emission of Sb2Se3 microcrystals is studied in detail under high photoluminescence excitation density using a pulsed UV laser (λ = 266 nm, pulse width 0.6 ns). Based on the peak energy positions and the excitation power density and temperature dependencies (T = 3–110 K) of the photoluminescence spectra, the emission is interpreted as a recombination of two pairs (A and B) of free excitons and biexcitons appearing because of valence band splitting. The magnitude of the valence band splitting due to the crystal field (Δcr = 20–22 meV) is estimated in the Brillouin zone center. At T = 3 K, the A and B biexciton emission at 1.302 and 1.322 eV, respectively, and the A and B free exciton emission at 1.311 and 1.333 eV, respectively, are observed. The binding energy of A and B biexcitons is 9 and 11 meV, respectively, and the binding energy of A free exciton is 6 meV. The activation energy of thermal quenching for all observed peaks is 20 meV.

Mechanistic understanding of entanglement and heralding in cascade emitters.

Semiconductor quantum light sources are favorable for a wide range of quantum photonic tasks, particularly quantum computing and quantum information processing. Here, we theoretically investigate the properties of quantum emitters as a source of entangled photons with practical quantum properties including heralding of on-demand single photons. Through the theoretical analysis, we characterize the properties of a cascade (biexciton) emitter, including (1) studies of single-photon purity, (2) investigating the first- and second-order correlation functions, and (3) determining the Schmidt number of the entangled photons. The analytical expression derived for the Schmidt number of the cascade emitters reveals a strong dependence on the ratio of decay rates of the first and second photons. Looking into the joint spectral density of the generated biphotons, we show how the purity and degree of entanglement are connected to the production of heralded single photons. Our model is further developed to include polarization effects, fine structure splitting, and the emission delay between the exciton and biexciton emission. The extended model offers more details about the underlying mechanism of entangled photon production, and it provides additional degrees of freedom for manipulating the system and characterizing purity of the output photon. The theoretical investigations and the analysis provide a cornerstone for the experimental design and engineering of on-demand single photons.

Magnetic and power tuning of spin-asymmetric multiple excitons in a GaAs quantum well

Abstract A comprehensive study of excitonic complexes in high-quality GaAs quantum wells has been performed. The polarization-resolved photoluminescence results show exciton, biexciton, and trion emissions tuned by temperature, excitation power, and by an external magnetic field. Excitons and biexcitons show important differences in their dependence on the external field. While the Zeeman splitting of biexcitons depends monotonically on the magnetic field, with a nearly constant g-factor, the behaviour of the exciton energy splitting is nonmonotonic and includes an inversion of sign as a function of the magnetic field. More importantly, we observe that a trion resonance emerges at a finite magnetic field, and only appears at low laser excitation power and for σ+ polarization emission. The non-trivial dependence of the energy levels on the external magnetic field, together with the polarization selective trion emission, leads to an intricate exciton and trion dynamics, which can be reproduced by a set of coupled rate equations. Based on this theoretical approach, we show that a fast spin-flip process can lead to the spin-asymmetric emission, which reveals a contrasting spin-dynamics of excitonic complexes ruled by their charge.

Directional Single‐Photon Emission from Deterministic Quantum Dot Waveguide Structures

Chiral light–matter interaction can lead to directional emission of two‐level quantum emitters in waveguides (WGs). This interesting physics effect has raised considerable attention in recent years especially in terms of on‐chip quantum systems. In this context, this work focuses on tailoring single semiconductor quantum dot–waveguide (QD–WG) systems to emit single photons with high directionality. Low‐temperature in situ electron‐beam lithography enabled by cathodoluminescence mapping is used to select suitable QDs and to integrate them deterministically into linear WG structures at specific chiral points determined by numerical calculations. Excitonic and biexcitonic emission is observed from the fabricated QD–WG structure in a confocal micro‐photoluminescence setup enabling the optical characterization in terms of directional emission of circularly polarized photons emitted by integrated QDs. The results show a high degree of anisotropy on the level of 54% for directional QD emission and antibunching in autocorrelation experiment confirming the fabricated QD–WG system, which is a prerequisite for using this effect in advanced applications in integrated quantum circuits.

Correlation between exciton polarized lifetime and fine structure splitting in InAs/GaAs quantum dots

Semiconductor self-assembled single quantum dots (QDs) provide a promising solid-state light source for single photons and entangled photons. The structural asymmetry in QDs results in fine structure splitting (FSS) of exciton and biexciton emission lines. Here, we propose a method to study QD symmetry by measuring the difference in two different polarized lifetimes of QD excitonic emission lines under applied stress. The method can be reasonably correlated with the direct FSS measurement. Actually, due to the limitation of the resolution of the spectrometer, the zero value of FSS is difficult to measure. Instead, the lifetime measurement is an effective method to judge the symmetry condition of single QDs.

Biexcitons in 2D (iso-BA)2PbI4 perovskite crystals

Abstract Two-dimensional (2D) organic-inorganic hybrid perovskites have attracted growing attention recently due to their naturally formed quantum-well structure, unique photoelectric properties and better environmental stability compared to three-dimensional perovskites. The reduced screening and enhanced Coulomb interaction in 2D perovskites result in the formation of excitonic complexes. While the properties of free excitons have been well investigated, studies on biexcitons remain elusive. Here, we report on the biexcitons in 2D (iso-BA)2PbI4 (BA=C4H9NH3) crystals. The biexciton emission can be observed under a very low excitation power density of 6.4 W/cm2 at 78 K. The biexciton exhibits a large biexciton binding energy of 46 meV due to the large exciton binding energy of (iso-BA)2PbI4. Furthermore, the biexcitons exhibit a favorable polarization orientation, resulting in different anisotropy between biexcitons and excitons. Our findings would motivate more studies on biexcitons in 2D perovskites and pave the way for exploiting the many-body physics for biexciton lasing and optical storage devices.

Band‐Edge Exciton Fine Structure and Exciton Recombination Dynamics in Single Crystals of Layered Hybrid Perovskites

Abstract2D perovskite materials have recently reattracted intense research interest for applications in photovoltaics and optoelectronics. As a consequence of the dielectric and quantum confinement effect, they show strongly bound and stable excitons at room temperature. Here, the band‐edge exciton fine structure and in particular its exciton and biexciton dynamics in high quality crystals of (PEA)2PbI4 are investigated. A comparison of bulk and surface exciton lifetimes yields a room temperature surface recombination velocity of 2 × 103 cm s−1 and an intrinsic lifetime of 185 ns. Biexciton emission is evidenced at room temperature, with a binding energy of ≈45 meV and a lifetime of 80 ps. At low temperature, exciton state splitting is observed, which is caused by the electron–hole exchange interaction. Transient photoluminescence resolves the low‐lying dark exciton state, with a bright/dark splitting energy estimated to be 10 meV. This work contributes to the understanding of the complex scenario of the elementary photoexcitations in 2D perovskites.

Superior properties in room-temperature colloidal-dot quantum emitters revealed by ultralow-dark-count detections of temporally-purified single photons

The realization of high-quality quantum emitters that can operate at room temperature is important for accelerating the application of quantum technologies, such as quantum communication, quantum information processing, and quantum metrology. In this work, we study the photon-antibunching properties on room-temperature emission from individual colloidal quantum dots (CQDs) using superconducting-nanowire single-photon detectors and temporal filtering of the photoluminescence decay curve. We find that high single-photon purities and high photon-generation rates can be simultaneously achieved by removing the signals originating from the sequential two-photon emission of biexcitons created by multiple excitation pulses. We successfully demonstrate that the ultrahigh performance of the room-temperature single-photon sources showing g(2)(0) ≪ 10−2 can be confirmed by the ultralow-dark-count detection of the temporally purified single photons. These findings provide strong evidence for the attractiveness of CQDs as candidates for high-quality room-temperature quantum light sources.

Room temperature continuous-wave excited biexciton emission in perovskite nanoplatelets via plasmonic nonlinear fano resonance

Biexcitons are a manifestation of many-body excitonic interactions, which are crucial for quantum information and computation in the construction of coherent combinations of quantum states. However, due to their small binding energy and low transition efficiency, most biexcitons in conventional semiconductors exist either at cryogenic temperatures or under femto-second pulse laser excitation. Herein, we demonstrated strong biexciton emissions from CsPbBr3 nanoplatelets with continuous-wave excitation at room temperature by coupling them with a plasmonic nanogap. The exciton occupancy required to generate biexciton was reduced ~106 times in the Ag nanowire–Ag film nanogaps. The extremely large enhancement of biexciton emissions was driven by nonlinear Fano resonance between biexcitons and surface plasmon cavity modes. These results provide new pathways to develop high efficiency non-blinking single photon sources of biexciton (with spectral filter for biexciton), entangled light sources, and lasers based on biexciton states.

Plasmon-Assisted Suppression of Surface Trap States and Enhanced Band-Edge Emission in a Bare CdTe Quantum Dot.

Colloidal quantum dots have emerged as a versatile photoluminescent and optoelectronic material. Limitations like fluorescence intermittency, nonradiative Auger recombination, and surface traps are commonly addressed by growing a wide-band-gap shell. However, the shell isolates the excitonic wave function and reduces its interaction with the external environment necessary for different applications. Furthermore, their long emission lifetime hinders their use in high-speed optoelectronics. Here, we demonstrate a high degree of control on the photophysics of a bare core CdTe quantum dot solely by plasmon coupling, showing that more than 99% of the surface defect-state emission from a trap-rich quantum dot can be quenched. Moreover, the band-edge state excitonic and biexcitonic emission rates are Purcell enhanced by 1460- and 613-fold, respectively. Our findings show how plasmon coupling on bare quantum dots could make chemical approaches developed for improving their optical properties unnecessary, with implications for nanoscale lasers, light-emitting devices, solar cells, and ultrafast single-photon sources.

Enhancement of Biexciton Emission Due to Long-Range Interaction of Single Quantum Dots and Gold Nanorods in a Thin-Film Hybrid Nanostructure.

Semiconductor quantum dots (QDs) are known for their ability to exhibit multiphoton emission caused by recombination of biexcitons (BX). However, the quantum yield (QY) of BX emission is low due to the fast Auger process. Plasmonic nanoparticles (PNPs) provide an attractive opportunity to accelerate BX radiative recombination. Here, we demonstrate the PNPs induced distance-controlled enhancement of BX emission of single QDs. Studying the same single QD before and after its integration with the PNPs, we observed a plasmon-mediated increase in the QY of BX emission. Remarkably, the enhancement of BX emission remains pronounced even at distances of 170 nm. We attribute this effect to efficient coupling, which results in the trade-off between resonance energy transfer from QD to gold nanorods and the Purcell effect at small QD-PNP separations and the predominant influence of the Purcell effect at longer distances. Our findings constitute a reliable approach to managing the efficiency of multiexciton emission over a wide span of distances, thus paving the way for new applications.

Photoluminescence Properties of Thin-Film Nanohybrid Material Based on Quantum Dots and Gold Nanorods

Semiconductor quantum dots (QDs) have been demonstrated to be a promising material for developing innovative optoelectronic systems and lasers. The strong and weak coupling effects between localized plasmons in noble metal nanoparticles and excitons in QDs can modulate photoluminescence properties of the latter, scaling up their applications. In particular, these effects can strongly affect the photoluminescence (PL) lifetime of QDs, opening prospects for significantly increasing the quantum yield of the biexciton emission in single QD. Here, we provide а convincing proof of the formation of many-exciton states in hybrid material based on CdSe/ZnS/CdS/ZnS core/multishell QDs and gold nanorods (NRs) embedded in thin films of PMMA. The presence of NRs causes at least an order-of-magnitude decrease in the PL lifetimes of single QD. The obtained results have demonstrated the possibility of detecting biexciton states in QDs as the main component of emission of the hybrid QD-NR material.

Synthesis of Anisotropic CdSe/CdS Dot-in-Giant-Rod Nanocrystals with Persistent Blue-Shifted Biexciton Emission

Anisotropic single-phase wurtzite CdSe/CdS nanocrystals were synthesized by colloidal chemistry, introducing ZnCl2 to increase the shell growth in the radial direction. As a result, dot-in-giant-rod nanocrystals were obtained, with a core diameter that varied between 3.2 and 7.5 nm and an overall diameter between 15 and 22 nm, corresponding to a 14–26 ML CdS shell. In addition to an extended fluorescence lifetime, typical for CdSe/CdS heteronanocrystals, all samples also yielded a blue-shifted biexciton emission peak. This contrasts with existing data on CdSe/CdS dot-in-rod nanocrystals with a thin shell, which yield a type-I band offset and attractive biexciton interactions for CdSe/CdS with a core larger than about 2.8 nm. However, k·p calculations support the blue shift, with a significant electron delocalization into the CdS shell even for large core diameter. We assign this effect to the influence of strain at the CdSe/CdS interface and associated reduction of the conduction band offset, as well as the buildup of a piezoelectric field along the nanorod long axis. The strain-induced electron–hole separation is particularly effective in large-core nanocrystals, providing a tool to engineer electron and hole wave functions that is complementary to quantum confinement.

Zeeman Splitting and Inverted Polarization of Biexciton Emission in Monolayer WS_{2}.

Atomically thin semiconductors provide an ideal testbed to investigate the physics of Coulomb-bound many-body states. We shed light on the intricate structure of such complexes by studying the magnetic-field-induced splitting of biexcitons in monolayer WS_{2} using polarization-resolved photoluminescence spectroscopy in out-of-plane magnetic fields up to 30T. The observed g factor of the biexciton amounts to about -3.9, closely matching the g factor of the neutral exciton. The biexciton emission shows an inverted circular field-induced polarization upon linearly polarized excitation; i.e., it exhibits preferential emission from the high-energy peak in a magnetic field. This phenomenon is explained by taking into account the hybrid configuration of the biexciton constituents in momentum space and their respective energetic behavior in magnetic fields. Our findings reveal the critical role of dark excitons in the composition of this many-body state.

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.

Acoustically regulated optical emission dynamics from quantum dot-like emission centers in GaN/InGaN nanowire heterostructures

We report on experimental studies of the effects induced by surface acoustic waves on the optical emission dynamics of GaN/InGaN nanowire quantum dots. We employ stroboscopic optical excitation with either time-integrated or time-resolved photoluminescence detection. In the absence of the acoustic wave, the emission spectra reveal signatures originated from the recombination of neutral exciton and biexciton confined in the probed nanowire quantum dot. When the nanowire is perturbed by the propagating acoustic wave, the embedded quantum dot is periodically strained and its excitonic transitions are modulated by the acousto-mechanical coupling. Depending on the recombination lifetime of the involved optical transitions, we can resolve acoustically driven radiative processes over time scales defined by the acoustic cycle. At high acoustic amplitudes, we also observe distortions in the transmitted acoustic waveform, which are reflected in the time-dependent spectral response of our sensor quantum dot. In addition, the correlated intensity oscillations observed during temporal decay of the exciton and biexciton emission suggest an effect of the acoustic piezoelectric fields on the quantum dot charge population. The present results are relevant for the dynamic spectral and temporal control of photon emission in III-nitride semiconductor heterostructures.

Enhanced biexciton emission from single quantum dots encased in N-type semiconductor nanoparticles

By encasing single near-infrared emitting CdSeTe/ZnS3ML core/multishell quantum dots (QDs) in N-type semiconductor indium tin oxide (ITO) nanoparticles, an enhanced biexciton emission can be realized. The ITO nanoparticles with a high electron density can increase the dielectric screening of single QDs to reduce the Coulomb interactions between carriers, thus suppressing the nonradiative Auger recombination of biexcitons. It is observed that an average g(2)(0) = 0.57 in the second-order correlation function curves, which indicates the effective creation of biexciton and subsequent two-photon emission from single QDs encased in ITO nanoparticles. The fluorescence quantum yield ratio of the biexciton to single-exciton emission is increased to ∼4.8 times, while the Auger recombination rate reduces by almost an order of magnitude.