Charged Exciton Emission Research Articles

Local piezoelectric doping of monolayer WSe2

We report non-contact local doping of a monolayer WSe2 transferred onto a piezoelectric substrate having surface potential wells (SPWs) induced by structural inhomogeneities. We used epitaxial GaN and InP/GaInP2 structures, in which there are SPWs ∼0.2 V deep and 0.1–2 μm in size. Using surface topography and potential scanning probe microscopy, as well as optical reflectance, photoluminescence, and Raman spectroscopy measurements, we observed strong enhancement of charged exciton emission and Raman intensity in the SPW regions of the monolayer WSe2, which indicate on piezoelectric doping at a level n ≥ 1012 cm−2 on a length scale ∼0.2–1 μm. Our results can be used to create electron/hole quantum puddles with anyon states in transition metal dichalcogenides, promising for the development of room temperature and magnetic-field-free fault-tolerant topological quantum computing.

Room‐Temperature Low‐Voltage Control of Excitonic Emission in Transition Metal Dichalcogenide Monolayers

AbstractCharge doping of materials with 2D and 3D quantum confinement is a flexible tool to tailor their excitonic emission. Here, using electron doping experiments on transition metal dichalcogenide (TMD) monolayers, reversible tuning of charged exciton emission within a redshift of up to 75 meV is demonstrated by applying very modest voltages (corresponding roughly to the band gap of TMDs), while also controlling the radiative lifetime and intensity. It is found that the neutral exciton ionization dynamics at increasing electron doping follows the Fermi–Dirac distribution, which allows to determine the size of the band gap as well as to extract experimental values for effective masses of electrons and holes at room temperature. The tunable excitonic emission, preserving coherence at room temperature, holds great promise for quantum technologies requiring deterministic coupling with integrated photonic and plasmonic devices.

Wafer-Scale Epitaxial Growth of Unidirectional WS2 Monolayers on Sapphire.

Realization of wafer-scale single-crystal films of transition metal dichalcogenides (TMDs) such as WS2 requires epitaxial growth and coalescence of oriented domains to form a continuous monolayer. The domains must be oriented in the same crystallographic direction on the substrate to inhibit the formation of inversion domain boundaries (IDBs), which are a common feature of layered chalcogenides. Here we demonstrate fully coalesced unidirectional WS2 monolayers on 2 in. diameter c-plane sapphire by metalorganic chemical vapor deposition using a multistep growth process to achieve epitaxial WS2 monolayers with low in-plane rotational twist (0.09°). Transmission electron microscopy analysis reveals that the WS2 monolayers are largely free of IDBs but instead have translational boundaries that arise when WS2 domains with slightly offset lattices merge together. By regulating the monolayer growth rate, the density of translational boundaries and bilayer coverage were significantly reduced. The unidirectional orientation of domains is attributed to the presence of steps on the sapphire surface coupled with growth conditions that promote surface diffusion, lateral domain growth, and coalescence while preserving the aligned domain structure. The transferred WS2 monolayers show neutral and charged exciton emission at 80 K with negligible defect-related luminescence. Back-gated WS2 field effect transistors exhibited an ION/OFF of ∼107 and mobility of 16 cm2/(V s). The results demonstrate the potential of achieving wafer-scale TMD monolayers free of inversion domains with properties approaching those of exfoliated flakes.

Stable charged exciton in a ZnO/(Zn,Mg)O quantum well at near room temperature

We report on the binding energy of a charged exciton (trion) confined in a single, epitaxially grown 1.7 nm thick ZnO/(Zn,Mg)O quantum well as large as 22 meV or 27.6 meV when determined in micro-photoluminescence or transmission measurements, respectively. Charged exciton emission is found to persist up to near room temperature. The binding energy comparable to thermal energy at room temperature is promising for trion based spintronic and optoelectronic applications.

Optical and electronic properties of low-density InAs/InP quantum-dot-like structures designed for single-photon emitters at telecom wavelengths

Due to their band-structure and optical properties, InAs/InP quantum dots (QDs) constitute a promising system for single-photon generation at third telecom window of silica fibers and for applications in quantum communication networks. However, obtaining the necessary low in-plane density of emitters remains a challenge. Such structures are also still less explored than their InAs/GaAs counterparts regarding optical properties of confined carriers. Here, we report on the growth via metal-organic vapor phase epitaxy and investigation of low-density InAs/InP QD-like structures, emitting in the range of 1.2-1.7 ${\mu}$m, which includes the S, C, and L bands of the third optical window. We observe multiple photoluminescence (PL) peaks originating from flat QDs with height of small integer numbers of material monolayers. Temperature-dependent PL reveals redistribution of carriers between families of QDs. Via time-resolved PL, we obtain radiative lifetimes nearly independent of emission energy in contrast to previous reports on InAs/InP QDs, which we attribute to strongly height-dependent electron-hole correlations. Additionally, we observe neutral and charged exciton emission from spatially isolated emitters. Using the 8-band k${\cdot}$p model and configuration-interaction method, we successfully reproduce energies of emission lines, the dispersion of exciton lifetimes, carrier activation energies, as well as the biexciton binding energy, which allows for a detailed and comprehensive analysis of the underlying physics.

Engineering radiative coupling of excitons in 2D semiconductors

The resonance energy and the transition rate of atoms, molecules and solids were understood as their intrinsic properties in classical electromagnetism. With the development of quantum electrodynamics, it is realized that these quantities are linked to the coupling of the transition dipole and the quantum vacuum. Such effects can be greatly amplified in macroscopic many-body systems from virtual photon exchange between dipoles, but are often masked by inhomogeneity and pure dephasing, especially in solids. Here, we observe an exceptionally large renormalization of exciton resonance and radiative decay rate in transition metal dichalcogenides monolayers due to interactions with the vacuum in both absorption and emission spectroscopy. Tuning the vacuum energy density near the monolayer, we demonstrate control of cooperative Lamb shift, radiative decay, and valley polarization as well as control of the charged exciton emission. Our work establishes a simple and robust experimental system for vacuum engineering of cooperative matter-light interactions.

Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit

We demonstrate the reduction of the inhomogeneous linewidth of the free excitons in atomically thin transition metal dichalcogenides (TMDCs) MoSe2, WSe2 and MoS2 by encapsulation within few nanometre thick hBN. Encapsulation is shown to result in a significant reduction of the 10 K excitonic linewidths down to ∼3.5 meV for n-MoSe2, ∼5.0 meV for p-WSe2 and ∼4.8 meV for n-MoS2. Evidence is obtained that the hBN environment effectively lowers the Fermi level since the relative spectral weight shifts towards the neutral exciton emission in n-doped TMDCs and towards charged exciton emission in p-doped TMDCs. Moreover, we find that fully encapsulated MoS2 shows resolvable exciton and trion emission even after high power density excitation in contrast to non-encapsulated materials. Our findings suggest that encapsulation of mechanically exfoliated few-monolayer TMDCs within nanometre thick hBN dramatically enhances optical quality, producing ultra-narrow linewidths that approach the homogeneous limit.

Pressure-Dependent Light Emission of Charged and Neutral Excitons in Monolayer MoSe2.

Tailoring the excitonic properties in two-dimensional monolayer transition metal dichalcogenides (TMDs) through strain engineering is an effective means to explore their potential applications in optoelectronics and nanoelectronics. Here we report pressure-tuned photon emission of trions and excitons in monolayer MoSe2 via a diamond anvil cell (DAC) through photoluminescence measurements and theoretical calculations. Under quasi-hydrostatic compressive strain, our results show neutral (X0) and charged (X-) exciton emission of monolayer MoSe2 can be effectively tuned by alcohol mixture vs inert argon pressure transmitting media (PTM). During this process, X- emission undergoes a continuous blue shift until reaching saturation, while X0 emission turns up splitting. The pressure-dependent charging effect observed in alcohol mixture PTM results in the increase of the X- exciton component and facilitates the pressure-tuned emission of X- excitons. This substantial tunability of X- and X0 excitons in MoSe2 can be extended to other 2D TMDs, which holds potential for developing strained and optical sensing devices.

Enhanced emission of charged-exciton polaritons from colloidal quantum dots on a SiN/SiO2 slab waveguide.

We investigate the photoluminescence (PL) spectra and the time-resolved PL decay process from colloidal quantum dots on SiN/SiO2 wet etched via BOE (HF:NH4F:H2O). The spectrum displays multi-peak shapes that vary with irradiation time. The evolution of the spectral peaks with irradiation time and collection angle demonstrates that the strong coupling of the charged-exciton emission to the leaky modes of the SiN/SiO2 slab waveguide predominantly produces short-wavelength spectral peaks, resulting in multi-peak spectra. We conclude that BOE etching enhances the charged-exciton emission efficiency and its contribution to the total emission compared with the unetched case. BOE etching smoothes the electron confinement potential, thus decreasing the Auger recombination rate. Therefore, the charged-exciton emission efficiency is high, and the charged-exciton-polariton emission can be further enhanced through strong coupling to the leaky mode of the slab waveguide.

Valley splitting and polarization by the Zeeman effect in monolayer MoSe2.

We have measured circularly polarized photoluminescence in monolayer MoSe2 under perpendicular magnetic fields up to 10 T. At low doping densities, the neutral and charged excitons shift linearly with field strength at a rate of ∓0.12 meV/T for emission arising, respectively, from the K and K' valleys. The opposite sign for emission from different valleys demonstrates lifting of the valley degeneracy. The magnitude of the Zeeman shift agrees with predicted magnetic moments for carriers in the conduction and valence bands. The relative intensity of neutral and charged exciton emission is modified by the magnetic field, reflecting the creation of field-induced valley polarization. At high doping levels, the Zeeman shift of the charged exciton increases to ∓0.18 meV/T. This enhancement is attributed to many-body effects on the binding energy of the charged excitons.

Charge tuning in [111] grown GaAs droplet quantum dots

We demonstrate charge tuning in strain free GaAs/AlGaAs quantum dots (QDs) grown by droplet epitaxy on a GaAs(111)A substrate. Application of a bias voltage allows the controlled charging of the QDs from −3|e| to +2|e|. The resulting changes in QD emission energy and exciton fine-structure are recorded in micro-photoluminescence experiments at T = 4 K. We uncover the existence of excited valence and conduction states, in addition to the s-shell-like ground state. We record a second series of emission lines about 25 meV above the charged exciton emission coming from excited charged excitons. For these excited interband transitions, a negative diamagnetic shift of large amplitude is uncovered in longitudinal magnetic fields.

Charge state control in single InAs/GaAs quantum dots by external electric and magnetic fields

We report a photoluminescence (PL) spectroscopy study of charge state control in single self-assembled InAs/GaAs quantum dots by applying electric and/or magnetic fields at 4.2 K. Neutral and charged exciton complexes were observed under applied bias voltages from −0.5 V to 0.5 V by controlling the carrier tunneling. The highly negatively charged exciton emission becomes stronger with increasing pumping power, arising from the fact that electrons have a smaller effective mass than holes and are more easily captured by the quantum dots. The integrated PL intensity of negatively charged excitons is affected significantly by a magnetic field applied along the sample growth axis. This observation is explained by a reduction in the electron drift velocity caused by an applied magnetic field, which increases the probability of non-resonantly excited electrons being trapped by localized potentials at the wetting layer interface, and results in fewer electrons distributed in the quantum dots. The hole drift velocity is also affected by the magnetic field, but it is much weaker.

Surface recombination and charged exciton in nanocrystal quantum dots on photonic crystals under two-photon excitation.

In this study, the two-photon excited fluorescence spectra from cadmium selenide quantum dots (QDs) on a silicon nitride photonic crystal (PhC) membrane under femtosecond laser irradiation were investigated. These spectra can be fit to a tri-Gaussian function in which one component is negative in amplitude, and in which the Gaussian components with positive amplitude are assigned to exciton emission and charged-exciton emission and that with negative amplitude is assigned to absorption from surface recombination. The photonic crystal enhance the charged-exciton emission and exciton emission and, at the same time, also the absorption from surface recombination. Both the charged-exciton emission and the surface recombination are related to Auger recombination; therefore, the photonic crystal controls both radiative recombination and non-radiative recombination. The asymmetries of the two-photon excited fluorescence spectra are due to not only the location of the resonant guide mode of the PhC slab but also the enhancement of the absorption from surface recombination by PhC.

Impact of heavy hole-light hole coupling on optical selection rules in GaAs quantum dots

We report strong heavy hole-light hole mixing in GaAs quantum dots grown by droplet epitaxy. Using the neutral and charged exciton emission as a monitor we observe the direct consequence of quantum dot symmetry reduction in this strain free system. By fitting the polar diagram of the emission with simple analytical expressions obtained from k⋅p theory we are able to extract the mixing that arises from the heavy-light hole coupling due to the geometrical asymmetry of the quantum dot.

Exciton Recombination and Upconverted Photoluminescence in Colloidal CdSe Quantum Dots

We studied photoluminescence (PL) of colloidal CdSe quantum dots (QDs) synthesized by a single-step method using cadmium oxide (CdO) and tri-n-octylphosphine selenide (TOPSe) as the Cd and Se sources, respectively, and tri-n-octylphosphine (TOP) as the reaction medium and subsequently dispersed in hexane. The QDs were excited by a narrow-band incoherent cw light source with photon energies near or below the first absorption maximum of the sample, and the resulting luminescence was dispersed and recorded. In the PL spectra, we identified two displaced by ∼16−38 meV strongly overlapping components with excitation energy dependent intensities. We also investigated lifetimes of the nonresonant PL decay at various excitation and emission energies using a frequency-domain method and observed multiexponential decay with three lifetimes approximately equal to 11.5(1.0), 41(2), and 155(15) ns. The low-energy component with the full width at half-maximum (fwhm) ranging from 135−155 meV was assigned to the charged exciton emission correlating with the shortest lifetime. The narrower high-energy component with the fwhm ranging from 80−90 meV was attributed to the band edge exciton emission with the middle lifetime. Photoexcitation of the QD sample in the onset of the absorption tail yielded blue-shifted (upconverted) luminescence. The blue-shifted PL was determined to result from a single-photon excitation. Therefore, we claimed that the upconversion process was thermally assisted. Numerical modeling showed the blue shift to be consistent with room temperature thermal phonon distribution in the colloidal QDs.

Charging of a InAs/GaAs single quantum dot from a n-ZnMnSe spin aligner

We demonstrate charging of a single InAs/GaAs quantum dot (SQD) via bias controlled electron tunneling from a n-doped ZnMnSe spin aligner. The single dot photoluminescence spectra show clear signatures of single charged exciton emission X − and the intensity ratio between charged and neutral exciton can be controlled via the external bias. These data emphasis that, in spite of the complications of the conduction band offset between ZnMnSe and GaAs, a SQD charging is feasible in this II–VI–III–V hybrid structure.

Charged exciton emission at 1.3μm from single InAs quantum dots grown by metalorganic chemical vapor deposition

We have studied the emission properties of self-organized InAs quantum dots (QDs) grown in an InGaAs quantum well by metalorganic chemical vapor deposition. Low-temperature photoluminescence spectroscopy shows emission from single QDs around 1300nm; we clearly observe the formation of neutral and charged exciton and biexciton states, and we obtain a biexciton binding energy of 3.1meV. The dots exhibit an s-p shell splitting of approximately 100meV, indicating strong confinement.

Electric Field Induced Switching of the Fluorescence of Single Semiconductor Quantum Rods

The exceptional fluorescence properties of single CdSe quantum rods (QRs) arising from internal and external electric fields are studied. Reversible external field induced switching of the emission in single QRs is reported for the first time. This effect was correlated with local field induced emission intensity reduction and newly observed darkening mechanism. Bimodal spectral jumps under a zero field were also observed and assigned to charged exciton emission, a phenomenon that was likewise directly controlled through an external field. These phenomena point to the use of single QRs as spectrally tunable charge sensitive fluorophores with polarized emission in fluorescence tagging and optical switching applications.

Surface-enhanced emission from single semiconductor nanocrystals.

The fluorescence behavior of single CdSe(ZnS) core-shell nanocrystal (NC) quantum dots is dramatically affected by electromagnetic interactions with a rough metal film. Observed changes include a fivefold increase in the observed fluorescence intensity of single NCs, a striking reduction in their fluorescence blinking behavior, complete conversion of the emission polarization to linear, and single NC exciton lifetimes that are >10(3) times faster. The enhanced excited state decay process for NCs coupled to rough metal substrates effectively competes with the Auger relaxation process, allowing us to observe both charged and neutral exciton emission from these NC quantum dots.

Photon correlation spectroscopy of a single quantum dot

We report photon correlation measurements that allow us to observe unique signatures of biexcitons in a single self-assembled InAs quantum dot. Photon correlation measurements of biexciton emission exhibit both bunching and antibunching under continuous-wave excitation while only antibunching is observed under pulsed excitation. Cross-correlation between biexciton and single-exciton peaks reveal highly asymmetric features, demonstrating that biexciton and exciton emissions have strong correlations due to cascaded emission. The anticipated correlation between the polarization of exciton and biexciton emissions however, is absent under our excitation conditions. Photon correlation measurements also provide evidence for the identification of the charged exciton emission.