Bidirectional bandgap tuning of single quantum dot by tip-induced phase transition

A phase transition material, VO2, with a semiconductor-to-metal transition (SMT) near 341 K (68 °C) has attracted significant research interest because of drastic changes in its electrical resistivity and optical dielectric properties. To address its application needs at specific temperatures, tunable SMT temperatures are highly desired. In this work, effective transition temperature (Tc) tuning of VO2 has been demonstrated via a novel Pt : VO2 nanocomposite design, i.e., uniform Pt nanoparticles (NPs) embedded in the VO2 matrix. Interestingly, a bidirectional tuning has been achieved, i.e., the transition temperature can be systematically tuned to as low as 329.16 K or as high as 360.74 K, with the average diameter of Pt NPs increasing from 1.56 to 4.26 nm. Optical properties, including transmittance (T%) and dielectric permittivity (ε') were all effectively tuned accordingly. All Pt : VO2 nanocomposite thin films maintain reasonable SMT properties, i.e. sharp phase transition and narrow width of thermal hysteresis. The bidirectional Tc tuning is attributed to two factors: the reconstruction of the band structure at the Pt : VO2 interface and the change of the Pt : VO2 phase boundary density. This demonstration sheds light on phase transition tuning of VO2 at both room temperature and high temperature, which provides a promising approach for VO2-based novel electronics and photonics operating under specific temperatures.

Memristors as electronic artificial synapses have attracted increasing attention in neuromorphic computing. Emulation of both “learning” and “forgetting” processes requires a bidirectional progressive adjustment of memristor conductance, which is a challenge for cutting‐edge artificial intelligence. In this work, a memristor device with a structure of Ag/Zr0.5Hf0.5O2:graphene oxide quantum dots/Ag is presented with the feature of bidirectional progressive conductance tuning. The conductance of proposed memristor is adjusted through voltage pulse number, amplitude, and width. A series of voltage pulses with an amplitude of 0.6 V and a width of 30 ns is enough to modulate conductance. The impacts of pulses with different parameters on conductance modulation are investigated, and the potential relationship between pulse amplitude and energy is revealed. Furthermore, it is proved that the pulse with low energy can realize the almost linear conductance regulation, which is beneficial to improve the accuracy of pattern recognition. The bidirectional progressive conduction modulation mimics various plastic synapses, such as spike‐timing‐dependent plasticity and paired‐pulse facilitation. This progressive conduction tuning mechanism might be attributed to the coexistence of tunneling effect and extrinsic electrochemical metallization effect. This work provides one way for memristor to attain attractive features such as bidirectional tuning, low‐power consumption, and fast speed switching that is in urgent demand for further evolution of neuromorphic chips.

Normally, wave functions in single quantum dots can be tuned transversely by a perpendicular magnetic field because of the cyclotron energy. In this work, we are presenting a longitudinal wave function control in single quantum dots with a magnetic field. For a pure InAs quantum dot with a shape of pyramid or truncated pyramid, the hole wave function always occupies the base because of the less confinement at base, which induces a permanent dipole oriented from base to apex. With applying magnetic field, the hole wave function shrinks in the base plane, resulting in that the center of effective mass moves towards apex. For electrons, however, the center of effective mass does not move much. This induces a permanent dipole moment change and an inverted electron-hole alignment along the magnetic field direction. Manipulating the wave function longitudinally not only provides an alternative way to control the charge distribution with magnetic field but also a new method to tune electron-hole interaction in single quantum dots. Additionally, the many-body exciton states in a coupled system with a single self-assembled quantum dot and a wetting layer are observed by strong anomalous diamagnetic shifts. A tremendous positive diamagnetic coefficient is observed when an electron in the wetting layer combines with a hole in quantum dot, which is nearly one order of magnitude larger than that of the excitonic states confined in quantum dots. When the electrons recombine with holes within quantum dot in the coupled system, a peculiar negative diamagnetic effect is observed. The properties of emitted photons depending on the large electron wave function extents in wetting layer indicate the coupling between the systems in different dimensionality, which was also verified by a magnetic field applied in different configurations.

We report about spatially resolved experiments on self-assembled InGaAs quantum dots. Single quantum dots can be investigated by using STM-induced luminescence spectroscopy. The quantum dot occupancy can be increased via the STM tip current, which results in state filling and therefore in the onset of discrete excited state luminescence. In the limit of low injection currents, a single emission line from the ground state of the dot is observed. Using near-field spectroscopy through shadow masks, we have investigated the optical properties of single self-assembled InGaAs quantum dots as a function of occupancy and magnetic field. This allows us to fully resolve diamagnetic/orbital effects, Zeeman splitting, and to determine manybody-corrections. Photoluminescence excitation spectra further reveal a strong contribution of phonon assisted processes in quantum dot absorption.

A technique is described which allows one to position a single InAs quantum dot or quantum dot arrays on the top of square based, pyramidal shaped InP nano-templated mesas. A simple geometrical calculation shows 80% of the InP material is incorporated during the template formation. Positioning of either a single quantum dot or quantum dot arrays is achieved depending on the size of the mesa top surface and the amount of dot material deposited as shown using both scanning electron microcopy and optical microscopy. Photoluminescence spectra from a single InAs quantum dot exhibits a clear s- and p-shell structure for the first time in this material system.

We report on the magneto-optical study of spin polarized energetic fine structures for exciton complex in single CdSe quantum dot (QD) by using micro- photoluminescence (micro-PL) spectroscopy. The zero-field splitting of exciton luminescence peak arisen from the anisotropic exchange interaction of carriers in the QDs was observed. The g-factors for exciton and negatively-charged exciton, i.e. trion in a single QD were determined by fitting the magnetic field dependence of the corresponding PL peaks. By exciting the single QD with circularly polarized light of σ- and σ+ polarization, the spin-up and spin-down trions were selectively generated. The ratio, τ/τsf, of the exciton lifetime and the time constants for the spin-flipping process of trion in a single QD was estimated to be 0.13, which implies a long spin-lifetime in single CdSe QD.

Single self-assembled quantum dots are among the most widely studied systems in the field of modern solid state spectroscopy. Neutral multi-exciton complexes have been investigated in quantum dots by power dependent photoluminescence spectroscopy. The experimental preparation of specific charged exciton states in a single quantum dot can be realized by bias controlled single electron charging and can be probed by optical spectroscopy. With respect to neutral single exciton configurations, the optical response of charged exciton complexes is modified due to few particle interaction of the carriers confined in the quantum dot. As a consequence of these renormalization effects we observe different emission energies for the neutral, single, and double charged excitons in single quantum dot spectroscopy. A quantitative comparison of the experimentally determined binding energies for single and double charged excitons with theoretical model calculations demonstrates a substantially stronger confinement of the hole wave function with respect to the electron wave function. The observation of spin dependent tunneling from singlet and triplet states at high magnetic fields nicely demonstrates that spin related phenomena can be considerably enhanced in quantum dots. The influence of the sample structure can be seen by the appearance of charge equilibrium and non-equilibrium states in bias dependent photoluminescence spectra of different single quantum dot photodiodes.

Summary form only given. Direct observations of the dynamics of single excitonic quantum dots require the use of transient optical spectroscopy. Measurements of the lifetimes of single QD states, Rabi oscillations, biexciton formation and decay, and the development of quantum logic gates are examples of dynamical effects in quantum dots most easily studied through transient nonlinear spectroscopy, but are extremely challenging at the single dot level. We report here the first observation of transient differential transmission from single quantum dots as well as evidence of Rabi oscillations in single quantum dots.Under investigation are quantum dots naturally formed by interface fluctuations in a 42 /spl Aring/ GaAs/Al/sub 0.3/Ga/sub 0.7/As quantum well. Excitons in isolated QD's are probed through 500 nm apertures in an Al mask laid directly onto the sample's surface.

The photoluminescence of single CdSe quantum dots in ZnSe grown by molecular beam epitaxy and that of the same system grown by atomic layer epitaxy were investigated. The spectral diffusion and on/off behaviour of single CdSe quantum dots were observed, and the spectral diffusion range was only about 1 meV. The spectral peak shifting became quicker as the temperature rose. The spectral change from blue-shift to red-shift (or vice versa) was much quicker than that found in CdSe quantum dots synthesized as colloids. The phenomena are qualitatively explained by a Stark effect which originated from an Auger ionization process. The spectral diffusion may be a common property among single quantum dots.

Photoluminescence blinking behavior from single quantum dots under steady illumination is an important but controversial topic. Its occurrence has impeded the use of single quantum dots in bioimaging. Different mechanisms have been proposed to account for it, although controversial, the most important of which is the non-radiative Auger recombination mechanism whereby photocharging of quantum dots can lead to the blinking phenomenon. Here, the singly charged trion, which maintains photon emission, including radiative recombination and non-radiative Auger recombination, leads to fluorescence non-blinking which is observed in photocharged single graphene quantum dots (GQDs). This phenomenon can be explained in terms of different energy levels in the GQDs, caused by various oxygen-containing functional groups in the single GQDs. The suppressed blinking is due to the filling of trap sites owing to a Coulomb blockade. These results provide a profound understanding of the special optical properties of GQDs, affording a reference for further in-depth research.

We report on the use of an aperture in an aluminum oxide layer to restrict current injection into a single self-assembled InAs quantum dot from an ensemble of such dots within a large mesa. The insulating aperture is formed through the wet oxidation of a layer of AlAs. Under photoluminescence we observe that only one quantum dot in the ensemble exhibits a Stark shift, and that the same single dot is visible under electroluminescence. Autocorrelation measurements performed on the electroluminescence confirm that we are observing emission from a single quantum dot.

Interferometric spectroscopy for excitons in InP single quantum dots

Single quantum dots have many potential applications across the field of quantum computation, ranging from the generation of single photons or entangled photon pairs to the storage and manipulation of qubits. Single InAs quantum dots are optically active and thus can be used as an interface between photonic flying qubits and spin-based stationary qubits. Incorporating single InAs quantum dots into semiconductor devices allows the stationary qubits to be manipulated, making this system a promising candidate for quantum computation. It is well known that the exciton state of quantum dots is split into two polarisation dependent states; the energy difference between the states is the fine-structure splitting, (s). A vertical electric field has been used to tune |s| over a large range of ∼ 100μeV, such that a dot which has |s| over 50μeV at zero field has been tuned to emit polarisation entangled photon pairs[1]. We observe coherent coupling between the two polarisation eigenstates. This coupling results in an anticrossing as the two states are tuned close to each other, and a rotation of the eigenstates through 90° as |s| is swept through its minimum value.

Subject of study. A single InAs quantum dot in a one-dimensional photonic crystal based on GaAs is examined. Aim of study. The aim of this study is to develop a method for controlling photon emission frequencies from a single quantum dot within a one-dimensional photonic crystal based on changes in the electromagnetic mass of an electron in the photonic crystal medium. Method. The proposed approach leverages the effect of changing the electromagnetic mass of an electron in the photonic crystal medium, manifesting as corrections to electron energy levels depending on the optical density of the medium. To control this density, the injection of free charge carriers and the quadratic electro-optic Kerr effect are proposed. Main results. The feasibility of in situ control of photon emission frequencies from a quantum dot was demonstrated using quantum transitions between the p- and s-states of a hydrogen-like InAs quantum dot situated in the air voids of a one-dimensional GaAs photonic crystal. This control is achieved through the effect of changing the electromagnetic mass of an electron, as well as tuning the refractive index of the photonic crystal via free charge carrier injection and the electro-optic Kerr effect. Calculations indicate that the photon energy control range available in experiments is limited to several tens of microelectronvolts, restricting practical applicability, and the observed displacement effect is smaller than experimentally recorded values. However, the energy level displacement, influenced by the quantum electrodynamic effect under investigation, exhibits a quadratic dependence on the refractive index of the material forming the photonic crystal. Consequently, the method is expected to scale significantly with increasing optical density. Such photonic crystals could be constructed using metamaterials with a high refractive index. Practical significance. The findings of this study, centered on developing a method for controlling photon emission frequencies from a single quantum dot in a one-dimensional photonic crystal, lay the groundwork for photon-emitter interfaces. These interfaces will incorporate key quantum functionalities, including photonic qubits, single-photon light sources, and nonlinear quantum photon-photon gates.

Formamidinium lead bromide (FAPbBr3) quantum dots (QDs) are promising materials for light emitting applications in the visible spectral region because of their high photoluminescence (PL) quantum yield (QY) and the enhanced chemical stability as compared to, for instance, methylammonium based analogues. Toward practical harnessing of their compelling optical characteristics, the exciton recombination process, and in particular the exciton-phonon interaction and the impact of crystal phase transition, has to be understood in detail. This is addressed in this contribution by PL studies on single colloidal FAPbBr3 QDs. Polarization-resolved PL measurements reveal a fine structure splitting of excitonic transitions due to the Rashba effect. Distinct phonon replica have been observed within energetic distances of 4.3 ± 0.5, 8.6 ± 0.9, and 13.2 ± 1.1 meV from the zero phonon line, which we attribute to vibrational modes of the lead bromide lattice. Additional vibrational modes of 18.6 ± 0.3 and 38.8 ± 1.1 meV are found and related to liberation modes of the formamidinium (FA) cation. Temperature-dependent PL spectra reveal a line broadening of the emission caused by exciton phonon interaction as well an unusual energy shift which is attributed to a crystal phase transition within the single QD.