Transitions In Quantum Dots Research Articles

InAs/GaAs SK quantum dots stacking: Impact of spacer layer on optical properties

In this paper, we report the optical properties of vertically stacked multilayers of self-organized InAs/GaAs quantum dots QDs with different GaAs spacer layer thicknesses of 10 and 15 nm, using photoluminescence PL measurement. The 10 K PL spectrum exhibits double-emission peaks ambiguously identified in PL spectra where the excitation power dependence reveals that these emission peaks are attributed to fundamental ground state GS of large quantum dots in the low energy side, and first excited state 1ES transitions of large quantum dots in coincidence with fundamental ground state GS of smaller ones, in the high energy side. Both the excitation power dependence and the temperature dependence measurement results exhibited competition between the latter's optical transitions in the QDs, which becomes more prevalent at higher excitation powers. The main PL peak is quenched above 190 K, giving rise to “a 1D miniband”, ascribed to the electronic coupling between QDs along the stacking direction and tuning the emission wavelength around 1.3 μm.Our results emphasize the Key role of the vertically stacked InAs/GaAs QDs structures with thin GaAs spacer layers in optimizing design for long-wavelength devices.

Various nonlinear transitions of a self-assembled quantum dot (SA-QD) semiconductor laser subject to negative optoelectronic feedback

Various nonlinear transitions of a self-assembled quantum dot (SA-QD) semiconductor laser subject to negative optoelectronic feedback

Fluorescence Enhancement of CdS:Ag Quantum Dots Co-Assembled with Au Nanoparticles in a Hollow Nanosphere Form.

Colloidal quantum dots (QDs) have exceptional fluorescence properties. Overcoming aggregation-induced quenching and enhancing the fluorescence of colloidal QDs have remained a challenging issue in this field. In this study, composite hollow nanospheres composed of Au nanoparticles (NPs) and CdS:Ag-doped QDs were successfully constructed through controlled microemulsion-based cooperative assembly. This method harnessed the localized surface plasmon resonance (LSPR) effect of Au NPs nearby doped QDs, resulting in enhanced doped QD fluorescence and the observation of the Purcell effect. The composite hollow nanospheres show a fluorescence enhancement compared to that of the pure CdS:Ag QDs. The enhanced fluorescence was demonstrated to come from the synergetic enhancement of the absorption and emission transition of the doped QDs. This approach provides a feasible technological pathway to address the challenge of improving the fluorescence performance of the doped QDs.

Influence of external magnetic field on intraband transitions in lens-shaped quantum dot

Intraband linear and nonlinear optical absorption in a strongly oblate lens-shaped Ge/Si quantum dot in the presence of an axial magnetic field was theoretically studied. Quantum transitions are considered in the heavy hole subband, when the scalar effective mass approximation is correct. The linear and nonlinear absorption coefficients, refractive index changes and the second harmonic generation coefficient were determined. The influence of the effects of temperature, size quantization and magnetic field on the behavior of the above parameters was revealed.

Multimodule microwave assembly for fast readout and charge-noise characterization of silicon quantum dots

Fast measurements of quantum devices is useful in areas such as quantum sensing, quantum computing, and nanodevice quality analysis. Here, we develop a superconductor-semiconductor multimodule microwave assembly to demonstrate charge-state readout at the state of the art. The assembly consist of a superconducting readout resonator interfaced to a silicon-on-insulator (SOI) chiplet containing quantum dots (QDs) in a high-κ nanowire transistor. The superconducting chiplet contains resonant and coupling elements as well as LC filters that, when interfaced with the silicon chip, result in a resonant frequency f=2.12 GHz, a loaded quality factor Q=850, and a resonator impedance Z=470Ω. Combined with the large gate lever arms of SOI technology, we achieve a minimum integration time for single and double QD transitions of 2.77 and 13.5 ns, respectively. We utilize the assembly to measure charge noise over 9 decades of frequency up to 500 kHz and find a 1/f dependence across the whole frequency spectrum as well as a charge-noise level of 4μeV/Hz at 1 Hz. The modular microwave circuitry presented here can be directly utilized in conjunction with other quantum devices to improve the readout performance as well as enable large bandwidth noise spectroscopy, all without the complexity of superconductor-semiconductor monolithic fabrication. Published by the American Physical Society 2024

Polarization-Selective Enhancement of Telecom Wavelength Quantum Dot Transitions in an Elliptical Bullseye Resonator.

Semiconductor quantum dots are promising candidates for the generation of nonclassical light. Coupling a quantum dot to a device capable of providing polarization-selective enhancement of optical transitions is highly beneficial for advanced functionalities, such as efficient resonant driving schemes or applications based on optical cyclicity. Here, we demonstrate broadband polarization-selective enhancement by coupling a quantum dot emitting in the telecom O-band to an elliptical bullseye resonator. We report bright single-photon emission with a degree of linear polarization of 96%, Purcell factor of 3.9 ± 0.6, and count rates up to 3 MHz. Furthermore, we present a measurement of two-photon interference without any external polarization filtering. Finally, we demonstrate compatibility with compact Stirling cryocoolers by operating the device at temperatures up to 40 K. These results represent an important step toward practical integration of optimal quantum dot photon sources in deployment-ready setups.

Reversible hydrochromic CsPbBr3/Cs4PbBr6@MCM-41 to enable organic solvent polarity detection

Hydrochromic materials have received much attention in anticounterfeiting due to their reversible photoemission properties toward water. However, existing hydrochromic materials usually suffer from slow hydrochromic response and limited stability, repeatability, and color tunability. This paper found for the first time that CsPbBr3/Cs4PbBr6 composites with quantum-limited domain effects had reversible hydrochromism. CsPbBr3/Cs4PbBr6 composites were successfully synthesized in molecular sieve MCM-41 using an improved mechanochemical method. The composites underwent a reversible phase transition from Cs4PbBr6/CsPbBr3 to CsPbBr3 upon treatment with a trace amount of water, the photoluminescence colors underwent a change from blue to green, and reversion occurred due to heating. Mechanistic investigation revealed that quantum dots underwent soft agglomeration due to van der Waals forces in polar solvent environments, affecting the action of quantum domain-limiting effects. Therefore, organic solvents with different polarities can cause different degrees of reversible discoloration of the material. This study provides new ideas for understanding the phase transition and agglomeration of metal halide perovskite quantum dots in polar solvent environments. Additionally, it offered new options for aqueous color-changing materials and organic solvent polar detection materials.

Enhancement of Spontaneous Photon Emission in Inverse Photoemission Transitions in Semiconductor Quantum Dots.

Inverse photoemission (IPE) is a radiative electron capture process where an electron is transiently captured in the conduction band (CB) followed by intraband de-excitation and spontaneous photon emission. IPE in quantum dots (QDs) bypasses optical selection rules for populating the CB and provides insights into the capacity for electron capture in the CB, the propensity for spontaneous photon emission, intraband transition energies where both initial and final states are in the CB, and the generation of photons with frequencies lower than the bandgap. Here, we demonstrate using time-dependent perturbation theory that judicious application of electric fields can significantly enhance the IPE transition in QDs. For a series of CdSe, CdS, PbSe, and PbS QDs, we present evidence of field-induced enhancement of IPE intensities (188% for Cd54Se54), field-dependent control of emitted photon frequencies (Δω = 0.73 eV for Cd54Se54), and enhancement of light-matter interaction using directed Stark fields (103% for Cd54Se54).

Symmetry breaking via alloy disorder to explain radiative Auger transitions in self-assembled quantum dots

Symmetry breaking via alloy disorder to explain radiative Auger transitions in self-assembled quantum dots

On the prospect of identifying visible emissions from optical measurements of self-assembled QDs

The work presented here focuses on the optical properties of molecular beam epitaxy-grown self-organized InAs quantum dots (QDs). Under low excitation power densities, the photoluminescence (PL) spectrum of the structure under study exhibits a double-peak profile, which has been related to the optical emission from the dots. To properly argue for or against explaining a high energy peak as being the result of different-sized QDs or excited state emissions, a comparative study of the optical properties of a set of two grown QD samples was employed. The laser power dependence of the linearity of the PL intensities of the QD transitions was shown to be very useful in determining the possible origins of the PL sub-bands detectable in a double-peak emission from an ensemble of self-organized QDs. Indeed, the change in the linearity of the dot-luminescence intensity with the increase of the excitation density could give helpful information about the active confinement states from which the dots are emitting. On the other hand, despite the use of very low excitation power densities, the optical measurements of the studied structure have revealed an appearance of a PL signal relating to the radiative emission from the first excited state of the dots. A random pathway of carrier capture by the intrinsic levels of the QDs is thought to be the most likely cause of this aspect.

Controllable Black-to-Yellow Phase Transition by Tuning the Lattice Symmetry in Perovskite Quantum Dots.

The black-to-yellow phase transition in perovskite quantum dots (QDs) is more complex than in bulk perovskites, regarding the role of surface energy. Here, with the assistance of in situ grazing-incidence wide-angle and small-angle X-ray scattering (GIWAXS/GISAXS), distinct phase behaviors of cesium lead iodide(CsPbI3 ) QDfilms under two different temperature profiles-instant heating-up (IHU) and slow heating-up (SHU) is investigated. The IHU process can cause the phase transition from black phase to yellow phase, while under the SHU process, the majority remains in black phase. Detailed studies and structural refinement analysis reveal that the phase transition is triggered by the removal of surface ligands, which switches the energy landscape. The lattice symmetry determines the transition rate and the coexistence black-to-yellow phase ratio. The SHU process allows longer relaxation time for a more ordered QD packing, which helps sustain the lattice symmetry and stabilizes the black phase. Therefore, one can use the lattice symmetry as a general index to monitor the CsPbI3 QD phase transition and finetune the coexistence black-to-yellow phase ratio for niche applications.

Quantum dot transition rate modifying by coupling to lattice plasmon

Quantum dot transition rate modifying by coupling to lattice plasmon

Two-state lasing in a quantum dot racetrack microlaser.

The peculiarities of two-state lasing in a racetrack microlaser with an InAs/GaAs quantum dot active region are investigated by measuring the electroluminescence spectra at various injection currents and temperatures. Unlike edge-emitting and microdisk lasers, where two-state lasing involves the ground and first excited-state optical transitions of quantum dots, in racetrack microlasers, we observe lasing through the ground and second excited states. As a result, the spectral separation between lasing bands is doubled to more than 150 nm. A temperature dependence of threshold currents for lasing via ground and second excited states of quantum dots was also obtained.

Photoreduced graphene oxide recovers graphene hot electron cooling dynamics

Reduced graphene oxide (rGO) is a bulk-processable quasi-amorphous 2D material with broad spectral coverage and fast electronic response. rGO sheets are suspended in a polymer matrix and sequentially photoreduced while measuring the evolving optical spectra and ultrafast electron relaxation dynamics. Photoreduced rGO yields optical absorption spectra that fit with the same Fano lineshape parameters as monolayer graphene. With increasing photoreduction time, rGO transient absorption kinetics accelerate monotonically, reaching an optimal point that matches the hot electron cooling in graphene. All stages of rGO ultrafast kinetics are simulated with a hot-electron cooling model mediated by disorder-assisted supercollisions. While the rGO room temperature 0.31 ps$^{-1}$ electronic cooling rate matches monolayer graphene, subsequent photoreduction can rapidly increase the rate by ~10-12$\times$. Such accelerated supercollision rates imply a reduced mean-free scattering length caused by photoionized point-defects on the rGO sp$^2$ sub-lattice. For visible range excitations of rGO, photoreduction shows three increasing spectral peaks that match graphene quantum dot (GQD) transitions, while a broad peak from oxygenated defect edge states shrinks. These three confined GQD states donate their hot carriers to the graphene sub-lattice with a 0.17 ps rise-time that accelerates with photoreduction. Collectively, many desirable photophysical properties of 2D graphene are replicated through selectively reducing rGO scaffolded within a 3D bulk polymeric network.

Distributed Bragg Reflector–Mediated Excitation of InAs/InP Quantum Dots Emitting in the Telecom C‐Band

Herein, it is demonstrated that optical excitation of InAs quantum dots (QDs) embedded directly in an InP matrix can be mediated via states in a quaternary compound constituting an InP/InGaAlAs bottom distributed Bragg reflector (DBR) and native defects in the InP matrix. It does not only change the carrier relaxation in the structure but could also lead to the imbalanced occupation of QDs with charge carriers, because the band structure favors the transfer of holes. Thermal activation of carrier transfer can be observed as an increase in the emission intensity versus temperature for excitation powers below saturation on the level of both an inhomogeneously broadened QD ensemble and single QD transitions. That increase in the QD emission is accompanied by a decrease in the emission from the InGaAlAs layer at low temperatures. Finally, carrier transfer between the InGaAlAs layer of the DBR and the InAs/InP QDs is directly proven by the photoluminescence excitation spectrum of the QD ensemble. The reported carrier transfer can increase the relaxation time of carriers into the QDs and thus be detrimental to the coherence properties of single and entangled photons. It is important to take it into account while designing QD‐based devices.

Narrow homogeneous linewidths and slow cooling dynamics across infrared intra-band transitions in n-doped HgSe colloidal quantum dots.

Intra-band transitions in colloidal quantum dots (QDs) are promising for opto-electronic applications in the mid-IR spectral region. However, such intra-band transitions are typically very broad and spectrally overlapping, making the study of individual excited states and their ultrafast dynamics very challenging. Here, we present the first full spectrum two-dimensional continuum infrared (2D CIR) spectroscopy study of intrinsically n-doped HgSe QDs, which exhibit mid-infrared intra-band transitions in their ground state. The obtained 2D CIR spectra reveal that underneath the broad absorption line shape of ∼500cm-1, the transitions exhibit surprisingly narrow intrinsic linewidths with a homogeneous broadening of 175-250cm-1. Furthermore, the 2D IR spectra are remarkably invariant, with no signof spectral diffusion dynamics at waiting times up to 50ps. Accordingly, we attribute the large static inhomogeneous broadening to the distribution of size and doping level of the QDs. In addition, the two higher-lying P-states of the QDs can be clearly identified in the 2D IR spectra along the diagonal with a cross-peak. However, there is no indication of cross-peak dynamics indicating that, despite the strong spin-orbit coupling in HgSe, transitions between the P-states must be longer than our maximum waiting time of 50ps. This study illustrates a new frontier of 2D IR spectroscopy enabling the study of intra-band carrier dynamics in nanocrystalline materials across the entire mid-infrared spectrum.

Two-State Lasing in Microdisk Laser Diodes with Quantum Dot Active Region

The two-state lasing phenomenon, which manifests itself in simultaneous laser emission through several optical transitions of quantum dots, is studied in microdisk diode lasers with different cavity diameters. The active region represents a multiply stacked array of self-organized InAs/InGaAs/GaAs quantum dots emitting in the wavelength range of 1.1–1.3 µm. Two-state lasing, which involves the ground-state and the first excited-state optical transitions, is observed in microdisks with cavity diameters of 20 to 28 µm, whereas two-state lasing via the first and the second excited-state optical transitions is observed in 9 µm microdisks. The threshold currents for one-state and two-state lasing are investigated as functions of the microdisk diameter. Optical loss in the microdisk lasers is evaluated by comparing the two-state lasing behavior of the microdisks with that of edge-emitting stripe lasers made of the same epitaxial wafer.

External Field‐induced Transitions in Quantum Dot: Role of Noise‐anharmonicity Interplay

AbstractThis work scrutinizes the time‐average excitation rate (TAER) among the GaAs quantum dot (QD) eigenstates under the aegis of Gaussian white noise (GWN) and the parity of the anharmonic potential (odd/even). GWN connects with the system by additive or multiplicative mode. The said excitation of the ground state population has been triggered by an external field which may be a polychromatic radiation field (PRF), or pulsed field (PF) or chirped pulsed field (CPF). The study reveals the subtle nuances of the interplay between noise (additive or multiplicative), anharmonicity (odd or even) and the external field (PRF, PF or CPF) that finally govern the attributes of the TAER diagrams. The TAER profiles exhibit persistent growth, persistent decline, maximization (important in view of production of prominent nonlinear optical properties), minimization and saturation (relevant to the dynamic freezing). The findings appear useful for regulating the TAER among the GaAs QD eigenstates which have substantial technological relevance.

Ultra-high-precision detection of single microwave photons based on a hybrid system between a Majorana zero mode and a quantum dot

The ability to detect single photons has become increasingly essential due to the rise of photon-based quantum computing. In this theoretical work, we propose a system consisting of a quantum dot (QD) side-coupled to a superconducting nanowire. The coupling opens a gap in both the QD mode and the Majorana zero mode (MZM) at the nanowire edge, enabling photon absorption in the system. We show that the absorbed photoelectron decays via rapid (subnanosecond to nanosecond) nonradiative heat transfer to the nanowire phonon modes rather than by spontaneous emission. Furthermore, we calculate the temperature increase and associated resistance increase induced by the absorption of a photon for a given appropriate set of material and environmental parameters, yielding a temperature increase in the millikelvin range and a resistance increase in the kiloohm range, vastly exceeding the photon-absorption-induced temperature and resistance increases for competing 2D-3D hybrid systems by 5 and 9 orders of magnitude, respectively. Last, we determine the detector efficiency and discuss the system density required for deterministic photon number measurement, demonstrating that a photon absorption probability of over 99.9 percent can be achieved for an integrated system consisting of an array of nanowire-QD complexes on-chip inside a cavity. Our results thus provide a basis for a deterministic microwave photon number detector with an unprecedented photon-number-detection resolution.

Edge States and Strain-Driven Topological Phase Transitions in Quantum Dots in Topological Insulators.

We present here a theory of the electronic properties of quasi two-dimensional quantum dots made of topological insulators. The topological insulator is described by either eight band k→·p→ Hamiltonian or by a four-band k→·p→ Bernevig-Hughes-Zhang (BHZ) Hamiltonian. The trivial versus topological properties of the BHZ Hamiltonian are characterized by the different topologies that arise when mapping the in-plane wavevectors through the BHZ Hamiltonian onto a Bloch sphere. In the topologically nontrivial case, edge states are formed in the disc and square geometries of the quantum dot. We account for the effects of compressive strain in topological insulator quantum dots by means of the Bir-Pikus Hamiltonian. Tuning strain allows topological phase transitions between topological and trivial phases, which results in the vanishing of edge states from the energy gap. This may enable the design of a quantum strain sensor based on strain-driven transitions in HgTe topological insulator square quantum dots.