We present a method of obtaining information about spin lifetimes in quantum dots from measurements of electrical transport. The dot is under resonant microwave irradiation and at temperatures comparable to or larger than the Zeeman energy. We find that the ratio of the spin coherence times T_{1}/T_{2} can be deduced from a measurement of current through the quantum dot as a function the applied magnetic field. We calculate the noise power spectrum of the dot current and show that a dip occurs at the Rabi frequency with a line width given by 1/T_{1}+1/T_{2}.
The self-assembled quantum dots (QDs) provide an ideal platform for realization of quantum information technology because it provides on demand single photons, entangled photon pairs from biexciton cascade pro- cess, single spin qubits, and so on. The fine structure splitting (FSS) of exciton is a fundamental property of QDs for thees applications. From the symmetry point of view, since the two bright exciton states belong to two different representations for QDs with C2v symmetry, they should not only have different energies, but also have different lifetimes, which is termed exciton lifetime…
We demonstrate the ability to control the spontaneous emission dynamics of self-assembled quantum dots via the local density of optical modes in 2D-photonic crystals. We show that an incomplete 2D photonic bandgap is sufficient to significantly lengthen the spontaneous emission lifetime ($>2\times$) over a wide bandwidth ($Δλ\geq40$ nm). For dots that are both \textit{spectrally} and \textit{spatially} coupled to strongly localized ($V_{mode}\sim1.5(λ/n)^{3}$), high $Q\sim2700$ optical modes, we have directly measured a strong Purcell enhanced shortening of the emission lifetime $\geq5.6\times…
Spin relaxation of electrons doped in InP quantum dots was studied by means of luminescence pump-probe and Hanle measurements. Optical pumping makes spins of doped electrons to be oriented in parallel to the helicity of the circularly polarized excitation. The luminescence pump-probe showed the spin orientation of the doped electrons decay on a millisecond time-scale. Hanle measurement clarified the spin dephasing relaxation time of doped electrons is 1.7 ns which is explained by the frozen fluctuation of nuclear spins.
Interfacing single emitters and photonic nanostructures enables modifying their emission properties, such as enhancing individual decay rates or controlling the emission direction. To achieve full control, the single emitter must be positioned in the nanostructures deterministically. Here, we use spectroscopy to gain spectral and spatial information about individual quantum dots in order to position each emitter in a pre-determined location in a unit cell of a photonic-crystal waveguide. Depending on the spatial and spectral positioning within the structured nanophotonic mode, we observe that …
We have observed the Zeeman-split excited state of a spin-1/2 multi-electron Si/SiGe depletion quantum dot and measured its spin relaxation time T1 in magnetic fields up to 2 T. Using a new step-and-reach technique, we have experimentally verified the g-value of 2.0 +/- 0.1 for the observed Zeeman doublet. We have also measured T1 of single- and multi-electron spins in InGaAs quantum dots. The lifetimes of the Si/SiGe system are appreciably longer than those for InGaAs dots for comparable magnetic field strengths, but both approach one second at sufficiently low fields (< 1 T for Si, and < 0.2…
Having already achieved near-unity quantum yields, with promising properties for light-emitting diode, lasing, and charge separation applications, colloidal core/shell quantum dots have great technological potential. The shell thickness and band alignment of the shell and core materials are known to influence the efficiency of these devices. In many such applications, a key to improving the efficiency requires a deep understanding of multiexcitonic states. Herein, we elucidate the shell thickness and band alignment dependencies of the biexciton Auger recombination lifetime for quasi-type-II Cd…
We present studies on Coulomb interactions in single self-assembled CdTe quantum dots. We use a field effect structure to tune the charge state of the dot and investigate the impact of the charge state on carrier wave functions. The analysis of the quantum confined Stark shifts of four excitonic complexes allows us to conclude that the hole wave function is softer than electron wave function, i. e. it is subject to stronger modifications upon changing of the dot charge state. These conclusions are corroborated by time-resolved photoluminescence studies of recombination lifetimes of different e…
Quantum dots are both excellent single-photon sources and hosts for single spins. This combination enables the deterministic generation of Raman-photons -- bandwidth-matched to an atomic quantum-memory -- and the generation of photon cluster states, a resource in quantum communication and measurement-based quantum computing. GaAs quantum dots in AlGaAs can be matched in frequency to a rubidium-based photon memory, and have potentially improved electron spin coherence compared to the widely used InGaAs quantum dots. However, their charge stability and optical linewidths are typically much worse…
We calculate the lifetime of low-energy electronic excitations in a two-dimensional quantum dot near a metallic gate. We find different behaviors depending on the relative values of the dot size, the dot-gate distance and the Thomas-Fermi screening length within the dot. The standard Fermi liquid behavior is obtained when the dot-gate distance is much shorter than the dot size or when it is so large that intrinsic effects dominate. Departures from the Fermi liquid behavior are found in the unscreened dipole case of small dots far away from the gate, for which a Caldeira-Leggett model is applic…
The decay rate of quasiparticles in quantum dots is studied through the real time calculation of the single-particle Green function in the self-consistent approximation. The method avoids exact diagonalization, transforming the problem into a system of coupled non-linear integral equations which may be solved iteratively. That allows us to study systems larger than previously treated in the literature. Our results for the inverse participation ratio of many-body states show that the threshold energy for the quasiparticle disintegration is $E^\ast \sim \sqrt{g} Δ$. The delocalization transition…
The dynamics of exciton recombination in an ensemble of indirect band-gap (In,Al)As/AlAs quantum dots with type-I band alignment is studied. The lifetime of confined excitons which are indirect in momentum-space is mainly influenced by the sharpness of the heterointerface between the (In,Al)As quantum dot and the AlAs barrier matrix. Time-resolved photoluminescence experiments and theoretical model calculations reveal a strong dependence of the exciton lifetime on the thickness of the interface diffusion layer. The lifetime of excitons with a particular optical transition energy varies because…
In this work the intersubband electronic properties of two laterally coupled dome-shaped InAs/GaAs quantum dots were investigated. The envelope functions and eigenenergies were calculated as function of distance between the dots. The coupling between the dots was studied using transition lifetime between the dots. The results showed that in close distances (smaller than 3 nm) the quantum dots are coupled and by increasing the distance transition lifetime fall down drastically and the dots become uncoupled.
We propose the concept of valley coherence and superradiance in the reciprocal space and show that it leads to an $N$-fold decrease of the bright exciton radiative lifetime in quantum dots (QDs) of an $N$-valley semiconductor. Next we explain why, despite this, the exciton radiative lifetimes in PbX (X = S, Se, Te) QDs, measured from the photoluminescence decay, are in the microsecond range. We also address peculiarities of the light-matter interaction in nanostructures made of narrow-gap materials with strong inter-band coupling.
The exciton lifetimes $T_1$ in arrays of InAs/GaAs vertically coupled quantum dot pairs have been measured by time-resolved photoluminescence. A considerable reduction of $T_1$ by up to a factor of $\sim$ 2 has been observed as compared to a quantum dots reference, reflecting the inter-dot coherence. Increase of the molecular coupling strength leads to a systematic decrease of $T_1$ with decreasing barrier width, as for wide barriers a fraction of structures shows reduced coupling while for narrow barriers all molecules appear to be well coupled. The coherent excitons in the molecules gain the…
Using a combination of continuous wave and time-resolved spectroscopy, we study the effects of interfacial conditions on the radiative lifetimes and photoluminescence intensities of colloidal CdTe/CdS quantum dots (QDs) embedded in a three-dimensional nanostructured silicon (NSi) matrix. The NSi matrix was thermally oxidized under different conditions to change the interfacial oxide thickness. QDs embedded in a NSi matrix with ~0.5 nm of interfacial oxide exhibited reduced photoluminescence intensity and nearly five times shorter radiative lifetimes (~16 ns) compared to QDs immobilized within …
We study theoretically nonradiative and radiative energy transfer between two localized quantum emitters, donor one (i.e. initially excited) and acceptor one (i.e. receiving the excitation). The rates of nonradiative and radiative processes are calculated depending on the spatial and spectral separation between donor and acceptor states and for different donor and acceptor lifetimes for typical parameters of semiconductor quantum dots. We find that the donor lifetime can be significantly modified only due to the nonradiative Förster energy transfer process at donor-acceptor separations $\sim 1…
We calculate the lifetime of conduction band excited states in self-assembled quantum dots by taking into account LO-phonon-electron interaction and various anharmonic phonon couplings. We show that polaron relaxation cannot be accurately described by a semi-classical model. The contributions of different anharmonic decay channels are shown to depend strongly on the polaron energy. We calculate the energy dependence of polaron lifetime and compare our results to available experimental measurements of polaron decay time in InAs/GaAs quantum dots.
In semiconductors, photoexcited electrons and holes (carriers) initially occupy high-energy states, but quickly lose energy to phonons and relax to the band edge within a picosecond [1]. Increasing the lifetime of carriers in light-absorbing materials is necessary to improve open-circuit voltage in photovoltaics [2], charge separation in organic solar cells [3], and charge transfer in photodetection de vices [4]. Here we demonstrate long lifetimes over one hundred picoseconds for electron-hole pairs in graphene quantum dots (GQDs) due to large transition energies and weak coupling to excitonic…
The valley degree of freedom presents challenges and opportunities for silicon spin qubits. An important consideration for singlet-triplet states is the presence of two distinct triplets, comprised of valley vs. orbital excitations. Here we show that both of these triplets are present in the typical operating regime, but that only the valley-excited triplet offers intrinsic protection against charge noise. We further show that this protection arises naturally in dots with stronger confinement. These results reveal an inherent advantage for silicon-based multi-electron qubits.
We construct an optimal set of single-particle states for few-electron quantum dots (QDs) using the method of natural orbitals (NOs). The NOs include also the effects of the Coulomb repulsion between electrons. We find that they agree well with the noniteracting orbitals for GaAs QDs of realistic parameters, while the Coulomb interactions only rescale the radius of the NOs compared to the noninteracting case. We use NOs to show that four-electron QDs are less susceptible to charge noise than their two-electron counterparts.
We analyze the decoherence of charge states in double quantum dots due to cotunneling. The system is treated using the Bloch-Redfield generalized master equation for the Schrieffer-Wolff transformed Hamiltonian. We show that the decoherence, characterized through a relaxation $τ_{r}$ and a dephasing time $τ_ϕ$, can be controlled through the external voltage and that the optimum point, where these times are maximum, is not necessarily in equilibrium. We outline the mechanism of this nonequilibrium-induced enhancement of lifetime and coherence. We discuss the relevance of our results for recent …
Single and multi-band (Burt-Foreman) k.p Hamiltonians for GaAs crystal phase quantum dots are developed and used to assess ongoing experimental activity on the role of such factors as quantum confinement, spontaneous polarization, valence band mixing and exciton Coulomb interaction. Spontaneous polarization is found to be a dominating term. Together with the control of dot thickness [Vainorious Nano Lett. 15, 2652 (2015)] it enables wide exciton wavelength and lifetime tunability. Several new phenomena are predicted for small diameter dots [Loitsch et al. Adv. Mater. 27, 2195 (2015)], includin…
We investigate charge relaxation rates due to acoustic phonons in weakly-confined quantum dot systems, including both deformation potential and piezoelectric field interactions. Single-electron excited states lifetimes are calculated for single and coupled quantum dot structures, both in homonuclear and heteronuclear devices. Piezoelectric field scattering is shown to be the dominant relaxation mechanism in many experimentally relevant situations. On the other hand, we show that appropriate structure design allows to minimize separately deformation potential and piezolectric field interactions…
Quantum dots (QDs) investigated through electron transport measurements often exhibit varying, state-dependent tunnel couplings to the leads. Under specific conditions, weakly coupled states can result in a strong suppression of the electrical current and they are correspondingly called blocking states. Using the combination of conductance and shot noise measurements, we investigate blocking states in carbon nanotube (CNT) QDs. We report negative differential conductance and super-Poissonian noise. The enhanced noise is the signature of electron bunching, which originates from random switches …
We investigate the magnetic field and temperature dependence of the single-electron spin lifetime in silicon quantum dots and find a lifetime of 2.8 ms at a temperature of 1.1 K. We develop a model based on spin-valley mixing and find that Johnson noise and two-phonon processes limit relaxation at low and high temperature respectively. We also investigate the effect of temperature on charge noise and find a linear dependence up to 4 K. These results contribute to the understanding of relaxation in silicon quantum dots and are promising for qubit operation at elevated temperatures.
We present measurements on gate-defined double quantum dots in Ge-Si core-shell nanowires, which we tune to a regime with visible shell filling in both dots. We observe a Pauli spin blockade and can assign the measured leakage current at low magnetic fields to spin-flip cotunneling, for which we measure a strong anisotropy related to an anisotropic g-factor. At higher magnetic fields we see signatures for leakage current caused by spin-orbit coupling between (1,1)-singlet and (2,0)-triplet states. Taking into account these anisotropic spin-flip mechanisms, we can choose the magnetic field dire…
Previous studies have shown that positron-annihilation spectroscopy is a highly sensitive probe of the electronic structure and surface composition of ligand-capped semiconductor Quantum Dots (QDs) embedded in thin films. Nature of the associated positron state, however, whether the positron is confined inside the QDs or localized at their surfaces, has so far remained unresolved. Our positron-annihilation lifetime spectroscopy (PALS) studies of CdSe QDs reveal the presence of a strong lifetime component in the narrow range of 358-371 ps, indicating abundant trapping and annihilation of positr…
We have investigated the noise properties of the tunneling current through vertically coupled self-assembled InAs quantum dots. We observe super-Poissonian shot noise at low temperatures. For increased temperature this effect is suppressed. The super-Poissonian noise is explained by capacitive coupling between different stacks of quantum dots.
Probing charge noise in bilayer graphene quantum dots by Landau-Zener-Stückelberg-Majorana spectroscopy
RWTH Aachen University（亚琛工业大学）；JARA-FIT；nd Institute of Physics, RWTH Aachen University（亚琛工业大学第二物理研究所）；Peter Grünberg Institute (PGI-9), Forschungszentrum Jülich（于利希研究中心彼得·格林伯格研究所（PGI-9））；Forschungszentrum Jülich（于利希研究中心）；CST - Compound Semiconductor Technology, RWTH Aachen University（亚琛工业大学化合物半导体技术）；University of Vienna, Faculty of Physics（维也纳大学物理系）；National Institute for Materials Science（国立材料研究所）
Electron spins in silicon quantum dots are promising qubits due to their long coherence times, scalable fabrication, and potential for all-electrical control. However, charge noise in the host semiconductor presents a major obstacle to achieving high-fidelity single- and two-qubit gates in these devices. In this work, we measure the charge-noise spectrum of a Si/SiGe singlet-triplet qubit over nearly 12 decades in frequency using a combination of methods, including dynamically-decoupled exchange oscillations with up to 512 π pulses during the qubit evolution. The charge noise is colored across…
Luminescence properties of colloidal quantum dots have found applications in imaging, light-sources, and displays. Despite wide interest, several experimental observations from these quantum dots, such as the short lifetime on the scale of microseconds and a zero-longitudinal optical phonon line in low-temperature photoluminescence spectrum, remain unexplained by existing models. Here we propose a model including the effect of solid-state environment on luminescence by capturing coherent and incoherent interactions of band-edge exciton with phonon modes. Our model predicts the formation of dre…
We use a configuration-interaction approach and Fermi golden rule to investigate electron-phonon interaction in realistic multi-electron quantum dots. Lifetimes are computed in the low-density, highly correlated regime. We report numerical evidence that electron-electron interaction generally leads to reduced decay rates of excited electronic states in weakly confined quantum dots, where carrier relaxation is dominated by the interaction with longitudinal acoustic phonons.
It has been recently demonstrated that a singlet-triplet spin qubit in semiconductor double quantum dots can be controlled by changing the height of the potential barrier between the two dots ("barrier control"), which has led to a considerable reduction of charge noises as compared to the traditional tilt control method. In this paper we show, through a molecular-orbital-theoretic calculation of double quantum dots influenced by a charged impurity, that the relative charge noise for a system under the barrier control not only is smaller than that for the tilt control, but actually decreases a…
We report both zinc-blende (ZB) and wurtzite (WZ) crystal phase self-assembled GaAs quantum dots (QDs) embedding in a single GaAs/AlGaAs core-shell nanowires (NWs). Optical transitions and single-photon characteristics of both kinds of QDs have been investigated by measuring photoluminescence (PL) and time-resolved PL spectra upon application of hydrostatic pressure. We find that the ZB QDs are of direct band gap transition with short recombination lifetime (~1 ns) and higher pressure coefficient (75-100 meV/GPa). On the contrary, the WZ QDs undergo a direct-to-pseudodirect bandgap transition …
Hole spin qubits are frontrunner platforms for scalable quantum computers, but state-of-the-art devices suffer from noise originating from the hyperfine interactions with nuclear defects. We show that these interactions have a highly tunable anisotropy that is controlled by device design and external electric fields. This tunability enables sweet spots where the hyperfine noise is suppressed by an order of magnitude and is comparable to isotopically purified materials. We identify surprisingly simple designs where the qubits are highly coherent and are largely unaffected by both charge and hyp…
Single photon emission was observed from site-controlled InGaN/GaN quantum dots. The single-photon nature of the emission was verified by the second-order correlation function up to 90 K, the highest temperature to date for site-controlled quantum dots. Micro-photoluminescence study on individual quantum dots showed linearly polarized single exciton emission with a lifetime of a few nanoseconds. The dimensions of these quantum dots were well controlled to the precision of state-of-the-art fabrication technologies, as reflected in the uniformity of their optical properties. The yield of optical…
We investigate the noise properties of a GaAs-AlAs-GaAs tunneling structure with embedded self-assembled InAs quantum dots in the single-electron tunneling regime. We analyze the dependence of the relative noise amplitude of the shot noise on bias voltage. We observe a non-monotonic behaviour of the Fano-factor $α$ with an average value of $α\approx 0.8$ consistent with the asymmetry of the tunneling barriers. Reproducible fluctuations observed in $α$ can be attributed to the successive participation of more and more InAs quantum dots in the tunneling current.
The dephasing time of the lowest bright exciton in CdSe/ZnS wurtzite quantum dots is measured from 5 K to 170 K and compared with density dynamics within the exciton fine structure using a sensitive three-beam four-wave-mixing technique unaffected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing of 109 ps at 5 K, much faster than the ~10 ns exciton radiative lifetime. The zero-phonon line dephasing is explained by phonon-assisted spin-flip from the lowest bright state to dark exciton states. This is…
The emission properties of single quantum dots in planar microcavities are studied experimentally and theoretically. Fivefold Enhanced spontaneous emission outside the microcavity is found for dots in resonance with the cavity mode, relative to detuned dots, while their radiative lifetime is only marginally decreased. Using high power excitation we obtain the in-plane cavity dispersion. Near field images of the emission show spatial distributions of several microns for resonant dots, which decrease in size with the detuning from resonance. These experimental findings are explained using a simp…
We study the relaxation of the exciton spin (longitudinal relaxation time $T_{1}$) in single asymmetrical quantum dots due to an interplay of the short--range exchange interaction and acoustic phonon deformation. The calculated relaxation rates are found to depend strongly on the dot size, magnetic field and temperature. For typical quantum dots and temperatures below 100 K, the zero--magnetic field relaxation times are long compared to the exciton lifetime, yet they are strongly reduced in high magnetic fields. We discuss explicitly quantum dots based on (In,Ga)As and (Cd,Zn)Se semiconductor …
Models of the spontaneous emission of photons coupled to the electronic states of quantum dots are important for understanding quantum interactions in dielectric media as applied to proposed solid-state quantum computers, single photon emitters, and single photon detectors. The characteristic lifetime of photon emission is traditionally modeled in the Weisskopf-Wigner approximation. Here we model the fully quantized spontaneous emission, including near field effects, of a photon from the excited state of a quantum dot beyond theWeisskopf-Wigner approximation. We propose the use of discretized …
Quantum dots play a promising role in the development of novel optical and biosensing devices. In this study, we investigated steady-state and time-dependent luminescence properties of InGaP/ZnS core/shell colloidal quantum dots in a solution phase at room temperature. The steady state experiments exhibited an emission maximum at 650 nm with full width at half maximum of ~ 85 nm, and strong first-excitonic absorption peak at 600 nm. The time-resolved luminescence measurements depicted a bi-exponential decay profile with lifetimes of τ1\sim 47 ns and τ 2\sim 142 ns at the emission maximum. Addi…
In this work we present a detailed analysis of the second-order piezoelectric effect in $c$-plane In$_{x}$Ga$_{1-x}$N/GaN quantum dots and its consequences for electronic and optical properties of these systems. Special attention is paid to the impact of increasing In content $x$ on the results. We find that in general the second-order piezoelectric effect leads to an increase of the electrostatic built-in field. Furthermore, our results show that for an In content $\geq$30\% this increase in the built-in field has a significant effect on the emission wavelength and the radiative lifetimes. Fo…
Controlled adiabatic transfer of a single electron through a chain of quantum dots has been recently achieved in GaAs and Si/SiGe based quantum dots, opening prospects for turning stationary spin qubits into mobile ones, and solving in this way the problem of long-distance communication between quantum registers in a scalable quantum computing architecture based on quantum dots. We consider theoretically the process of such an electron transfer between two tunnel-coupled quantum dots, focusing on control by slowly varying the detuning of energy levels in the dots. We take into account the fluc…
We investigate shot noise for quantum dots whose classical phase space consists of both regular and chaotic regions. The noise is systematically suppressed below the universal value of fully chaotic systems, by an amount which varies with the positions of the leads. We analyze the dynamical origin of this effect by a novel way to incorporate diffractive impurity scattering. The dependence of the shot noise on the scattering rate shows that the suppression arises due to the deterministic nature of transport through regular regions and along short chaotic trajectories. Shot noise can be used to …
PbS quantum dots are promising active emitters for use with high-quality Si nanophotonic devices in the telecommunications-band. Measurements of low quantum dot densities are limited both because of low fluorescence levels and the challenges of single photon detection at these wavelengths. Here, we report on methods using a fiber taper waveguide to efficiently extract PbS quantum dot photoluminescence. Temperature dependent ensemble measurements reveal an increase in emitted photons concomitant with an increase in excited-state lifetime from 58.9 ns at 293 K to 657 ns at 40 K. Measurements are…
We show how to realize a quantum interface between optical fields and the polarized nuclear spins in a singly charged quantum dot, which is strongly coupled to a high-finesse optical cavity. An effective direct coupling between cavity and nuclear spins is obtained by adiabatically eliminating the (far detuned) excitonic and electronic states. The requirements needed to map qubit and continuous variable states of cavity or traveling-wave fields to the collective nuclear spin are investigated: For cavity fields, we consider adiabatic passage processes to transfer the states. It is seen that a si…
We investigate gate voltage dependence of electrical readout noise in high-speed rf reflectometry using gallium arsenide quantum dots. The fast Fourier transform spectrum from the real time measurement reflects build-in device noise and circuit noise including the resonator and the amplifier. We separate their noise spectral components by model analysis. Detail of gate voltage dependence of the flicker noise is investigated and compared to the charge sensor sensitivity. We point out that the dominant component of the readout noise changes by the measurement integration time.
We study shot noise for generic quantum dots coupled to two leads and allow for an arbitrary strength of diffractive impurity scattering inside the dots. The ballistic quantum dots possess a mixed classical phase space, where regular and chaotic regions coexist. In absence of disorder, the noise is systematically suppressed below the universal value of fully chaotic systems, by an amount which varies with the positions of the leads. This suppression is due to the deterministic nature of transport through regular regions and along short chaotic trajectories, and disappears by increasing the sca…
We show that the intriguing observation of noise enhancement in the charge transport through two vertically coupled quantum dots can be explained by the interplay of quantum coherence and strong Coulomb blockade. We demonstrate that this novel mechanism for super-Poissonian charge transfer is very sensitive to decoherence caused by electron-phonon scattering as inferred from the measured temperature dependence.
We investigate shot noise of photon-excited electron-hole pairs in open multi-terminal, multi-channel chaotic dots. Coulomb interactions in the dot are treated self-consistently giving a gauge-invariant expression for the finite frequency correlations. The Coulomb interactions decrease the noise, the strong interaction limit coincides with the non-interacting adiabatic limit. Inelastic scattering and dephasing in the dot are described by voltage and dephasing probe models respectively. We find that dephasing leaves the noise invariant, but inelastic scattering decreases correlations eventually…
