Tuning spin properties of excitons in single CdTe quantum dots by annealing

Using polarization-resolved photoluminescence imaging in external magnetic fields we measure statistically significant distributions of exchange splitting, diamagnetic shift and effective g-factor of excitons in tens of single CdTe quantum dots. Comparison between the as-grown and annealed structures shows strong suppression of ensemble inhomogeneities, with the average exchange splitting reduced by half and significant narrowing of the g-factor distribution. Remarkably, the average value of the excitonic g-factor remains unchanged. This unique ability to yield highly uniform quantum dot ensembles without hampering the exciton Zeeman splitting makes annealing a highly attractive means for tuning the spin properties of quantum dot excitons.     

Electron eigenstates in quantum dots revealed by temperature derivative capacitance spectroscopy

A novel method is presented for detecting confined energy states in quantum dots embedded in a junction space charge region, where the reverse bias is used to discharge the initially occupied energy levels. By determining the temperature derivative of junction capacitance as a function of bias voltage and temperature, spectra are obtained with peaks revealing the existence of electron states in InGaAs/GaAs quantum dots structure grown by molecular beam epitaxy. The method is compared with admittance based techniques and theory used earlier for interpretation of experimental data.     

Synthesis and photoluminescence of ZnS quantum dots

Single-phase zinc sulphide (ZnS) quantum dots were synthesized by a chemical method. The influence of the pH value of the Zn(CH3COO)2 solution on the size and photoluminescence properties of the ZnS quantum dots was evaluated. X-ray power diffraction, transmission electron microscopy, and ultraviolet-visible spectroscopy were used to characterize the structure, size, surface states, and photoluminescence properties of ZnS quantum dots. The results showed that the crystal structure of ZnS quantum dots was a cubic zinc blende structure, and their average diameter was about 3.0 nm. ZnS quantum dots with good distribution and high purity were obtained. A strong broad band centered at about 320 nm was observed in the excitation spectrum of ZnS quantum dots. Their emission spectrum peaking at about 408 nm, was due mostly to the trap-state emission. The relative integrated emission intensity of ZnS quantum dots decreased as the pH value of the Zn(CH3COO)2 solution increased, which could be ascribed to the increase in average diameter of the ZnS quantum dots as the pH value of Zn(CH3COO)2 solution increased.     

圆偏振光诱导CdTe量子点再生长及其对光致发光的影响

实验研究了以3-巯基丙酸为配体合成的水溶性CdTe量子点经过非偏振光与圆偏振光照射处理后, 量子点的再生长变化规律。采用光致发光谱、紫外-可见吸收光谱、透射电子显微镜与X射线衍射等表征手段分析表明: 非偏振光会促进CdTe量子点的光氧化, 导致量子点尺寸缩小, 荧光发光峰位蓝移, 且发光效率降低; 而圆偏振光增强了配体的光氧化, 在量子点表面形成CdS层, 导致量子点尺寸进一步增大, 荧光发光峰红移, 且发光效率提升。进一步讨论了CdTe量子点与配体之间的键合作用, 相关光化学反应机制及其对量子点光致发光性质的影响。     

Observation of room temperature negative differential resistance in multi-layer heterostructures of quantum dots and conducting polymers

Multi-layer heterostructure negative differential resistance devices based on poly-[2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylenevinylene] (MEH-PPV) conducting polymer and CdSe quantum dots is reported. The conducting polymer MEH-PPV acts as a barrier while CdSe quantum dots form the well layer. The devices exhibit negative differential resistance (NDR) at low voltages. For these devices, strong negative differential resistance is observed at room temperature. A maximum value of 51 for the peak-to-valley ratio of current is reported. Tunneling of electrons through the discrete quantum confined states in the CdSe quantum dots is believed to be responsible for the multiple peaks observed in the I-V measurement. Depending on the observed NDR signature, operating mechanisms are explored based on resonant tunneling and Coulomb blockade effects.     

Tunable quantum dots in bilayer graphene

We demonstrate theoretically that quantum dots in bilayers of graphene can be realized. A position-dependent doping breaks the equivalence between the upper and lower layer and lifts the degeneracy of the positive and negative momentum states of the dot. Numerical results show the simultaneous presence of electron and hole confined states for certain doping profiles and a remarkable angular momentum dependence of the quantum dot spectrum, which is in sharp contrast with that for conventional semiconductor quantum dots. We predict that the optical spectrum will consist of a series of nonequidistant peaks.     

High extractive single-photon emissions from InGaAs quantum dots on a GaAs pyramid-like multifaceted structure

This work investigates the single-photon emissions from self-assembled InGaAs quantum dots that are grown on an apex plane of a GaAs pyramid-like multifaceted structure. The number of QDs on a multifaceted structure is estimated by scanning electron microscopy. Single-exciton emissions from individual quantum dots are examined by micro-photoluminescence and by making photon correlation measurements. This experiment demonstrates the improvement of the single-photon extraction efficiency as quantum dots are grown on a reduced apex plane of a multifaceted structure.     

Measure of Entanglement States of Two Interacting Electrons in Vertically Coupled Quantum Dots Induced by a Time-Dependent Electric Field

We study the dynamics of two electrons located in two vertically tunnel-coupled quantum dots in the presence of an oscillatory electric field. By solving the time-dependent Schrödinger equation, we predict the dynamical generation of entangled electron states, such as the EPR (Einstein, Podolsky, and Rosen) pairs or Bell states. The Schmidt rank and the von Neumann entropy are evaluated to characterize the degree of entanglement of the two electron states.     

Quantum oscillations in magnetically doped colloidal nanocrystals

Progress in the synthesis of colloidal quantum dots has recently provided access to entirely new forms of diluted magnetic semiconductors, some of which may find use in quantum computation. The usefulness of a spin qubit is defined by its Rabi frequency, which determines the operation time, and its coherence time, which sets the error correction window. However, the spin dynamics of magnetic impurity ions in colloidal doped quantum dots remain entirely unexplored. Here, we use pulsed electron paramagnetic resonance spectroscopy to demonstrate long spin coherence times of ～0.9 μs in colloidal ZnO quantum dots containing the paramagnetic dopant Mn(2+), as well as Rabi oscillations with frequencies ranging between 2 and 20 MHz depending on microwave power. We also observe electron spin echo envelope modulations of the Mn(2+) signal due to hyperfine coupling with protons outside the quantum dots, a situation unique to the colloidal form of quantum dots, and not observed to date.     

Electronic energy transfer between long-range resonance states of 3-mercaptopropionic acid capped CdTe quantum dots in aqueous media

We demonstrate electronic energy transfer between resonance states of 2 and 2.8?nm CdTe quantum dots in aqueous media using steady-state photoluminescence spectroscopy without using any external linker molecule. With increasing concentration of larger dots, there is subsequent quenching of luminescence in smaller dots accompanied by the enhancement of luminescence in larger dots. Our experimental evidence suggests that there is long-range resonance energy transfer among electronic excitations, specifically from the electronically confined states of the smaller dots to the higher excited states of the larger dots.     

Laterally defined freely suspended quantum dots in GaAs/AlGaAs heterostructures

Free-standing beams containing a two-dimensional electron system are shaped from a GaAs/AlGaAs heterostructure. Quantum point contacts and (double) quantum dots are laterally defined using metal top gates. We investigate the electronic properties of these nanostructures by transport spectroscopy. Tunable localized electron states in freely suspended nanostructures are a promising tool to investigate the electron-phonon interaction.     

Ultrafast spin dynamics in colloidal ZnO quantum dots

Time-resolved Faraday rotation measurements in the ultraviolet have been performed to reveal the ultrafast spin dynamics of electrons in colloidal ZnO quantum dots. Oscillating Faraday rotation signals are detected at frequencies corresponding to an effective g factor of g = 1.96. Biexponential oscillation decay is observed that is due to (i) rapid depopulation of the fundamental exciton (tau = 250 ps) and (ii) slow electron spin dephasing ( T 2 = 1.2 ns) within a metastable state formed by hole-trapping at the quantum dot surface.     

Quantitative excited state spectroscopy of a single InGaAs quantum dot molecule through multi-million-atom electronic structure calculations

Atomistic electronic structure calculations are performed to study the coherent inter-dot couplings of the electronic states in a single InGaAs quantum dot molecule. The experimentally observed excitonic spectrum by Krenner et al (2005) Phys. Rev. Lett. 94 057402 is quantitatively reproduced, and the correct energy states are identified based on a previously validated atomistic tight binding model. The extended devices are represented explicitly in space with 15-million-atom structures. An excited state spectroscopy technique is applied where the externally applied electric field is swept to probe the ladder of the electronic energy levels (electron or hole) of one quantum dot through anti-crossings with the energy levels of the other quantum dot in a two-quantum-dot molecule. This technique can be used to estimate the spatial electron-hole spacing inside the quantum dot molecule as well as to reverse engineer quantum dot geometry parameters such as the quantum dot separation. Crystal-deformation-induced piezoelectric effects have been discussed in the literature as minor perturbations lifting degeneracies of the electron excited (P and D) states, thus affecting polarization alignment of wavefunction lobes for III-V heterostructures such as single InAs/GaAs quantum dots. In contrast, this work demonstrates the crucial importance of piezoelectricity to resolve the symmetries and energies of the excited states through matching the experimentally measured spectrum in an InGaAs quantum dot molecule under the influence of an electric field. Both linear and quadratic piezoelectric effects are studied for the first time for a quantum dot molecule and demonstrated to be indeed important. The net piezoelectric contribution is found to be critical in determining the correct energy spectrum, which is in contrast to recent studies reporting vanishing net piezoelectric contributions.     

石墨烯量子点/CdS/CdSe共敏化太阳能电池

以三维锐钛矿TiO₂微球为上层光散射层材料, 以商业纳米TiO₂为下层连接材料, 采用刮刀法制备了一种新颖的双层TiO₂薄膜, 并应用于量子点敏化太阳能电池(QDSSC)。其中, 石墨烯量子点(GQDs)采用滴液法引入, CdS/CdSe量子点采用连续离子层吸附法(SILAR)制备。采用场发射扫描电镜、透射电镜、X射线衍射、紫外-可见漫反射光谱及荧光光谱对样品进行表征。实验还制备了CdS/CdSe量子点敏化及石墨烯量子点/CdS/CdSe共敏化太阳能电池, 并研究了石墨烯量子点及CdS不同敏化周期及对电池性能影响。研究结果表明, 石墨烯量子点及CdS不同敏化周期对薄膜的光学性质、电子传输及载流子复合均有较大影响。优选条件下, TiO₂/QGDs/CdS(4)/CdSe电池的光电转换效率为1.24%, 光电流密度为9.47 mA/cm², 显著高于TiO₂/CdS(4)/CdSe电池的这些参数(0.59%与6.22 mA/cm²)。这主要是由于TiO₂表层吸附石墨烯量子点后增强了电子的传输, 减少了载流子的复合。     

CdS量子点的制备和光学性质

以醋酸镉、硫粉为原料制备CdS量子点,研究了硫的加入量对其光学性质的影响,结果表明:合成的CdS量子点粒径均匀,分散性较好,随着硫加入量的增加CdS量子点的粒径增大;反应中过量的硫能有效地填补硫空位,从而抑制表面态发光,同时,ODA的修饰也能有效地钝化表面态,减小表面态的发光强度.     

A Ge/Si heterostructure nanowire-based double quantum dot with integrated charge sensor

One proposal for a solid-state-based quantum bit (qubit) is to control coupled electron spins on adjacent semiconductor quantum dots. Most experiments have focused on quantum dots made from III-V semiconductors; however, the coherence of electron spins in these materials is limited by hyperfine interactions with nuclear spins. Ge/Si core/shell nanowires seem ideally suited to overcome this limitation, because the most abundant nuclei in Ge and Si have spin zero and the nanowires can be chemically synthesized defect-free with tunable properties. Here, we present a double quantum dot based on Ge/Si nanowires in which we can completely control the coupling between the dots and to the leads. We also demonstrate that charge on the double dot can be detected by coupling it capacitively to an adjacent nanowire quantum dot. The double quantum dot and integrated charge sensor serve as an essential building block to form a solid-state qubit free of nuclear spin.     

Direct mapping of hot-electron relaxation and multiplication dynamics in PbSe quantum dots

How hot electrons relax in semiconductor quantum dots is of critical importance to many potential applications, such as solar energy conversion, light emission, and photon detection. A quantitative answer to this question has not been possible due in part to limitations of current experimental techniques in probing hot electron populations. Here we use femtosecond time-resolved two-photon photoemission spectroscopy to carry out a complete mapping in time- and energy-domains of hot electron relaxation and multiexciton generation (MEG) dynamics in lead selenide quantum dots functionalized with 1,2-ethanedithiols. We find a linear scaling law between the hot electron relaxation rate and its energy above the conduction band minimum. There is no evidence of MEG from intraband hot electron relaxation for excitation photon energy as high as three times the bandgap (3E(g)). Rather, MEG occurs in this system only from interband hot electron transitions at sufficiently high photon energies (~4E(g)).     

Crystallization behavior of silicon quantum dots in a silicon nitride matrix

Silicon quantum dot superlattice was fabricated by alternating deposition of silicon rich nitride (SRN) and Si3N4 layers using RF magnetron co-sputtering. Samples were then annealed at temperatures between 800 and 1,100 degrees C and characterized by grazing incident X-ray diffraction (GIXRD), transmission electron microscopy (TEM), Raman spectroscopy, and Fourier transform infrared spectroscopy (FTIR). GIXRD and Raman analyses show that the formation of silicon quantum dots occurs with annealing above 1,100 degrees C for at least 60 minutes. As the annealing time increased the crystallization of silicon quantum dots was also increased. TEM images clearly showed SRN/Si3N4 superlattice structure and silicon quantum dots formation in SRN layers after annealing at 1,100 degrees C for more than 60 minutes. The changes in FTIR transmission spectra observed with annealing condition corresponded to the configuration of Si-N bonds. Crystallization of silicon quantum dots in a silicon nitride matrix started stabilizing after 60 minutes' annealing and approached completion after 120 minutes'. The systematic investigation of silicon quantum dots in a silicon nitride matrix and their properties for solar cell application are presented.     

Charging and Spin Effects in Triple Dot Artificial Molecules

We have fabricated artificial molecules consisting of three coupled quantum dots defined in the two-dimensional electron gas of a GaAs/AlGaAs heterostructure using lithographically patterned gates and trenches. The three dots are arranged in a ring structure, where each dot is coupled to the other two dots. We find that, when tuned to the Coulomb blockade regime, the triple quantum dot device acts as a charge rectifier: an electron enters the third dot where it is trapped, producing a jamming effect where no other electron may enter the first dot. Triple quantum dots coupled in a ring will allow for the study of new molecular phases using artificial molecules and may also serve as building blocks of two-dimensional arrays for quantum computation.     

Electronic transient processes and optical spectra in quantum dots for quantum computing

Quantum dot systems are studied theoretically from the point of view of realization of quantum bit using the orbital state of electronic motion in a quantum dot. Attention is paid to several effects which can influence significantly the application of quantum dot electronic orbital states in quantum computing, for example, the effect of upconversion of the population and the incomplete depopulation of electronic orbital states, the effect of optical line broadening and presence of continuous background in optical spectra. Attention is also paid to the effect of upconversion of electronic population to the wetting-layer or above-barrier electronic states in quantum dot samples. Interaction of electrons with the longitudinal optical phonons is shown to play a significant role in these effects. Possible impact of these phenomena on the realization of quantum bit based on electronic orbital states in quantum dots is discussed.