SPIN-RESOLVED MAGNETO-OPTICAL STUDY OF CdSe SINGLE QUANTUM DOT

The photoluminescence correlation from a single CdSe nanocrystal under pulsed excitation is studied, and a single photon is realized at wavelength 655 nm at room temperature. The single colloidal CdSe quantum dot is prepared on a SiO2/silicon surface by a drop-and-drag technique. The long-term stability of the single-photon source is investigated; it is found that the antibunching effect weakens with excitation time, and the reason for the weakening is attributed to photobleaching. The lifetimes of photoluminescence from a single quantum dot are analyzed at different excitation times. By analyzing the probability distribution of on and off times of photoluminescence, the Auger assisted tunneling and Auger assisted photobleaching models are applied to explain the antibunching phenomenon.

Single self-assembled CdSe quantum dots (QDs) are shown to exhibit random fluctuations of the ground state emission energy as well as a spontaneous on/off blinking of the luminescence. A comparison of samples with different densities of extendend crystal defects indicates that Frenkel stacking faults are involved in the mechanism of these phenomena. We demonstrate that single emission lines originating from the same QD show a strong correlation of their transient energy shifts as well as simultaneous blinking.

Single molecule time-resolved fluorescence spectroscopy of CdSe/ZnS core-shell quantum dots (QDs) localized near a rough gold thin film demonstrates significant enhancement of multiphoton emission while at the same time showing a decrease in single photon emission. A rigorous analysis of time-resolved photon correlation spectroscopy and fluorescence lifetime data on single quantum dots at room temperature reveals an increase in radiative recombination rate of multiexcitons that is much higher than expected and, perhaps more significantly, is not correlated with concomitant increases in single exciton recombination rates. We believe that these results confirm a stronger coupling of multiexcitons to plasmon modes via a coupling to plasmon multipole modes.

Summary form only given. The excitonic optical response of single quantum dots (QD) has recently been isolated by using high spatial resolution techniques. Photoluminescence (PL) magneto-optical studies of these confined systems have shown interesting physical phenomena such as Zeeman splittings, diamagnetic shifts and the Overhauser effect. Coherent nonlinear optical spectroscopy provides a powerful additional tool for the study of the interaction between magnetic substrates, as has been demonstrated for a single quantum dot. By directly probing the quantum dot resonances under the effect of a magnetic field we can obtain information about spin relaxation times and the presence of dark states. In this paper we show the effect of a magnetic field on single quantum dot resonances (i.e. Zeeman splitting and diamagnetic shift) and report the nonlinear optical response as a function of magnetic field.

We report the optical properties of GaAs quantum dots embedded in (Al,Ga)As nanowires grown by the vapor–liquid–solid method. We used the micro-photoluminescence (PL) technique to observe PL peaks, which are assigned as exciton and biexciton emissions from single quantum dots. In addition, unusual features appear in the excitation power dependence of the energies and linewidths of the two PL peaks. The PL also depends on the optical polarization axis, indicating that the nanostructures have a highly asymmetrical shape. The results show that our method is a promising way of engineering the positions and optical properties of GaAs/(Al,Ga)As nanostructures.

In recent years interest arose into the study of transport through quantum dots. The interest is driven by two reasons. First, small devices like quantum dots and charging effects [1] In such devices open the possibility for future applications in electronics as transistors, memory cells, sensors etc. Small devices are especially interesting in high frequency applications due to their small capacitances. Although different schemes for applications have been proposed, none of it is under development or even in production and it is not clear what will be of real use in the end. The second reason for the interest into these systems is a basic physics point-of-view. These systems are extremely interesting since single quantum dots can be seen as a sort of artificial atom. In this manner-of-speaking coupled quantum dots can be called artificial molecules. These quantum dots are similar to atoms or molecules since a certain number of electrons is confined in a potential. But, in contrast to real atoms, in these artificial systems the number of electrons, the size of the system and the strength of the confinement potential can easily be changed. Therefore, in these quantum dots parameters, such as the ratio between cyclotron frequency and confinement energy or coupling strength between two quantum dots etc, can be easily varied, which is not achievable in real atoms or molecules.

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.

A system of quantum dots based on Al x In1−xAs/Al y Ga1−yAs solid solutions is investigated. The use of Al x In1−xAs wide-gap solid solutions as the basis of quantum dots substantially extends the spectral emission range to the short-wavelength region, including the wavelength region near 770 nm, which is of interest for the development of aerospace systems of quantum cryptography. The optical characteristics of Al x In1−xAs single quantum dots grown by the Stranski–Krastanov mechanism were studied by cryogenic microphotoluminescence. The statistics of the emission of single quantum dot excitons was studied using a Hanbury Brown–Twiss interferometer. The pair photon correlation function indicates the sub-Poissonian nature of the emission statistics, which directly confirms the possibility of developing single-photon emitters based on Al x In1−xAs quantum dots. The fine structure of quantum dot exciton states was investigated at wavelengths near 770 nm. The splitting of the exciton states is found to be similar to the natural width of exciton lines, which is of great interest for the development of entangled photon pair emitters based on Al x In1−xAs quantum dots.

Introduction The advanced growth of semiconductor quantum dots (QDs) with high optical quality is one key to realizing novel devices in various research disciplines related to modern semiconductor technologies. Despite recent progress in the top-down lithographic fabrication of single semiconductor QD-like emitters [43], bottom-up fabrication methods are commonly applied for the realization of high quality light emitting QDs [7]. The exploitation of high-density QD arrays as an active material in laser diodes [17] and vertical cavity surface emitting lasers (VCSEL) resulted in a new class of devices featuring lower lasing thresholds and improved device performance (such as temperature stability) in comparison to devices with higher dimensional gain [2, 3]. Spintronics and quantum information processing are intensively studied fields in order to provide complementary or entirely novel routes to a future information technology [12, 5]. Single self-assembled quantum dots (QDs) grown in low-density arrays are promising candidates for realizing functional building blocks in these research fields as they allow to confine single charge carriers or spin carriers while providing a solid-state platform capable of electrical injection or manipulation. Extensive research has resulted in the realization of various devices relying on few or single QDs, for instance quantum light emitters such as single photon sources [23, 36], sources of pairs of entangled photons [1, 45], and fewto single-QD lasers [38]. Moreover, many milestone experiments have been performed with In(Ga)As QDs grown on GaAs, for instance the observation of the Purcell effect [10] or reaching the strong QD exciton–photon coupling regime [26], demonstration of the indistinguishability of photons emitted by a QD [29], or complete control of a single spin by ultrafast optical pulses [25].

The observation of photoluminescence spectra of self-assembled single InGaAs quantum dots at room temperature was performed under weak excitation conditions using a near-field scanning optical microscope. Operation in illumination-collection mode with a highly sensitive double-tapered optical fibre probe enabled detection of weak photoluminescence signals at room temperature with high efficiency and high spatial resolution. Each single quantum dot was imaged with a spatial resolution of about 250 nm, which corresponded to a quarter of the wavelength of the photoluminescence from quantum dots. The photoluminescence yields of individual quantum dots were widely distributed and were found to decrease with photoluminescence energy. This result serves as a clue to be pursued for better understanding of the thermal excitation of the carrier from confined states in quantum dots.

We demonstrate a straightforward way to obtain single well-isolated quantum dots emitting in the visible part of the spectrum and characterize the optical emission from single quantum dots using this method. Self-assembled InP quantum dots are grown using gas-source molecular-beam epitaxy over a wide range of InP deposition rates, using an ultralow growth rate of about 0.01 atomic monolayers/s, a quantum-dot density of 1 dot/μm2 is realized. The resulting isolated InP quantum dots embedded in an InGaP matrix are individually characterized without the need for lithographical patterning and masks on the substrate. Such low-density quantum dots show excitonic emission at around 670 nm with a linewidth limited by instrument resolution. This system is applicable as a single-photon source for applications such as quantum cryptography.

A detailed understanding of the population and coherence dynamics in optically driven individual emitters in solids and their signatures in ultrafast nonlinear-optical signals is of prime importance for their applications in future quantum and optical technologies. In a combined experimental and theoretical study on exciton complexes in single semiconductor quantum dots we reveal a detailed picture of the dynamics employing three-beam polarization-resolved four-wave mixing (FWM) micro-spectroscopy. The oscillatory dynamics of the FWM signals in the exciton-biexciton system is governed by the fine-structure splitting and the biexciton binding energy in an excellent quantitative agreement between measurement and analytical description. The analysis of the excitation conditions exhibits a dependence of the dynamics on the specific choice of polarization configuration, pulse areas and temporal ordering of driving fields. The interplay between the transitions in the four-level exciton system leads to rich evolution of coherence and population. Using two-dimensional FWM spectroscopy we elucidate the exciton-biexciton coupling and identify neutral and charged exciton complexes in a single quantum dot. Our investigations thus clearly reveal that FWM spectroscopy is a powerful tool to characterize spectral and dynamical properties of single quantum structures.

Even as today’s most prominent spin-based qubit technologies are maturing in terms of capability and sophistication, there is growing interest in exploring alternate material platforms that may provide advantages, such as enhanced qubit control, longer coherence times, and improved extensibility. Recent advances in heterostructure material growth have opened new possibilities for employing hole spins in semiconductors for qubit applications. Undoped, strained Ge/SiGe quantum wells are promising candidate hosts for hole spin-based qubits due to their low disorder, large intrinsic spin–orbit coupling strength, and absence of valley states. Here, we use a simple one-layer gated device structure to demonstrate both a single quantum dot as well as coupling between two adjacent quantum dots. The hole effective mass in these undoped structures, m* ∼ 0.08 m0, is significantly lower than for electrons in Si/SiGe, pointing to the possibility of enhanced tunnel couplings in quantum dots and favorable qubit–qubit interactions in an industry-compatible semiconductor platform.

Control over the interaction between single photons and individual optical emitters is an outstanding problem in quantum science and engineering. It is of interest for ultimate control over light quanta, as well as for potential applications such as efficient photon collection, single-photon switching and transistors, and long-range optical coupling of quantum bits. Recently, substantial advances have been made towards these goals, based on modifying photon fields around an emitter using high-finesse optical cavities. Here we demonstrate a cavity-free, broadband approach for engineering photon-emitter interactions via subwavelength confinement of optical fields near metallic nanostructures. When a single CdSe quantum dot is optically excited in close proximity to a silver nanowire, emission from the quantum dot couples directly to guided surface plasmons in the nanowire, causing the wire's ends to light up. Non-classical photon correlations between the emission from the quantum dot and the ends of the nanowire demonstrate that the latter stems from the generation of single, quantized plasmons. Results from a large number of devices show that efficient coupling is accompanied by more than 2.5-fold enhancement of the quantum dot spontaneous emission, in good agreement with theoretical predictions.

Photoluminescence (PL) intermittency characteristics are examined for single quantum dots (QDs) in a CdSe QD sample synthesized at a slow rate at 75 degrees C. Although the PL quantum efficiency was relatively low ( approximately 0.25), we noticed that the PL intensity of single CdSe QDs fluctuated on a subsecond time scale with short-lived "on" and "off" states. The subsecond PL intensity fluctuations of CdSe QDs are different from "on" and "off" PL blinking generally observed for QDs fluctuating on a millisecond to minute time scale. We characterized single QDs by identifying polarized excitations, topographic imaging using atomic force microscopy (AFM), and transmission electron microscopy (TEM). From analysis of the PL intensity trajectories from >100 single CdSe QDs, the average intermittency time was 213 ms. From the PL quantum efficiency, slow growth of QDs, intensity trajectory analyses, and previous reports relating surface trap states and PL properties of QDs, we attribute the subsecond PL intensity fluctuations of single CdSe QDs and short-lived "on" and "off" states to a high-density distribution of homogeneous surface trap states.