Single Quantum Dot Research Articles

Colloidal Quantum Dots as Platforms for Quantum Information Science.

Colloidal quantum dots (QDs) are nanoscale semiconductor crystals with surface ligands that enable their dispersion in solvents. Quantum confinement effects facilitate wave function engineering to sculpt the spatial distribution of charge and spin states and thus the energy and dynamics of QD optical transitions. Colloidal QDs can be integrated in devices using solution-based assembly methods to position single QDs and to create ordered QD arrays. Here, we describe the synthesis, assembly, and photophysical properties of colloidal QDs that have captured scientific imagination and have been harnessed in optical applications. We focus especially on the current understanding of their quantum coherent effects and opportunities to exploit QDs as platforms for quantum information science. Freedom in QD design to isolate and control the quantum mechanical properties of charge, spin, and light presents various approaches to create systems with robust, addressable quantum states. We consider the attributes of QDs for optically addressable qubits in emerging quantum computation, sensing, simulation, and communication technologies, e.g., as robust sources of indistinguishable, single photons that can be integrated into photonic structures to amplify, direct, and tune their emission or as hosts for isolated, coherent spin states that can be coupled to light or to other spins in QD arrays.

Contribution to the Study of Sub-Bandgap Photon Absorption in Quantum Dot InAs/AlGaAs Intermediate Band Solar Cells

Intermediate band solar cells (IBSCs) pursue the increase in efficiency by absorbing below-bandgap energy photons while preserving the output voltage. Experimental IBSCs based on quantum dots (QDs) have already demonstrated that both below-bandgap photon absorption and the output voltage preservation are possible. However, the experimental work has also revealed that the below-bandgap absorption of light is weak and insufficient to boost the efficiency of the solar cells. The objective of this article is to contribute to the study of this absorption by manufacturing and characterizing a QD IBSC with a single QD layer with and without light trapping elements. Using 1-D substrate texturing, our results show a three-fold increase in the absorption of below-bandgap energy photons in the lowest energy region of the spectrum, a region not previously explored using this approach. Furthermore, we also measure, at 9K, a distinguished split of quasi-Fermi levels between the conduction and intermediate bands, which is a necessary condition to preserve the output voltage of the cell.

Photoluminescence Blinking and Biexciton Auger Recombination in Single Colloidal Quantum Dots with Sharp and Smooth Core/Shell Interfaces.

There is an inconsistence on whether a smooth core/shell interface can reduce Auger recombination and suppress photoluminescence (PL) blinking in single colloidal quantum dots (QDs). Here, we investigate the influence of a core/shell interface on PL blinking and biexciton Auger recombination by comparing the single-dot PL spectra of CdxZn1-xSeyS1-y/ZnS core/shell QDs with sharp and smooth interfaces. The inconsistence can be clarified when considering different PL blinking mechanisms. For the single QDs showing Auger blinking, a smooth core/shell interface potential can suppress PL blinking through reducing the Auger recombination. In contrast, we find slightly reduced biexciton Auger recombination rates but increased PL blinking activities in the band-edge carrier (BC)-blinking QDs with the smooth core/shell interface. This is because the smooth interface potential cannot reduce the PL blinking caused by the transfer of electrons to the surface states; however, there is potential to increase electron wave function delocalization for reducing the biexciton Auger recombination rate.

Unconventional Blinking Characteristics of Single Quantum Dots Revealed by Timing Analyses

Discontinuous emission, or “blinking”, from colloidal quantum dots (QDs) hampers the practical applications of QDs in numerous areas. The blinking of individual QDs does not have characteristic tim...

Direct high-resolution resonant Raman scattering measurements of dynamic nuclear spin polarization states of an InAs quantum dot

We report on the direct measurement of the electron spin splitting and the accompanying nuclear Overhauser (OH) field, and thus the underlying nuclear spin polarization (NSP) and fluctuation bandwidth, in a single InAs quantum dot under resonant excitation conditions with unprecedented spectral resolution. The electron spin splitting is measured directly via resonant spin-flip single photon Raman scattering detected by superconducting nanowires to generate excitation-emission energy maps. The observed two-dimensional maps reveal an OH field that has a non-linear dependence on excitation frequency. This study provides new insight into earlier reports of so-called avoidance and tracking, showing two distinct NSP responses directly by the addition of a emission energy axis. The data show that the polarization processes depend on which electron spin state is optically driven, with surprising differences in the polarization fluctuations for each case: in one case, a stabilized field characterized by a single-peaked distribution shifts monotonically with the laser excitation frequency resulting in a nearly constant optical interaction strength across a wide detuning range, while in the other case the previously reported avoidance behavior is actually the result of a nonlinear dependence on the laser excitation frequency near zero detuning leading to switching between two distinct mesoscopic nuclear spin states. The magnitude of the field, which is as large as 400 mT, is measured with sub-100 nuclear spin sensitivity. Stable/unstable points of the OH field distribution are observed, resulting from the non-linear feedback loop in the electron-trion-nuclear system. Nuclear spin polarization state switching occurs between fields differing by 160 mT at least as fast as 25 ms. Control experiments indicate that the strain-induced quadrupolar interaction may explain the measured OH fields.

Inducing micromechanical motion by optical excitation of a single quantum dot.

Hybrid quantum optomechanical systems1 interface a macroscopic mechanical degree of freedom with a single two-level system such as a single spin2-4, a superconducting qubit5-7 or a single optical emitter8-12. Recently, hybrid systems operating in the microwave domain have witnessed impressive progress13,14. Concurrently, only a few experimental approaches have successfully addressed hybrid systems in the optical domain, demonstrating that macroscopic motion can modulate the two-level system transition energy9,10,15. However, the reciprocal effect, corresponding to the backaction of a single quantum system on a macroscopic mechanical resonator, has remained elusive. In contrast to an optical cavity, a two-level system operates with no more than a single energy quantum. Hence, it requires a much stronger hybrid coupling rate compared to cavity optomechanical systems1,16. Here, we build on the large strain coupling between an oscillating microwire and a single embedded quantum dot9. We resonantly drive the quantum dot's exciton using a laser modulated at the mechanical frequency. State-dependent strain then results in a time-dependent mechanical force that actuates microwire motion. This force is almost three orders of magnitude larger than the radiation pressure produced by the photon flux interacting with the quantum dot. In principle, the state-dependent force could constitute a strategy to coherently encode the quantum dot quantum state onto a mechanical degree of freedom1.

Biexciton Dynamics in Single Colloidal CdSe Quantum Dots.

The investigation of biexciton dynamics in single colloidal quantum dots (QDs) is critical to biexciton-based applications. Generally, a biexciton exhibits an extremely low photoluminescence (PL) quantum yield as well as very fast PL decay due to strong nonradiative Auger recombination, making it difficult to investigate the biexciton dynamics. Here, we develop a quantitative method based on intensity- and time-resolved photon statistics to investigate the biexciton dynamics in single colloidal QDs. This robust method can be used under high-excitation conditions to determine the absolute radiative and Auger recombination rates of both neutral and charged biexciton states in a single QD level, and the corresponding ratios between the two states agree with the theoretical predictions of the asymmetric band structures of CdSe-based QDs. Furthermore, the surface traps are found to provide additional nonradiative recombination pathways for the biexcitons, and their contributions are quantified by the method.

“Can quantum dot in form of molecular ground be implied in IETS to measure the voltage effectively by sudden potential rise due to phonon assisted electron tunneling as Klein paradox?”

Abstract Sudden break in the passage of electron beam things conducting barrier shall either enhance or decrease electron beam with provided effect on spectral band of unknown metal, j/?dv –V at d2/dv2 plot gives characteristic of tunnel junction. At liquid helium temperature qv = hὐ implication for JV curve is observed at bias V where v denotes the frequency of molecular compounds present in the barrier, In case barrier emitting phonon interacts with the lattice of implied nano particles like Ga, As Ge Se coupled barrier in molecular state can be observed a specific band of Raman spectra and infra red thermally nactivated long wave spectra as IETS under Josephson effect. Single quantum dot in ultraclean carbonnanotube can be annexed with novel double quantum dot as result of klein paradox. At relatvistic QFT. In this context single spin1/2 can be confined with the hole emplacement and confinement as second double dot.

Self-induction and magnetic effects in electron transport through a photon cavity

We explore higher order dynamical effects in the transport through a two-dimensional nanoscale electron system embedded in a three-dimensional far-infrared photon cavity. The nanoscale system is considered to be a short quantum wire with a single circular quantum dot defined in a GaAs heterostructure. The whole system, the external leads and the central system are placed in a constant perpendicular magnetic field. The Coulomb interaction of the electrons, the para- and diamagnetic electron-photon interactions are all treated by a numerically exact diagonalization using step-wise truncations of the appropriate many-body Fock spaces. We focus on the difference in transport properties between a description within an electric dipole approximation and a description including all higher order terms in a single photon mode model. We find small effects mostly caused by an electrical quadrupole and a magnetic dipole terms that depend strongly on the polarization of the cavity field with respect to the transport direction and the photon energy. When the polarization is aligned along the transport direction we find indications of a weak self-induction that we analyze and compare to the classical counterpart, and the self-energy contribution of high-order interaction terms to the states the electrons cascade through on their way through the system. Like expected the electron-photon interaction is well described in the dipole approximation when it is augmented by the lowest order diamagnetic part for a nanoscale system in a cavity in an external magnetic field.

Photoexcitation Dynamics in Electrochemically Charged CdSe Quantum Dots: From Hot Carrier Cooling to Auger Recombination of Negative Trions

Fulfilling the potential of colloidal semiconductor quantum dots (QDs) in electrically driven applications remains a challenge largely since operation of such devices involves charged QDs with drastically different photophysical properties compared to their well-studied neutral counterparts. In this work, the full picture of excited state dynamics in charged CdSe QDs at various time scales has been revealed via transient absorption spectroscopy combined with electrochemistry as a direct manipulation tool to control the negative charging of CdSe QDs. In trions, excited states of single charged QDs, the additional electron in the conduction band speeds up the hot electron cooling by enhanced electron-electron scattering followed by charge redistribution and polaron formation in a picosecond time scale. The trions are finally decayed by the Auger process in a 500 ps time scale. Double charging in QDs, on the other hand, decelerates the polaron formation process while accelerates the following Auger decay. Our work demonstrates the potential of photoelectrochemistry as a platform for ultrafast spectroscopy of charged species and paves the way for further studies to develop comprehensive knowledge of the photophysical processes in charged QDs more than the well-known Auger decay, facilitating their use in future optoelectronic applications. (Less)

Thermal stability of emission from single InGaAs/GaAs quantum dots at the telecom O-band

Single-photon sources are key building blocks in most of the emerging secure telecommunication and quantum information processing schemes. Semiconductor quantum dots (QD) have been proven to be the most prospective candidates. However, their practical use in fiber-based quantum communication depends heavily on the possibility of operation in the telecom bands and at temperatures not requiring extensive cryogenic systems. In this paper we present a temperature-dependent study on single QD emission and single-photon emission from metalorganic vapour-phase epitaxy-grown InGaAs/GaAs QDs emitting in the telecom O-band at 1.3 μm. Micro-photoluminescence studies reveal that trapped holes in the vicinity of a QD act as reservoir of carriers that can be exploited to enhance photoluminescence from trion states observed at elevated temperatures up to at least 80 K. The luminescence quenching is mainly related to the promotion of holes to higher states in the valence band and this aspect must be primarily addressed in order to further increase the thermal stability of emission. Photon autocorrelation measurements yield single-photon emission with a purity of {g}_{50K}^{(2)}left(0right)=0.13 up to 50 K. Our results imply that these nanostructures are very promising candidates for single-photon sources at elevated (e.g., Stirling cryocooler compatible) temperatures in the telecom O-band and highlight means for improvements in their performance.

Deterministically fabricated strain-tunable quantum dot single-photon sources emitting in the telecom O-band

Most quantum communication schemes aim at the long-distance transmission of quantum information. In the quantum repeater concept, the transmission line is subdivided into shorter links interconnected by entanglement distribution via Bell-state measurements to overcome inherent channel losses. This concept requires on-demand single-photon sources with a high degree of multi-photon suppression and high indistinguishability within each repeater node. For a successful operation of the repeater, a spectral matching of remote quantum light sources is essential. We present a spectrally tunable single-photon source emitting in the telecom O-band with the potential to function as a building block of a quantum communication network based on optical fibers. A thin membrane of GaAs embedding InGaAs quantum dots (QDs) is attached onto a piezoelectric actuator via gold thermocompression bonding. Here, the thin gold layer acts simultaneously as an electrical contact, strain transmission medium, and broadband backside mirror for the QD-micromesa. The nanofabrication of the QD-micromesa is based on in situ electron-beam lithography, which makes it possible to integrate pre-selected single QDs deterministically into the center of monolithic micromesa structures. The QD pre-selection is based on distinct single-QD properties, signal intensity, and emission energy. In combination with strain-induced fine tuning, this offers a robust method to achieve spectral resonance in the emission of remote QDs. We show that the spectral tuning has no detectable influence on the multi-photon suppression with g(2)(0) as low as 2%–4% and that the emission can be stabilized to an accuracy of 4 μeV using a closed-loop optical feedback.

Deacetylation-activated construction of single quantum dot-based nanosensor for sirtuin 1 assay

Sirtuin 1 (SIRT1) is an important histone deacetylase that regulates biological functions ranging from DNA repair to metabolism. The alteration of SIRT1 is associated with a variety of diseases including diabetes, inflammation, aging-related diseases, and cancers. Consequently, the detection of SIRT1 activity is of great therapeutic importance. Herein, we demonstrate for the first time the deacetylation-activated construction of single quantum dot (QD)-based nanosensor for sensitive SIRT1 assay. This nanosensor is composed of a Cy5-labeled peptide substrate and a streptavidin-coated QD. The peptide with one lysine acetyl group acts as both the Cy5 fluorophore carrier and the substrate for sensing SIRT1. In the presence of SIRT1, it removes the acetyl group in the acetylated peptide, and the resultant deacetylated peptide can react with the NHS-activated biotin reagent (sulfo-NHS-biotin) to form the biotinylated peptide. The multiple biotinylated peptides can assemble on single QD surface via biotin-streptavidin interaction, inducing efficient fluorescence resonance energy transfer (FRET) from the QD to Cy5, generating distinct Cy5 signal which can be simply quantified by total internal reflection fluorescence-based single-molecule detection. This single QD-based nanosensor can sensitively detect SIRT1 with a detection limit of as low as 3.91 pM, and it can be applied for the measurement of enzyme kinetic parameters and the screening of SIRT1 inhibitors. Moreover, this nanosensor can be used to detect the SIRT1 activity in cancer cells, providing a powerful platform for epigenetic research and SIRT1-targeted drug discovery.

Blinking Mechanisms and Intrinsic Quantum-Confined Stark Effect in Single Methylammonium Lead Bromide Perovskite Quantum Dots.

Lead halide perovskite quantum dots (QDs) are promising materials for next-generation photoelectric devices because of their low preparation costs and excellent optoelectronic properties. In this study, the blinking mechanisms and the intrinsic quantum-confined Stark effect (IQCSE) in single organic-inorganic hybrid CH3 NH3 PbBr3 perovskite QDs using single-dot photoluminescence (PL) spectroscopy is investigated. The PL quantum yield-recombination rates distribution map allows the identification of different PL blinking mechanisms and their respective contributions to the PL emission behavior. A strong correlation between the excitation power and the blinking mechanisms is reported. Most single QDs exhibit band-edge carrier blinking under a low excitation photon fluence. While under a high excitation photon fluence, different proportions of Auger-blinking emerge in their PL intensity trajectories. In particular, significant IQCSEs in the QDs that exhibit more pronounced Auger-blinking are observed. Based on these findings, an Auger-induced IQCSE model to explain the observed IQCSE phenomena is observed.

Fabrication of Quantum Dots@Metal–Organic Frameworks Nanocomposites By Direct Surface Modification

Semiconductor quantum dots (QDs), have been attracting much attention as the next generation of light-emitting materials due to their unique properties, such as their broad absorption range and narrow band-edge photoluminescence (PL) with high emission quantum yield. Since, in particular, precise controllability of luminescent color by changing the QD size is quite attractive and useful, they have been practically used in devices such as back light films of liquid crystal display. Although highly dense QDs are required for color filters and on chip light sources with high efficiency, Förster resonance energy transfer (FRET) to non-fluorescent QDs is inevitable when each QDs adjacently exists, resulting in large decline in quantum yields (QY). One of the reasons to generate non-fluorescent QDs is the accumulation of damage over time to the organic ligands attached to the surface as a passivation layer. To overcome the QD degradation derived from organic ligands desorption, the development of robust and easily grown surface protective materials is important.Metal–organic frameworks (MOFs), which are a new class of microporous crystalline materials formed by the self-assembly of metal ions and organic linkers, are promising candidates as new surface modification materials for QDs. Owing to their versatile architecture and adjustable functionality derived from the combination of their components, MOFs possess high variety of applications, such as gas storage, catalysts, and semiconductors. Among them, the combinations of MOFs with other categories of nanomaterials, such as metal nanoparticles, have attracted much attention lately to give further functionalities to MOFs. Therefore, if MOFs are utilizable as new classes of surface modifiers for fluorescent QDs, not only the stability improvement but also new functionality appearance of QDs are expected.In this study, the aforementioned possibility of MOFs toward fluorescent QDs was investigated. CdSe/CdS core/shell QDs were attempted to be covered by zeolitic imidazolate framework-8 (ZIF-8) through a direct link between the two without using any other bonding materials like polymers. The QDs were observed to be fully incorporated into the ZIF-8 crystal and were photoluminescent with a solid-state PL QY as high as 40%. Narrow band-edge emission unique to the QDs was maintained during and after the modification with ZIF-8. In addition, we visually confirmed the structure of ZIF-8 crystals gradually transformed from a roughly spherical shape to rhombic dodecahedra (Fig. 1). The incorporation of a single QD into a ZIF-8 crystal was also successfully accomplished by changing the ligands on the starting QDs. To evaluate the potential of ZIF-8 as a protecting shell for QDs, 1,4-benzoquinone, one of the efficient electron acceptors that can quench the PL from CdSe/CdS core/shell QDs, was added to the solution of pyridine-capped CdSe/CdS core/shell QDs as well as a suspension of CdSe/CdS QD@ZIF-8 composite. As shown in Fig. 2, the addition of 1,4-benzoquinone hardly affected the PL of the QDs after ZIF-8 modification, indicating complete incorporation of the QDs into ZIF-8 crystals. Figure 1

Strong coupling of single quantum dots with low-refractive-index/high-refractive-index materials at room temperature.

Strong coupling between a cavity and transition dipole moments in emitters leads to vacuum Rabi splitting. Researchers have not reported strong coupling between a single emitter and a dielectric cavity at room temperature until now. In this study, we investigated the photoluminescence (PL) spectra of colloidal quantum dots on the surface of a SiO2/Si material at various collection angles at room temperature. We measured the corresponding reflection spectra for the SiO2/Si material and compared them with the PL spectra. We observed PL spectral splitting and regarded it as strong coupling between colloidal quantum dots and the SiO2/Si material. Upper polaritons and lower polaritons exhibited anticrossing behavior. We observed Rabi splitting from single-photon emission in the dielectric cavity at room temperature. Through analysis, we attributed the Rabi splitting to strong coupling between quantum dots and bound states in the continuum in the low-refractive-index/high-refractive-index hybrid material.

Unraveling the Origin of the Long Fluorescence Decay Component of Cesium Lead Halide Perovskite Nanocrystals.

A common signature of nearly all nanoscale emitters is fluorescence intermittency, which is a rapid switching between “on”-states exhibiting a high photon emission rate and “off”-states with a much lower rate. One consequence of fluorescence intermittency occurring on time scales longer than the exciton decay time is the so-called delayed photon emission, manifested by a long radiative decay component. Besides their dominant fast radiative decay, fully inorganic cesium lead halide perovskite quantum dots exhibit a long fluorescence decay component at cryogenic temperatures that is often attributed to the decay of the dark exciton. Here, we show that its origin is delayed photon emission by investigating temporal variations in fluorescence intensity and concomitant decay times found in single CsPbBr3 perovskite quantum dots. We attribute the different intensity levels of the intensity trace to a rapid switching between a high-intensity exciton state and an Auger-reduced low-intensity trion state that occurs when the excitation is sufficiently strong. Surprisingly, we observe that the exponent of this power-law-dependent delayed emission is correlated with the emission intensity, which cannot be explained with existing charge carrier trapping models. Our analysis reveals that the long decay component is mainly governed by delayed emission, which is present in both the exciton and trion state. The absence of a fine structure in trions clarifies the vanishing role of the dark exciton state for the long decay component. Our findings are essential for the development of a complete photophysical model that captures all observed features of fluorescence variations in colloidal nanocrystals.

Plasmon-Field-Induced Metastable States in the Wetting Layer: Detected by the Fluorescence Decay Time of InAs/GaAs Single Quantum Dots

We report a new way to slow down the spontaneous emission rate of excitons in the wetting layer (WL) through radiative field coupling between the exciton emissions and the dipole field of metal isl...

Optical absorption coefficient calculations of GaSb/GaAs quantum dots for intermediate band solar cell applications

Absorption coefficients of GaSb/GaAs quantum dots (QDs) are calculated by the 8-band strain-dependent k· p method and Fermi’s golden rule. A more realistic but simple approach to model the QD ensemble with wetting layer is described. Effects of the QD size and density, and the GaAs spacer thickness for multi-stacked QDs on absorption characteristics are studied. Absorption spectra of the single QD, single layer of QDs, and multi-stacked QDs are presented and discussed. Interband absorption is found to be more intense than intraband absorption. The calculated absorption spectra are brought into the drift-diffusion model coupled with rate equations to determine the current density-voltage curves of the GaSb/GaAs QD solar cells, which are compared with measured data in literature for validation. The models proposed in this work are capable of predicting the short-circuit current density and open-circuit voltage of real devices, and would have the potential to investigate the impact of doping and position of the QD layers, which is necessary for intermediate band solar cell analysis and design.

Features of Two-Dimensional Bifurcations during Dissipative Electron Tunneling in Arrays of Au Nanoparticles

Within the 2D theory of dissipative tunneling in the semiclassical approximation (a rarefied gas of instanton–anti-instanton pairs) at a finite temperature in the presence of an external electric field, the features of tunneling transport in the planar structures with the quantum dots made of colloidal gold—which, presumably, possess the properties of a metamaterial—are investigated. It is shown experimentally that either a single effect or a double effect of 2D tunnel bifurcations (in the form of a kink or kinks on the tunneling current–voltage curve) is observed depending on the position of the cantilever tip of a combined atomic force and scanning tunneling microscope (AFM/STM), which can be either above a single quantum dot or between two adjacent quantum dots, respectively. As our theoretical model shows, such a regime of double bifurcation (a double smoothed kink on the tunneling current–voltage curve) that is associated with the manifestation of the properties of a metamaterial by the structure under study. A convincing qualitative agreement is obtained between the experimental current–voltage characteristics and the field dependence of the probability of 2D dissipative tunneling in the two investigated regimes with due regard for the observed quantum beats (oscillations) in the vicinity of 2D bifurcation points.