Linearly polarized emission from colloidal semiconductor quantum rods

Colloidal quantum rods of cadmium selenide (CdSe) exhibit linearly polarized emission. Empirical pseudopotential calculations predict that slightly elongated CdSe nanocrystals have polarized emission along the long axis, unlike spherical dots, which emit plane-polarized light. Single-molecule luminescence spectroscopy measurements on CdSe quantum rods with an aspect ratio between 1 and 30 confirm a sharp transition from nonpolarized to purely linearly polarized emission at an aspect ratio of 2. Linearly polarized luminescent chromophores are highly desirable in a variety of applications.     

Optical signatures of coupled quantum dots

An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function. The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots. Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots. This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing.     

Slow electron cooling in colloidal quantum dots

Hot electrons in semiconductors lose their energy very quickly (within picoseconds) to lattice vibrations. Slowing this energy loss could prove useful for more efficient photovoltaic or infrared devices. With their well-separated electronic states, quantum dots should display slow relaxation, but other mechanisms have made it difficult to observe. We report slow intraband relaxation (>1 nanosecond) in colloidal quantum dots. The small cadmium selenide (CdSe) dots, with an intraband energy separation of approximately 0.25 electron volts, are capped by an epitaxial zinc selenide (ZnSe) shell. The shell is terminated by a CdSe passivating layer to remove electron traps and is covered by ligands of low infrared absorbance (alkane thiols) at the intraband energy. We found that relaxation is markedly slowed with increasing ZnSe shell thickness.     

Suppressing spin qubit dephasing by nuclear state preparation

Coherent spin states in semiconductor quantum dots offer promise as electrically controllable quantum bits (qubits) with scalable fabrication. For few-electron quantum dots made from gallium arsenide (GaAs), fluctuating nuclear spins in the host lattice are the dominant source of spin decoherence. We report a method of preparing the nuclear spin environment that suppresses the relevant component of nuclear spin fluctuations below its equilibrium value by a factor of approximately 70, extending the inhomogeneous dephasing time for the two-electron spin state beyond 1 microsecond. The nuclear state can be readily prepared by electrical gate manipulation and persists for more than 10 seconds.     

Water-soluble quantum dots for multiphoton fluorescence imaging in vivo

The use of semiconductor nanocrystals (quantum dots) as fluorescent labels for multiphoton microscopy enables multicolor imaging in demanding biological environments such as living tissue. We characterized water-soluble cadmium selenide-zinc sulfide quantum dots for multiphoton imaging in live animals. These fluorescent probes have two-photon action cross sections as high as 47,000 Goeppert-Mayer units, by far the largest of any label used in multiphoton microscopy. We visualized quantum dots dynamically through the skin of living mice, in capillaries hundreds of micrometers deep. We found no evidence of blinking (fluorescence intermittency) in solution on nanosecond to millisecond time scales.     

Mode locking of electron spin coherences in singly charged quantum dots

The fast dephasing of electron spins in an ensemble of quantum dots is detrimental for applications in quantum information processing. We show here that dephasing can be overcome by using a periodic train of light pulses to synchronize the phases of the precessing spins, and we demonstrate this effect in an ensemble of singly charged (In,Ga)As/GaAs quantum dots. This mode locking leads to constructive interference of contributions to Faraday rotation and presents potential applications based on robust quantum coherence within an ensemble of dots.     

柱形量子点的能级与电子结构

在EMA(Effective Mass Approximation)的理论框架下,研究了柱形量子点的能级和电子结构.计算了柱形量子点的激发态(m=1)基态(m=0)能量,并作出柱形量子点能量图;还计算了柱形量子点的电子概率密度,并作出电子概率分布图.     

Optical gain and stimulated emission in nanocrystal quantum dots

The development of optical gain in chemically synthesized semiconductor nanoparticles (nanocrystal quantum dots) has been intensely studied as the first step toward nanocrystal quantum dot lasers. We examined the competing dynamical processes involved in optical amplification and lasing in nanocrystal quantum dots and found that, despite a highly efficient intrinsic nonradiative Auger recombination, large optical gain can be developed at the wavelength of the emitting transition for close-packed solids of these dots. Narrowband stimulated emission with a pronounced gain threshold at wavelengths tunable with the size of the nanocrystal was observed, as expected from quantum confinement effects. These results unambiguously demonstrate the feasibility of nanocrystal quantum dot lasers.     

量子点及其在食品安全检测中的应用

量子点是近年来发展起来的一种新型荧光探针,与传统有机荧光染料相比具有优良光学性质,以其为基础衍生出的检测技术具有简单、快速、灵敏、稳定和高通量等特点.为了解量子点及其在食品安全检测中的应用研究现状,为量子点在食品安全检测中的进一步推广应用,从量子点的光学特性、制备及表面修饰、量子点在食品安全检测中的应用等方面的研究进行...     

Excitation spectra of circular, few-electron quantum dots

Studies of the ground and excited states in semiconductor quantum dots containing 1 to 12 electrons showed that the quantum numbers of the states in the excitation spectra can be identified and compared with exact calculations. A magnetic field induces transitions between the ground and excited states. These transitions were analyzed in terms of crossings between single-particle states, singlet-triplet transitions, spin polarization, and Hund's rule. These impurity-free quantum dots allow "atomic physics" experiments to be performed in magnetic field regimes not accessible for atoms.     

Probing and controlling the bonds of an artificial molecule

We demonstrate how molecular quantum states of coupled semiconductor quantum dots are coherently probed and manipulated in transport experiments. The applied method probes quantum states by the virtual cotunneling of two electrons and hence resolves the sequences of molecular states simultaneously. This result is achieved by weakly probing the quantum system through parallel contacts to its constituting quantum dots. The overlap of the dots' wave functions and, in turn, the splitting of molecular states are adjusted by the direct influence of coupling electrodes.     

Coupling and entangling of quantum states in quantum dot molecules

We demonstrate coupling and entangling of quantum states in a pair of vertically aligned, self-assembled quantum dots by studying the emission of an interacting electron-hole pair (exciton) in a single dot molecule as a function of the separation between the dots. An interaction-induced energy splitting of the exciton is observed that exceeds 30 millielectron volts for a dot layer separation of 4 nanometers. The results are interpreted by mapping the tunneling of a particle in a double dot to the problem of a single spin. The electron-hole complex is shown to be equivalent to entangled states of two interacting spins.     

Conditional dynamics of interacting quantum dots

Conditional quantum dynamics, where the quantum state of one system controls the outcome of measurements on another quantum system, is at the heart of quantum information processing. We demonstrate conditional dynamics for two coupled quantum dots, whereby the probability that one quantum dot makes a transition to an optically excited state is controlled by the presence or absence of an optical excitation in the neighboring dot. Interaction between the dots is mediated by the tunnel coupling between optically excited states and can be optically gated by applying a laser field of the right frequency. Our results represent substantial progress toward realization of an optically effected controlled-phase gate between two solid-state qubits.     

Coherent optical spectroscopy of a strongly driven quantum dot

Quantum dots are typically formed from large groupings of atoms and thus may be expected to have appreciable many-body behavior under intense optical excitation. Nonetheless, they are known to exhibit discrete energy levels due to quantum confinement effects. We show that, like single-atom or single-molecule two- and three-level quantum systems, single semiconductor quantum dots can also exhibit interference phenomena when driven simultaneously by two optical fields. Probe absorption spectra are obtained that exhibit Autler-Townes splitting when the optical fields drive coupled transitions and complex Mollow-related structure, including gain without population inversion, when they drive the same transition. Our results open the way for the demonstration of numerous quantum level-based applications, such as quantum dot lasers, optical modulators, and quantum logic devices.     

Excimers and exciplexes of conjugated polymers

Observations of intermolecular excimers in several pi-conjugated polymers and exciplexes of these polymers with tris(p-tolyl) amine are reported. It is shown that the luminescence of conjugated polymer thin films originates from excimer emission and that the generally low quantum yield is the result of self-quenching. Thus, in sufficiently dilute solution, the "single-chain" emission has a quantum yield of unity. Exciplex luminescence and exciplex-mediated charge photogeneration have much higher quantum yields than the excimer-mediated photophysical processes. These results provide a basis for understanding and controlling the photophysics of conjugated polymers in terms of supramolecular structure and morphology.     

量子点标记技术在食源性病原体检测中的研究进展

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Fermionic bell-state analyzer for spin qubits

We propose a protocol and physical implementation for partial Bell-state measurements of Fermionic qubits, allowing for deterministic quantum computing in solid-state systems without the need for two-qubit gates. Our scheme consists of two spin qubits in a double quantum dot where the two dots have different Zeeman splittings and resonant tunneling between the dots is only allowed when the spins are antiparallel. This converts spin parity into charge information by means of a projective measurement and can be implemented with established technologies. This measurement-based qubit scheme greatly simplifies the experimental realization of scalable quantum computers in electronic nanostructures.     

Peak external photocurrent quantum efficiency exceeding 100% via MEG in a quantum dot solar cell

Multiple exciton generation (MEG) is a process that can occur in semiconductor nanocrystals, or quantum dots (QDs), whereby absorption of a photon bearing at least twice the bandgap energy produces two or more electron-hole pairs. Here, we report on photocurrent enhancement arising from MEG in lead selenide (PbSe) QD-based solar cells, as manifested by an external quantum efficiency (the spectrally resolved ratio of collected charge carriers to incident photons) that peaked at 114 ± 1% in the best device measured. The associated internal quantum efficiency (corrected for reflection and absorption losses) was 130%. We compare our results with transient absorption measurements of MEG in isolated PbSe QDs and find reasonable agreement. Our findings demonstrate that MEG charge carriers can be collected in suitably designed QD solar cells, providing ample incentive to better understand MEG within isolated and coupled QDs as a research path to enhancing the efficiency of solar light harvesting technologies.     

The Kondo effect in an artificial quantum dot molecule

Double quantum dots provide an ideal model system for studying interactions between localized impurity spins. We report on the transport properties of a series-coupled double quantum dot as electrons are added one by one onto the dots. When the many-body molecular states are formed, we observe a splitting of the Kondo resonance peak in the differential conductance. This splitting reflects the energy difference between the bonding and antibonding states formed by the coherent superposition of the Kondo states of each dot. The occurrence of the Kondo resonance and its magnetic field dependence agree with a simple interpretation of the spin status of a double quantum dot.     

Quantum-confined stark effect in single CdSe nanocrystallite quantum dots

The quantum-confined Stark effect in single cadmium selenide (CdSe) nanocrystallite quantum dots was studied. The electric field dependence of the single-dot spectrum is characterized by a highly polarizable excited state ( approximately 10(5) cubic angstroms, compared to typical molecular values of order 10 to 100 cubic angstroms), in the presence of randomly oriented local electric fields that change over time. These local fields result in spontaneous spectral diffusion and contribute to ensemble inhomogeneous broadening. Stark shifts of the lowest excited state more than two orders of magnitude larger than the linewidth were observed, suggesting the potential use of these dots in electro-optic modulation devices.