Optically induced entanglement of excitons in a single quantum Dot

Optically induced entanglement is identified by the spectrum of the phase-sensitive homodyne-detected coherent nonlinear optical response in a single gallium arsenide quantum dot. The electron-hole entanglement involves two magneto-excitonic states differing in transition energy and polarization. The strong coupling needed for entanglement is provided through the Coulomb interaction involving the electrons and holes. The result presents a first step toward the optical realization of quantum logic operations using two or more quantum dots.     

An all-optical quantum gate in a semiconductor quantum dot

We report coherent optical control of a biexciton (two electron-hole pairs), confined in a single quantum dot, that shows coherent oscillations similar to the excited-state Rabi flopping in an isolated atom. The pulse control of the biexciton dynamics, combined with previously demonstrated control of the single-exciton Rabi rotation, serves as the physical basis for a two-bit conditional quantum logic gate. The truth table of the gate shows the features of an all-optical quantum gate with interacting yet distinguishable excitons as qubits. Evaluation of the fidelity yields a value of 0.7 for the gate operation. Such experimental capability is essential to a scheme for scalable quantum computation by means of the optical control of spin qubits in dots.     

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.     

Quantization of multiparticle auger rates in semiconductor quantum dots

We have resolved single-exponential relaxation dynamics of the 2-, 3-, and 4-electron-hole pair states in nearly monodisperse cadmium selenide quantum dots with radii ranging from 1 to 4 nanometers. Comparison of the discrete relaxation constants measured for different multiple-pair states indicates that the carrier decay rate is cubic in carrier concentration, which is characteristic of an Auger process. We observe that in the quantum-confined regime, the Auger constant is strongly size-dependent and decreases with decreasing the quantum dot size as the radius cubed.     

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.     

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.     

Exciton storage in semiconductor self-assembled quantum dots

Storage and retrieval of excitons were demonstrated with semiconductor self-assembled quantum dots (QDs). The optically generated excitons were dissociated and stored as separated electron-hole pairs in coupled QD pairs. A bias voltage restored the excitons, which recombined radiatively to provide a readout optical signal. The localization of the spatially separated electron-hole pair in QDs was responsible for the ultralong storage times, which were on the order of several seconds. The present limits of this optical storage medium are discussed.     

Coupled quantum dots fabricated by cleaved edge overgrowth: from artificial atoms to molecules

Atomically precise quantum dots of mesoscopic size have been fabricated in the gallium arsenide-aluminum gallium arsenide material system by cleaved edge overgrowth, with a high degree of control over shape, composition, and position. The formation of bonding and antibonding states between two such "artificial atoms" was studied as a function of quantum dot separation by microscopic photoluminescence (PL) spectroscopy. The coupling strength within these "artificial molecules" is characterized by a systematic dependence of the separation of the bonding and antibonding levels, and of the PL linewidth, on the "interatomic" distance. This model system opens new insights into the physics of coupled quantum objects.     

Multiple exciton collection in a sensitized photovoltaic system

Multiple exciton generation, the creation of two electron-hole pairs from one high-energy photon, is well established in bulk semiconductors, but assessments of the efficiency of this effect remain controversial in quantum-confined systems like semiconductor nanocrystals. We used a photoelectrochemical system composed of PbS nanocrystals chemically bound to TiO(2) single crystals to demonstrate the collection of photocurrents with quantum yields greater than one electron per photon. The strong electronic coupling and favorable energy level alignment between PbS nanocrystals and bulk TiO(2) facilitate extraction of multiple excitons more quickly than they recombine, as well as collection of hot electrons from higher quantum dot excited states. Our results have implications for increasing the efficiency of photovoltaic devices by avoiding losses resulting from the thermalization of photogenerated carriers.     

The role of driving energy and delocalized States for charge separation in organic semiconductors

The electron-hole pair created via photon absorption in organic photoconversion systems must overcome the Coulomb attraction to achieve long-range charge separation. We show that this process is facilitated through the formation of excited, delocalized band states. In our experiments on organic photovoltaic cells, these states were accessed for a short time (<1 picosecond) via infrared (IR) optical excitation of electron-hole pairs bound at the heterojunction. Atomistic modeling showed that the IR photons promote bound charge pairs to delocalized band states, similar to those formed just after singlet exciton dissociation, which indicates that such states act as the gateway for charge separation. Our results suggest that charge separation in efficient organic photoconversion systems occurs through hot-state charge delocalization rather than energy-gradient-driven intermolecular hopping.     

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.     

Scanned probe imaging of single-electron charge states in nanotube quantum dots

An atomic force microscope was used to study single-electron motion in nanotube quantum dots. By applying a voltage to the microscope tip, the number of electrons occupying the quantum dot could be changed, causing Coulomb oscillations in the nanotube conductance. Spatial maps of these oscillations were used to locate individual dots and to study the electrostatic coupling between the dot and the tip. The electrostatic forces associated with single electrons hopping on and off the quantum dot were also measured. These forces changed the amplitude, frequency, and quality factor of the cantilever oscillation, demonstrating how single-electron motion can interact with a mechanical oscillator.     

Electrochromic nanocrystal quantum dots

Incorporating nanocrystals into future electronic or optoelectronic devices will require a means of controlling charge-injection processes and an understanding of how the injected charges affect the properties of nanocrystals. We show that the optical properties of colloidal semiconductor nanocrystal quantum dots can be tuned by an electrochemical potential. The injection of electrons into the quantum-confined states of the nanocrystal leads to an electrochromic response, including a strong, size-tunable, midinfrared absorption corresponding to an intraband transition, a bleach of the visible interband exciton transitions, and a quench of the narrow band-edge photoluminescence.     

Deterministic coupling of single quantum dots to single nanocavity modes

We demonstrate a deterministic approach to the implementation of solid-state cavity quantum electrodynamics (QED) systems based on a precise spatial and spectral overlap between a single self-assembled quantum dot and a photonic crystal membrane nanocavity. By fine-tuning nanocavity modes with a high quality factor into resonance with any given quantum dot exciton, we observed clear signatures of cavity QED (such as the Purcell effect) in all fabricated structures. This approach removes the major hindrances that had limited the application of solid-state cavity QED and enables the realization of experiments previously proposed in the context of quantum information processing.     

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.     

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.     

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.     

A tunable kondo effect in quantum dots

A tunable Kondo effect has been realized in small quantum dots. A dot can be switched from a Kondo system to a non-Kondo system as the number of electrons on the dot is changed from odd to even. The Kondo temperature can be tuned by means of a gate voltage as a single-particle energy state nears the Fermi energy. Measurements of the temperature and magnetic field dependence of a Coulomb-blockaded dot show good agreement with predictions of both equilibrium and nonequilibrium Kondo effects.     

Coherent optical control of the quantum state of a single quantum Dot

Picosecond optical excitation was used to coherently control the excitation in a single quantum dot on a time scale that is short compared with the time scale for loss of quantum coherence. The excitonic wave function was manipulated by controlling the optical phase of the two-pulse sequence through timing and polarization. Wave function engineering techniques, developed in atomic and molecular systems, were used to monitor and control a nonstationary quantum mechanical state composed of a superposition of eigenstates. The results extend the concept of coherent control in semiconductors to the limit of a single quantum system in a zero-dimensional quantum dot.     

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.