Evidence for energy relaxation via a radiative cascade in surface-passivated PbS quantum dots

Multiple emission peaks have been observed from surface passivated PbS nanocrystals displaying strong quantum confinement. The emission spectra are shown to be strongly dependent on the excited-state parity. We also find that intraband energy relaxation from initial states excited far above the band-edge is nearly three orders of magnitude slower than that found in other nanocrystal quantum dots, providing evidence of inefficient energy relaxation via phonon emission. The initial-state parity dependence of the photoluminescent emission properties suggests that energy relaxation from the higher excited states occurs via a radiative cascade, analogous to energy relaxation in atomic systems. Such radiative cascade emission is possible from ideal zero-dimensional semiconductors, where electronic transitions can be decoupled from phonon modes.

Spin boson models for quantum decoherence of electronic excitations of biomolecules and quantum dots in a solvent

We give a theoretical treatment of the interaction of electronic excitations (excitions) in biomolecules and quantum dots with the surrounding polar solvent. Significant quantum decoherence occurs due to the interaction of the electric dipole moment of the solute with the fluctuating electric dipole moments of the individual molecules in the solvent. We introduce spin boson models which could be used to describe the effects. of decoherence on the quantum dynamics of biomolecules which undergo light-induced conformational change and on biomolecules or quantum dots which are coupled by Forster resonant energy transfer.

Entangled two-photon source using biexciton emission of an asymmetric quantum dot in a cavity

A semiconductor based scheme has been proposed for generating entangled photon pairs from the radiative decay of an electrically pumped biexciton in a quantum dot. Symmetric dots produce polarization entanglement, but experimentally realized asymmetric dots produce photons entangled in both polarization and frequency. In this work, we investigate the possibility of erasing the “which-path” information contained in the frequencies of the photons produced by asymmetric quantum dots to recover polarization-entangled photons. We consider a biexciton with nondegenerate intermediate excitonic states in a leaky optical cavity with pairs of degenerate cavity modes close to the nondegenerate exciton transition frequencies. An open quantum system approach is used to compute the polarization entanglement of the two-photon state after it escapes from the cavity, measured by the visibility of two-photon interference fringes. We explicitly relate the two-photon visibility to the degree of the Bell-inequality violation, deriving a threshold at which Bell-inequality violations will be observed. Our results show that an ideal cavity will produce maximally polarization-entangled photon pairs, and even a nonideal cavity will produce partially entangled photon pairs capable of violating a Bell-inequality.

Mesoscopic one-way channels for quantum state transfer via the quantum hall effect

We show that the one-way channel formalism of quantum optics has a physical realization in electronic systems. In particular, we show that magnetic edge states form unidirectional quantum channels capable of coherently transporting electronic quantum information. Using the equivalence between one-way photonic channels and magnetic edge states, we adapt a proposal for quantum state transfer to mesoscopic systems using edge states as a quantum channel, and show that it is feasible with reasonable experimental parameters. We discuss how this protocol may be used to transfer information encoded in number, charge, or spin states of quantum dots, so it may prove useful for transferring quantum information between parts of a solid-state quantum computer

Tunable molecular resonances of a double quantum dot Aharonov-Bohm interferometer

We investigate resonant tunnelling through molecular states of an Aharonov-Bohm (AB) interferometer composed of two coupled quantum dots. The conductance of the system shows two resonances associated with the bonding and the antibonding quantum states. We predict that the two resonances are composed of a Breit-Wigner resonance and a Fano resonance, of which the widths and Fano factor depend on the AB phase very sensitively. Further, we point out that the bonding properties, such as the covalent and ionic bonding, can be identified by the AB oscillations.

A PbS quantum-cube: conducting polymer composite for photovoltaic applications

We have developed a new non-polar synthesis for lead sulfide (PbS) quantum-cubes in the conjugated polymer poly-2-methoxy, 5-(2-ethyl-hexyloxy-p-phenylenevinylene) MEH-PPV. The conducting polymer acts to template and control the quantum-cube growth. Transmission electron microscopy of the composites has shown a bimodal distribution of cube sizes between 5 and 15 nm is produced with broad optical absorption from 300 to 650 nm. Photoluminescence suggests electronic coupling between the cubes and the conducting polymer matrix. The synthesis and initial characterization are presented in this paper. (C) 2003 Elsevier B.V. All rights reserved.

Foundations of quantum technology

Recent progress in fabrication and control of single quantum systems presage a nascent technology based on quantum principles. We review these principles in the context of specific examples including: quantum dots, quantum electromechanical systems, quantum communication and quantum computation.

TEM characterization of nanostructure and chemistry of semiconductor quantum structures

The power of advanced transmission electron microscopy in determining the nanostructures and chemistry of nanosized materials on the applications in semiconductor quantum structures was demonstrated.

Criteria for quantum coherent transfer of excitations between chromophores in a polar solvent

We show that the quantum decoherence of Forster resonant energy transfer between two optically active molecules can be described by a spin-boson model. This allows us to give quantitative criteria that are necessary for coherent quantum oscillations of excitations between the chromophores. Experimental tests of our results should be possible with flourescent resonant energy transfer (FRET) spectroscopy. Although we focus on the case of protein-pigment complexes our results are also relevant to quantum dots and organic molecules in a dielectric medium. (c) 2006 Elsevier B.V. All rights reserved.

Quantum gate based on Stark tunable nanocrystal interactions with ultrahigh-Q/V field modes in fused silica microcavities

We investigate the use of nanocrystal quantum dots as a quantum bus element for preparing various quantum resources for use in photonic quantum technologies. Using the Stark-tuning property of nanocrystal quantum dots as well as the biexciton transition, we demonstrate a photonic controlled-NOT (CNOT) interaction between two logical photonic qubits comprising two cavity field modes each. We find the CNOT interaction to be a robust generator of photonic Bell states, even with relatively large biexciton losses. These results are discussed in light of the current state of the art of both microcavity fabrication and recent advances in nanocrystal quantum dot technology. Overall, we find that such a scheme should be feasible in the near future with appropriate refinements to both nanocrystal fabrication technology and microcavity design. Such a gate could serve as an active element in photonic-based quantum technologies.

Noise in detection of qubit states using a quantum point contact

We present a model for detection of the states of a coupled quantum dots (qubit) by a quantum point contact. Most proposals for measurements of states of quantum systems are idealized. However in a real laboratory the measurements cannot be perfect due to practical devices and circuits. The models using ideal devices are not sufficient for describing the detection information of the states of the quantum systems. Our model therefore includes the extension to a non-ideal measurement device case using an equivalent circuit. We derive a quantum trajectory that describes the stochastic evolution of the state of the system of the qubit and the measuring device. We calculate the noise power spectrum of tunnelling events in an ideal and a non-ideal quantum point contact measurement respectively. We found that, for the strong coupling case it is difficult to obtain information of the quantum processes in the qubit by measurements using a non-ideal quantum point contact. The noise spectra can also be used to estimate the limits of applicability of the ideal model.

[0 0 1] zone-axis bright-field diffraction contrast from coherent Ge(Si) islands on Si(0 0 1): Dedicated to Professor Fang-hua Li on the occasion of her 70th birthday

Coherent Ge(Si)/Si(001) quantum dot islands grown by solid source molecular beam epitaxy at a growth temperature of 700degreesC were investigated using transmission electron microscopy working at 300 kV. The [001] zone-axis bright-field diffraction contrast images of the islands show strong periodicity with the change of the TEM sample substrate thickness and the period is equal to the effective extinction distance of the transmitted beam. Simulated images based on finite element models of the displacement field and using multi-beam dynamical diffraction theory show a high degree of agreement. Studies for a range of electron energies show the power of the technique for investigating composition segregation in quantum dot islands. (C) 2003 Elsevier B.V. All rights reserved.

Direct observation of mixed-parity excited states in surface-passivated PbS nanocrystals

Photoluminescent emission is observed from surface-passivated PbS nanocrystals following the two-photon excitation of high-energy excitonic states. The emission appears directly at the excitation energy with no detectable Stokes-shift for a wide range of excitation energies. The observation of direct emission from states excited by two-photon absorption indicates that the parity of the excited states of surface-passivated PbS nanocrystals is partially mixed.