Inorganic surface passivation of PbS nanocrystals resulting in strong photoluminescent emission

Strong photoluminescent emission has been obtained from 3 nm PbS nanocrystals in aqueous colloidal solution, following treatment with CdS precursors. The observed emission can extend across the entire visible spectrum and usually includes a peak near 1.95 eV. We show that much of the visible emission results from absorption by higher-lying excited states above 3.0 eV with subsequent relaxation to and emission from states lying above the observed band-edge of the PbS nanocrystals. The fluorescent lifetimes for this emission are in the nanosecond regime, characteristic of exciton recombination.

Polarized photoluminescence from surface-passivated lead sulfide nanocrystals

Effective surface passivation of lead sulfide (PbS) nanocrystals (NCs) in an aqueous colloidal solution has been achieved following treatment with CdS precursors. The resultant photoluminescent emission displays two distinct components, one originating from the absorption band edge and the other from above the absorption band edge. We show that both of these components are strongly polarized but display distinctly different behaviours. The polarization arising from the band edge shows little dependence on the excitation energy while the polarization of the above-band-edge component is strongly dependent on the excitation energy. In addition, time-resolved polarization spectroscopy reveals that the above-band-edge polarization is restricted to the first couple of nanoseconds, while the band edge polarization is nearly constant over hundreds of nanoseconds. We recognize an incompatibility between the two different polarization behaviours, which enables us to identify two distinct types of surface-passivated PbS NC.

Simulations of Bose fields at finite temperature

We introduce a time-dependent projected Gross-Pitaevskii equation to describe a partially condensed homogeneous Bose gas, and find that this equation will evolve randomized initial wave functions to equilibrium. We compare our numerical data to the predictions of a gapless, second order theory of Bose-Einstein condensation [S. A. Morgan, J. Phys. B 33, 3847 (2000)], and find that we can determine a temperature when the theory is valid. As the Gross-Pitaevskii equation is nonperturbative, we expect that it can describe the correct thermal behavior of a Bose gas as long as all relevant modes are highly occupied. Our method could be applied to other boson fields.

Time-reversal test for stochastic quantum dynamics

The calculation of quantum dynamics is currently a central issue in theoretical physics, with diverse applications ranging from ultracold atomic Bose-Einstein condensates to condensed matter, biology, and even astrophysics. Here we demonstrate a conceptually simple method of determining the regime of validity of stochastic simulations of unitary quantum dynamics by employing a time-reversal test. We apply this test to a simulation of the evolution of a quantum anharmonic oscillator with up to 6.022×1023 (Avogadro's number) of particles. This system is realizable as a Bose-Einstein condensate in an optical lattice, for which the time-reversal procedure could be implemented experimentally.

Superchemistry: dynamics of coupled atomic and molecular Bose condensates

We analyze the dynamics of a dilute, trapped Bose-condensed atomic gas coupled to a diatomic molecular Bose gas by coherent Raman transitions. This system is shown to result in a new type of “superchemistry,” in which giant collective oscillations between the atomic and the molecular gas can occur. The phenomenon is caused by stimulated emission of bosonic atoms or molecules into their condensate phases.

Gauge P-representations for quantum-dynamical problems: Removal of boundary terms

P-representation techniques, which have been very successful in quantum optics and in other fields, are also useful for general bosonic quantum-dynamical many-body calculations such as Bose-Einstein condensation. We introduce a representation called the gauge P representation, which greatly widens the range of tractable problems. Our treatment results in an infinite set of possible time evolution equations, depending on arbitrary gauge functions that can be optimized for a given quantum system. In some cases, previous methods can give erroneous results, due to the usual assumption of vanishing boundary conditions being invalid for those particular systems. Solutions are given to this boundary-term problem for all the cases where it is known to occur: two-photon absorption and the single-mode laser. We also provide some brief guidelines on how to apply the stochastic gauge method to other systems in general, quantify the freedom of choice in the resulting equations, and make a comparison to related recent developments.

Investigation of the role of cadmium sulfide in the surface passivation of lead sulfide quantum dots

Surface passivation of PbS nanocrystals (NC), resulting in strong photoluminescence, can be achieved by the introduction of CdS precursors. The role of CdS in the surface passivation of PbS NCs is uncertain, as the crystalline structure of CdS and PbS are different, which should impede effective epitaxial overgrowth. Absorption spectroscopy is used to show that the CdS precursors strongly interact with the PbS NC surface. Electron microscopy reveals that the introduction of CdS precursors results in an increased particle size, consistent with overcoating. However, we also find the process to be highly non-uniform. Nevertheless, evidence for epitaxial growth is found, suggesting that effective surface passivation may be possible.

Separating fluorescent species of aqueous PbS semiconductor nanocrystals using micro-emulsions

Colloidal PbS nanocrystals over-coated with CdS are prepared in aqueous solutions and exhibit strong photoluminescence with two distinct peaks in the visible regime. A photoluminescence peak is observed at 640 nm, which is attributed to the band edge recombination in the PbS nanocrystals, and another peak at 510 nm, which is above the band edge of the PbS nanocrystals. The two PL peaks are isolated by extracting separate species of nanocrystal based upon their surface morphology. Micro-emulsions of hexane:PVA are used to remove the species containing the PL peak at 640 nm from the solution, leaving a singular peak at 510 nm. We show conclusively that the double-peaked structure observed in the photoluminescence spectra of PbS nanocrystals over-coated with CdS is due to the presence of two distinctly different nanocrystal species.

Temperature dependence of the magnetic susceptibility for triangular-lattice antiferromagnets with spatially anisotropic exchange constants

We present the temperature dependence of the uniform susceptibility of spin-half quantum antiferromagnets on spatially anisotropic triangular lattices, using high-temperature series expansions. We consider a model with two exchange constants J1 and J2 on a lattice that interpolates between the limits of a square lattice (J1=0), a triangular lattice (J2=J1), and decoupled linear chains (J2=0). In all cases, the susceptibility, which has a Curie-Weiss behavior at high temperatures, rolls over and begins to decrease below a peak temperature Tp. Scaling the exchange constants to get the same peak temperature shows that the susceptibilities for the square lattice and linear chain limits have similar magnitudes near the peak. Maximum deviation arises near the triangular-lattice limit, where frustration leads to much smaller susceptibility and with a flatter temperature dependence. We compare our results to the inorganic materials Cs2CuCl4 and Cs2CuBr4 and to a number of organic molecular crystals. We find that the former (Cs2CuCl4 and Cs2CuBr4) are weakly frustrated and their exchange parameters determined through the temperature dependence of the susceptibility are in agreement with neutron-scattering measurements. In contrast, the organic materials considered are strongly frustrated with exchange parameters near the isotropic triangular-lattice limit.

Entanglement between a qubit and the environment in the spin-boson model

The quantitative description of the quantum entanglement between a qubit and its environment is considered. Specifically, for the ground state of the spin-boson model, the entropy of entanglement of the spin is calculated as a function of α, the strength of the ohmic coupling to the environment, and ɛ, the level asymmetry. This is done by a numerical renormalization group treatment of the related anisotropic Kondo model. For ɛ=0, the entanglement increases monotonically with α, until it becomes maximal for α→1-. For fixed ɛ>0, the entanglement is a maximum as a function of α for a value, α=αM

Superconductivity mediated by charge fluctuations in layered molecular crystals

We consider the competition between superconducting, charge ordered, and metallic phases in layered molecular crystals with the theta and beta" structures. Applying slave-boson theory to the relevant extended Hubbard model, we show that the superconductivity is mediated by charge fluctuations and the Cooper pairs have d(xy) symmetry. This is in contrast to the kappa-(BEDT-TTF)(2)X family, for which theoretical calculations give superconductivity mediated by spin fluctuations and with d(x)2(-y)2 symmetry. We predict several materials that should become superconducting under pressure.

Radiative Relaxation Quantum Yields for Synthetic Eumelanin

We report absolute values for the radiative relaxation quantum yield of synthetic eumelanin as a function of excitation energy. These values were determined by correcting for pump beam attenuation and emission reabsorption in both eumelanin samples and fluorescein standards over a large range of concentrations. Our results confirm that eumelanins are capable of dissipating >99.9% of absorbed UV and visible radiation through nonradiative means. Furthermore, we have found that the radiative quantum yield of synthetic eumelanin is excitation energy dependent. This observation is supported by corrected emission spectra, which also show a clear dependence of both peak position and peak width on excitation energy. Our findings indicate that photoluminescence emission in eumelanins is derived from ensembles of small chemically distinct oligomeric units that can be selectively pumped. This hypothesis lends support to the theory that the basic structural unit of eumelanin is oligomeric rather than heteropolymeric.