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Statistical reconstruction of optical quantum states based on mutually complementary quadrature quantum measurements
We describe a new method for reconstructing the quantum state of the electromagnetic field from the results of mutually complementary optical quadrature measurements. This method is based on the root approach and displaces squeezed Fock states are used as the basis. Theoretical analysis and numerical experiments demonstrate the considerable advantage of the developed tools over those described in the literature.
Criticality of quantum energy teleportation at phase transition points in quantum field theory
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The Structural Transition Behavior of CdSe/ZnS Core/shell Quantum Dots under High Pressure
The structural phase transition of CdSe/ZnS core/shell quantum dots (QDs) has been studied by in situ angle-dispersive X-ray diffraction under high pressure up to 53.6?GPa. The CdSe core transforms from wurtzite to rock-salt structure near 6.3?GPa and then to Cmcm or distorted Cmcm structure probably occurs at 45.1?GPa which has not been observed in CdSe nanomaterials before. The critical pressure from wurtzite to rock-salt and the bulk modulus of rock-salt phase are much higher than those for bulky and uncapped nanoparticle CdSe. The released sample can be kept in rock-salt phase for a certain time, verified by photoluminescence (PL) spectra, quite different from the reversible transition for pure CdSe. A reasonable interpretation of the experimental phenomena is given by comparing the bulk modulus of the core and shell and studying the stress sate of the core after decompression. Our study suggests that capping a hard shell is an effective approach to quench the high pressure phase of nanomaterial with a reversible phase transition.
Molecular Dynamical and Quantum Mechanical Exploration of the Site-Specific Dynamics of Cy3 Dimers Internally Linked to dsDNA
Performing spectroscopic measurements on biomolecules labeled with fluorescent probes is a powerful approach to locating the molecular behavior and dynamics of large systems at specific sites within their local environments. The indocarbocyanine dye Cy3 has emerged as one of the most commonly used chromophores. The incorporation of Cy3 dimers into DNA enhances experimental resolution owing to the spectral characteristics influenced by the geometric orientation of excitonically coupled monomeric units. Various theoretical models and simulations have been utilized to aid in the interpretation of the experimental spectra. In this study, we employ all-atom molecular dynamics simulations to study the structural dynamics of Cy3 dimers internally linked to the dsDNA backbone. We used quantum mechanical calculations to derive insights from both the linear absorption spectra and the circular dichroism data. Furthermore, we explore potential limitations within a commonly used force field for cyanine dyes. The molecular dynamics simulations suggest the presence of four possible Cy3 dimeric populations. The spectral simulations on the four populations show one of them to agree better with the experimental signatures, suggesting it to be the dominant population. Furthermore, the relative orientation of Cy3 in this population compares very well with previous predictions from the Holstein–Frenkel Hamiltonian model.
Pathways of CdS Quantum Dot Degradation during Photocatalysis: Implications for Enhancing Stability and Efficiency for Organic Synthesis
CdS quantum dots (QDs) are widely employed as photocatalysts for reactions such as hydrogen evolution, and their degradation under aerobic aqueous conditions is well understood. However, despite evidence of aggregation and precipitation of CdS QD photocatalysts under anaerobic conditions, catalyst speciation and degradation under such conditions are underexplored. In this work, we demonstrate that during a reductive dehalogenation reaction, CdS QDs undergo surface ligand etching, which leads to a loss of colloidal stability and the formation of microcrystalline cadmium metal deposits. We hypothesize that this results from the accumulation of electrons on the QD surface. In addition, we demonstrate mild surface sulfur oxidation and the formation of an ammonium salt byproduct of a commonly used hole quencher. Furthermore, this work adds to our atomic-level understanding of the reactions occurring at the QD surface during photocatalysis, so that we can design more stable and efficient photocatalysts for organic synthesis.
Semiconductor Quantum Dots Are Efficient and Recyclable Photocatalysts for Aqueous PET-RAFT Polymerization
This Letter describes the use of CdSe quantum dots (QDs) as photocatalysts for photoinduced electron transfer reversible addition–fragmentation chain transfer (PET-RAFT) polymerization of a series of aqueous acrylamides and acrylates. In this work, the high colloidal solubility and photostability of these QDs allowed polymerization to occur with high efficiency (>90% conversion in 2.5 h), low dispersity (PDI < 1.1), and ultralow catalyst loading (<0.5 ppm). The use of protein concentrators enabled the removal of the photocatalyst from the polymer and monomer with tolerable metal contamination (8.41 ug/g). These isolated QDs could be recycled for four separate polymerizations without a significant decrease in efficiency. By changing the pore size of the protein concentrators, the QDs and polymer could be separated from the remaining monomer, allowing for the synthesis of block copolymers using a single batch of QDs with minimal purification steps and demonstrating the fidelity of chain ends.
Charge Trapping in Bright and Dark States of Coupled PbS Quantum Dot Films
Analysis of photoluminescence (PL) from chemically treated lead sulfide (PbS) quantum dot (QD) films versus temperature reveals the effects of QD size and ligand binding on the motion of carriers between bright and dark trap states. For strongly coupled QDs, the PL exhibits temperature-dependent quenching and shifting consistent with charges residing in a shallow exponential tail of quasi-localized states below the band gap. The depth of the tail varies from 15 to 40 meV, similar to or smaller than exponential band tail widths measured for polycrystalline Si. The trap state distribution can be manipulated with QD size and surface treatment, and its characterization should provide a clearer picture of charge separation and percolation in disordered QD films than what currently exists.
Semiconductor Hyperbolic Metamaterials at the Quantum Limit
We study semiconductor hyperbolic metamaterials (SHMs) at the quantum limit experimentally using spectroscopic ellipsometry as well as theoretically using a new microscopic theory. The theory is a combination of microscopic density matrix approach for the material response and Green’s function approach for the propagating electric field. Our approach predicts absorptivity of the full multilayer system and for the first time allows the prediction of in-plane and out-of-plane dielectric functions for every individual layer constructing the SHM as well as effective dielectric functions that can be used to describe a homogenized SHM.
Structural properties and spatial ordering in multilayered ZnMgTe/ZnSe type-II quantum dot structures
We report the structural properties and spatial ordering of multilayer ZnMgTe quantum dots (QDs) embedded in ZnSe, where sub-monolayer quantities of Mg were introduced periodically during growth in order to reduce the valence band offset of ZnTe QDs. The periodicity, period dispersion, individual layer thickness, and the composition of the multilayer structures were determined by comparing the experimental high resolution x-ray diffraction (HRXRD) spectra to simulated ones for the allowed (004) and quasi-forbidden (002) reflections in combination with transmission electron microscopy (TEM) results. Secondary ion mass spectroscopy (SIMS) profiles confirmed the incorporation of Mg inside the QD layers, and the HRXRD analysis revealed that there is approximately 32% Mg in the ZnMgTe QDs. The presence of Mg contributes to higher scattering intensity of the HRXRD, leading to the observation of higher order superlattice peaks in both the (004) and (002) reflections. The distribution of scattered intensity in the reciprocal space map (RSM) shows that the diffuse scattered intensity is elongated along the q{sub x} axis, indicating a vertical correlation of the dots, which is found to be less defined for the sample with larger periodicity. The diffuse scattered intensity is also found to be weakly correlated along the q{sub z} direction indicating a weak lateral correlation of the dots.
Single InAs quantum dot coupled to different 'environments' in one wafer for quantum photonics
Self assembled small InAs quantum dots (SQDs) were formed in various densities and environments using gradient InAs deposition on a non-rotating GaAs substrate. Two SQD environments (SQD I and SQD II) were characterized. SQD I featured SQDs surrounded by large QDs, and SQD II featured individual SQDs in the wetting layer (WL). Micro-photoluminescence of single QDs embedded in a cavity under various excitation powers and electric fields gave insight into carrier transport processes. Potential fluctuations of the WL in SQD II, induced by charge redistribution, show promise for charge-tunable QD devices; SQD I shows higher luminescence intensity as a single-photon source.
Influence of GaAs surface termination on GaSb/GaAs quantum dot structure and band offsets
We have investigated the influence of GaAs surface termination on the nanoscale structure and band offsets of GaSb/GaAs quantum dots (QDs) grown by molecular-beam epitaxy. Transmission electron microscopy reveals both coherent and semi-coherent clusters, as well as misfit dislocations, independent of surface termination. Cross-sectional scanning tunneling microscopy and spectroscopy reveal clustered GaSb QDs with type I band offsets at the GaSb/GaAs interfaces. We discuss the relative influences of strain and QD clustering on the band offsets at GaSb/GaAs interfaces.
Enhancing structural transition by carrier and quantum confinement: Stabilization of cubic InN quantum dots by Mn incorporation
We demonstrate in this work controllable synthesis of cubic InN nanocrystals through Mn doping. We show that the pristine nanocrystal has the wurtzite structure, but can be converted into the zinc-blende (ZB) structure when it is doped with Mn. Our first-principles calculations show that the phase transition is caused by the stronger p-d coupling between the host p valence state and the impurity d level in the ZB structure, which makes the hole generation in the ZB structure easier. Quantum confinement in the nanocrystals further enhanced this effect. This observation lays an important foundation for defects control of crystal phases.
Effect of quantum dot position and background doping on the performance of quantum dot enhanced GaAs solar cells
The effect of the position of InAs quantum dots (QD) within the intrinsic region of pin-GaAs solar cells is reported. Simulations suggest placing the QDs in regions of reduced recombination enables a recovery of open-circuit voltage (V{sub OC}). Devices with the QDs placed in the center and near the doped regions of a pin-GaAs solar cell were experimentally investigated. While the V{sub OC} of the emitter-shifted device was degraded, the center and base-shifted devices exhibited V{sub OC} comparable to the baseline structure. This asymmetry is attributed to background doping which modifies the recombination profile and must be considered when optimizing QD placement.