Entropy of quantum states: Ambiguities

The von Neumann entropy of a generic quantum state is not unique unless the state can be uniquely decomposed as a sum of extremal or pure states. As pointed out to us by Sorkin, this happens if the GNS representation (of the algebra of observables in some quantum state) is reducible, and some representations in the decomposition occur with non-trivial degeneracy. This non-unique entropy can occur at zero temperature. We will argue elsewhere in detail that the degeneracies in the GNS representation can be interpreted as an emergent broken gauge symmetry, and play an important role in the analysis of emergent entropy due to non-Abelian anomalies. Finally, we establish the analogue of an H-theorem for this entropy by showing that its evolution is Markovian, determined by a stochastic matrix.

Near infrared detectors based on HgSe and HgCdSe quantum dots generated at the liquid-liquid interface

HgSe and Hg0.5Cd0.5Se quantum dos (QDs) are synthesized at room temperature by a novel liquid-liquid interface method and their photodetection properties in the near-IR region are investigated. The photodetection properties of our Te-free systems are found to be comparable to those of the previously reported high performance QD vis-IR detectors including HgTe. The present synthesis indicates the cost-effectiveness of selenium based IR detectors owing to the abundance and lower toxicity of selenium compared to tellurium.

Evolution of ferromagnetism from a frustrated state in LixNi(2-x)O2 (0.67 < x < 0.98)

Two-dimensional triangular-lattice antiferromagnetic systems continue to be an interesting area in condensed matter physics and LiNiO2 is one such among them. Here we present a detailed experimental magnetic study of the quasi-stoichiometric LixNi2-xO2 system (0.67

Highly photoactive heterostructures of PbO quantum dots on TiO2

We present a non-hydrolytic sol-gel combustion method for synthesizing nanocomposites of PbO quantum dots on anatase TiO2 with a high surface area. XRD, electron microscopy, DRS, cathodoluminescence and BET were employed for structural, microstructural and optical characterization of the composites. The photocatalytic activity of TiO2 and PbO/TiO2 was investigated and compared with Degussa P-25. The results indicate that the photocatalytic activity of quantum dot dispersed TiO2 is higher than that of bare TiO2 and much higher than that of commercial Degussa P-25. The origin of enhanced photoreactivity of the synthesized material can be assigned to a synergetic effect of high surface area, higher number of active sites and an engineered band structure in the heterostructure. The mechanisms for photocatalytic activity are discussed based on production of photogenerated reactive species. The knowledge gained through this report open up ideal synthesis routes for designing advanced functional heterostructures with engineered band structure and has important implications in solar energy based applications.

Tuning the parameters to establish Quenching and enhancement regimes in hybrid Gold nanoparticles and CdSe Quantum dots monolayer

The multi-component nanomaterials combine the individual properties and give rise to emergent phenomenon. Optical excitations in such hybrid nonmaterial's ( for example Exciton in semiconductor quantum dots and Plasmon in Metal nanomaterials) undergo strong weak electromagnetic coupling. Such exciton-plasmon interactions allow design of absorption and emission properties, control of nanoscale energy-transfer processes, and creation of new excitations in the strong coupling regime.This Exciton plasmon interaction in hybrid nanomaterial can lead to both enhancement in the emission as well as quenching. In this work we prepared close-packed hybrid monolayer of thiol capped CdSe and gold nanoparticles. They exhibit both the Quenching and enhancements the in PL emission.The systematic variance of PL from such hybrid nanomaterials monolayer is studied by tuning the Number ratio of Gold per Quantum dots, the surface density of QDs and the spectral overlap of emission spectrum of QD and absorption spectrum of Gold nanoparticles. Role of Localized surface Plasmon which not only leads to quenching but strong enhancements as well, is explored.

EFFICIENT QUANTUM RANDOM NUMBER GENERATION USING QUANTUM INDISTINGUISHABILITY

In this paper, we propose a quantum method for generation of random numbers based on bosonic stimulation. Randomness arises through the path-dependent indeterministic amplification of two competing bosonic modes. We show that the process provides an efficient method for macroscopic extraction of microscopic randomness.

Atomic Structure of Quantum Gold Nanowires: Quantification of the Lattice Strain

Theoretical studies exist to compute the atomic arrangement in gold nanowires and the influence on their electronic behavior with decreasing diameter. Experimental studies, e.g., by transmission electron microscopy, on chemically synthesized ultrafine wires are however lacking owing to the unavailability of suitable protocols for sample preparation and the stability of the wires under electron beam irradiation. In this work, we present an atomic scale structural investigation on quantum single crystalline gold nanowires of 2 nm diameter, chemically prepared on a carbon film grid. Using low dose aberration-corrected high resolution (S)TEM, we observe an inhomogeneous strain distribution in the crystal, largely concentrated at the twin boundaries and the surface along with the presence of facets and surface steps leading to a noncircular cross section of the wires. These structural aspects are critical inputs needed to determine their unique electronic character and their potential as a suitable catalyst material. Furthermore, electron-beam-induced structural changes at the atomic scale, having implications on their mechanical behavior and their suitability as interconnects, are discussed.

Improved photovoltaic performance of CdSe/CdS/PbS quantum dot sensitized ZnO nanorod array solar cell

Single crystalline zinc oxide (ZnO) nanorod array has been used for the fabrication of CdSe/CdS/PbS/ZnO quantum dot sensitized solar cell (QDSSC). The ZnO nanorod array photoanodes are sensitized with consecutive layer of PbS, CdS and CdSe quantum dots by employing simple successive ion layer adsorption and reaction (SILAR) and chemical bath deposition (CBD) techniques. The performances of the QDSSCs are examined in detail using polysulfide electrolyte with copper sulfide (CuS) counter electrode. The combination of two successive layers of PbS with CdSe/CdS/ZnO shows an improved short circuit current density (12.223 mA cm(-2)) with a maximum power to conversion efficiency of 2.352% under 1 sun illumination. This enhancement is mainly attributed due to the better light harvesting ability of the PbS quantum dots and make large accumulation of photo-injected electrons in the conduction band of ZnO, and CdSe/CdS layers lower the recombination of photo-injected electrons with the electrolyte, these are well evidenced with the photovoltaic studies and electrochemical impedance spectroscopy. (C) 2013 Elsevier B.V. All rights reserved.

Quantum chemical study on influence of intermolecular hydrogen bonding on the geometry, the atomic charges and the vibrational dynamics of 2,6-dichlorobenzonitrile

FT-IR (4000-400 cm(-1)) and FT-Raman (4000-200 cm(-1)) spectral measurements on solid 2,6-dichlorobenzonitrile (2,6-DCBN) have been done. The molecular geometry, harmonic vibrational frequencies and bonding features in the ground state have been calculated by density functional theory at the B3LYP/6-311++G (d,p) level. A comparison between the calculated and the experimental results covering the molecular structure has been made. The assignments of the fundamental vibrational modes have been done on the basis of the potential energy distribution (PED). To investigate the influence of intermolecular hydrogen bonding on the geometry, the charge distribution and the vibrational spectrum of 2,6-DCBN; calculations have been done for the monomer as well as the tetramer. The intermolecular interaction energies corrected for basis set superposition error (BSSE) have been calculated using counterpoise method. Based on these results, the correlations between the vibrational modes and the structure of the tetramer have been discussed. Molecular electrostatic potential (MEP) contour map has been plotted in order to predict how different geometries could interact. The Natural Bond Orbital (NBO) analysis has been done for the chemical interpretation of hyperconjugative interactions and electron density transfer between occupied (bonding or lone pair) orbitals to unoccupied (antibonding or Rydberg) orbitals. UV spectrum was measured in methanol solution. The energies and oscillator strengths were calculated by Time Dependent Density Functional Theory (TD-DFT) and matched to the experimental findings. TD-DFT method has also been used for theoretically studying the hydrogen bonding dynamics by monitoring the spectral shifts of some characteristic vibrational modes involved in the formation of hydrogen bonds in the ground and the first excited state. The C-13 nuclear magnetic resonance (NMR) chemical shifts of the molecule were calculated by the Gauge independent atomic orbital (GIAO) method and compared with experimental results. Standard thermodynamic functions have been obtained and changes in thermodynamic properties on going from monomer to tetramer have been presented. (C) 2013 Elsevier B.V. All rights reserved.

Nonlinear optical second harmonic generation in ZnS quantum dots and observation on optical properties of ZnS/PMMA nanocomposites

ZnS quantum dots (QDs) of different sizes are synthesized by a simple chemical co-precipitation method at room temperature, by varying pH value of the reaction mixture. Samples are characterized by an X-ray diffractometer, transmission electron microscope, energy-dispersive X-ray analysis, etc. Linear optical properties, including UV-visible absorption and photoluminescence emission characteristics, of as-prepared QDs are measured. Size dependent nonlinear optical property, such as second harmonic generation (SHG) of 1064 nm Nd:YAG laser fundamental radiation in the synthesized ZnS QDs, is reported for the first time, to the best of our knowledge, by using the standard Kurtz-Perry powder method. In not to study the possibility of the synthesized ZnS QDs in different device applications ZnS/PMMA (polymethylmethacrylate) nanocomposites are also synthesized. The presence of weak chemical interaction between the polymer matrix and ZnS QDs is confirmed by Fourier transform infrared spectroscopy. Thermal properties of the nanocomposites are studied by differential scanning calorimetry and thermo-gravimetric analysis techniques, which show that the composites are stable up to similar to 300 degrees C temperature. (C) 2013 Elsevier B.V. All rights reserved.

Electrostatic modulation of periodic potentials in a two-dimensional electron gas: from antidot lattice to quantum dot lattice

We use a dual gated device structure to introduce a gate-tuneable periodic potential in a GaAs/AlGaAs two dimensional electron gas (2DEG). Using only a suitable choice of gate voltages we can controllably alter the potential landscape of the bare 2DEG, inducing either a periodic array of antidots or quantum dots. Antidots are artificial scattering centers, and therefore allow for a study of electron dynamics. In particular, we show that the thermovoltage of an antidot lattice is particularly sensitive to the relative positions of the Fermi level and the antidot potential. A quantum dot lattice, on the other hand, provides the opportunity to study correlated electron physics. We find that its current-voltage characteristics display a voltage threshold, as well as a power law scaling, indicative of collective Coulomb blockade in a disordered background.

Modulation of glyceraldehyde-3-phosphate dehydrogenase activity by surface functionalized quantum dots

Enzymatic regulation is a fast and reliable diagnosis tool via identification and design of inhibitors for modulation of enzyme function. Previous reports on quantum dots (QDs)-enzyme interactions reveal a protein-surface recognition ability leading to promising applications in protein stabilization, protein delivery, bio-sensing and detection. However, the direct use of QDs to control enzyme inhibition has never been revealed to date. Here we show that a series of biocompatible surface-functionalized metal-chalcogenide QDs can be used as potent inhibitors for malignant cells through the modulation of enzyme activity, while normal cells remain unaffected. The in vitro activity of glyceraldehyde-3-phosphate dehydrogenase (GAPDH), an enzyme involved critically in the glycolysis of cancer cells, is inactivated selectively in a controlled way by the QDs at a significantly low concentration (nM). Cumulative kinetic studies delineate that the QDs undergo both reversible and irreversible inhibition mechanisms owing to the site-specific interactions, enabling control over the inhibition kinetics. These complementary loss-of-function probes may offer a novel route for rapid clinical diagnosis of malignant cells and biomedical applications.

Reentrant Superspin Glass Phase in a La0.82Ca0.18MnO3 Ferromagnetic Insulator

We report results of the magnetization and ac susceptibility measurements down to very low fields on a single crystal of the perovskite manganite, La-0.82 Ca-0.18 MnO3. This composition falls in the intriguing ferromagnetic insulator region of the manganite phase diagram. In contrast to earlier beliefs, our investigations reveal that magnetically (and in every other sense), this is a single- phase system with a ferromagnetic ordering temperature of around 170 K. However, this ferromagnetic state is magnetically frustrated, and the system exhibits pronounced glassy dynamics below 90 K. Based on measured dynamical properties, we propose that this quasi-long-ranged ferromagnetic phase, and the associated superspin glass behavior, is the true magnetic state of the system, rather than being a macroscopic mixture of ferromagnetic and antiferromagnetic phases, as often suggested. Our results provide an understanding of the quantum phase transition from an antiferromagnetic insulator to a ferromagnetic metal via this ferromagnetic state as a function of x in La1-xCaxMnO3, in terms of the possible formation of magnetic polarons.

Counterfactual quantum certificate authorization

We present a multipartite protocol in a counterfactual paradigm. In counterfactual quantum cryptography, secure information is transmitted between two spatially separated parties even when there is no physical travel of particles transferring the information between them. We propose here a tripartite counterfactual quantum protocol for the task of certificate authorization. Here a trusted third party, Alice, authenticates an entity Bob (e.g., a bank) that a client Charlie wishes to securely transact with. The protocol is counterfactual with respect to either Bob or Charlie. We prove its security against a general incoherent attack, where Eve attacks single particles.

Quantum-Confined ZnO Nanoshell Photoanodes for Mesoscopic Solar Cells

We present a photoanode for dye-sensitized solar cell (DSC) based on ZnO nanoshell deposited by atomic layer deposition at 150 degrees C on a mesoporous insulating template. An ultrathin layer of ZnO between. 3 and 6 nm, which exhibits quantum confinement effect, is found to be sufficient to transport the photogenerated electrons to the external contacts and exhibits near-unity collection efficiency. A 6 nm ZnO nanoshell on a 2.5 mu m mesoporous nanoparticle Al2O3 template yields photovoltaic power conversion efficiency (PCE) of 4.2% in liquid DSC. Perovskite absorber (CH3NH3PbI3) based solid state solar cells made with similar ZnO nanostructures lead to a high PCE of 7%.