A Joint Venture of Ab Initio Molecular Dynamics, Coupled Cluster Electronic Structure Methods, and Liquid-State Theory to Compute Accurate Isotropic Hyperfine Constants of Nitroxide Probes in Water

The isotropic hyperfine coupling constant (HFCC, Aiso) of a pH-sensitive spin probe in a solution, HMI (2,2,3,4,5,5-hexamethylimidazolidin-1-oxyl, C9H19N2O) in water, is computed using an ensemble of state-of-the-art computational techniques and is gauged against X-band continuous wave electron paramagnetic resonance (EPR) measurement spectra at room temperature. Fundamentally, the investigation aims to delineate the cutting edge of current first-principles-based calculations of EPR parameters in aqueous solutions based on using rigorous statistical mechanics combined with correlated electronic structure techniques. In particular, the impact of solvation is described by exploiting fully atomistic, RISM integral equation, and implicit solvation approaches as offered by ab initio molecular dynamics (AIMD) of the periodic bulk solution (using the spin-polarized revPBE0-D3 hybrid functional), embedded cluster reference interaction site model integral equation theory (EC-RISM), and polarizable continuum embedding (using CPCM) of microsolvated complexes, respectively. HFCCs are obtained from efficient coupled cluster calculations (using open-shell DLPNO-CCSD theory) as well as from hybrid density functional theory (using revPBE0-D3). Re-solvation of “vertically desolvated” spin probe configuration snapshots by EC-RISM embedding is shown to provide significantly improved results compared to CPCM since only the former captures the inherent structural heterogeneity of the solvent close to the spin probe. The average values of the Aiso parameter obtained based on configurational statistics using explicit water within AIMD and from EC-RISM solvation are found to be satisfactorily close. Using either such explicit or RISM solvation in conjunction with DLPNO-CCSD calculations of the HFCCs provides an average Aiso parameter for HMI in aqueous solution at 300 K and 1 bar that is in good agreement with the experimentally determined one. The developed computational strategy is general in the sense that it can be readily applied to other spin probes of similar molecular complexity, to aqueous solutions beyond ambient conditions, as well as to other solvents in the longer run

Phase diagrams of classical spin fluids: the influence of an external magnetic field on the liquid-gas transition

The influence of an external magnetic field on the liquid-gas phase transition in Ising, XY, and Heisenberg spin fluid models is studied using a modified mean field theory and Gibbs ensemble Monte Carlo simulations. It is demonstrated that the theory is able to reproduce quantitatively all characteristic features of the field dependence of the critical temperature T_c(H) for all the three models. These features include a monotonic decrease of T_c with rising H in the case of the Ising fluid as well as a more complicated nonmonotonic behavior for the XY and Heisenberg models. The nonmonotonicity consists in a decrease of T_c with increasing H at weak external fields, an increase of T_c with rising H in the strong field regime, and the existence of a minimum in T_c(H) at intermediate values of H. Analytical expressions for T_c(H) in the large field limit are presented as well. The magnetic para-ferro phase transition is also considered in simulations and described within the mean field theory.Comment: 14 pages, 12 figures (to be submitted to Phys. Rev. E

The Structure of IR Luminous Galaxies at 100 Microns

We have observed twenty two galaxies at 100 microns with the Kuiper Airborne Observatory in order to determine the size of their FIR emitting regions. Most of these galaxies are luminous far-infrared sources, with L_FIR > 10^11 L_sun. This data constitutes the highest spatial resolution ever achieved on luminous galaxies in the far infrared. Our data includes direct measurements of the spatial structure of the sources, in which we look for departures from point source profiles. Additionally, comparison of our small beam 100 micron fluxes with the large beam IRAS fluxes shows how much flux falls beyond our detectors but within the IRAS beam. Several sources with point- like cores show evidence for such a net flux deficit. We clearly resolved six of these galaxies at 100 microns and have some evidence for extension in seven others. Those galaxies which we have resolved can have little of their 100 micron flux directly emitted by a point-like active galactic nucleus (AGN). Dust heated to ~40 K by recent bursts of non-nuclear star formation provides the best explanation for their extreme FIR luminosity. In a few cases, heating of an extended region by a compact central source is also a plausible option. Assuming the FIR emission we see is from dust, we also use the sizes we derive to find the dust temperatures and optical depths at 100 microns which we translate into an effective visual extinction through the galaxy. Our work shows that studies of the far infrared structure of luminous infrared galaxies is clearly within the capabilities of new generation far infrared instrumentation, such as SOFIA and SIRTF.Comment: 8 tables, 23 figure

Low frequency 1/f noise in doped manganite grain-boundary junctions

We have performed a systematic analysis of the low frequency 1/f-noise in single grain boundary junctions in the colossal magnetoresistance material La_{2/3}Ca_{1/3}MnO_{3-delta}. The grain boundary junctions were formed in epitaxial La_{2/3}Ca_{1/3}MnO_{3-delta} films deposited on SrTiO_3 bicrystal substrates and show a large tunneling magnetoresistance of up to 300% at 4.2 K as well as ideal, rectangular shaped resistance versus applied magnetic field curves. Below the Curie temperature T_C the measured 1/f noise is dominated by the grain boundary. The dependence of the noise on bias current, temperature and applied magnetic field gives clear evidence that the large amount of low frequency noise is caused by localized sites with fluctuating magnetic moments in a heavily disordered grain boundary region. At 4.2 K additional temporally unstable Lorentzian components show up in the noise spectra that are most likely caused by fluctuating clusters of interacting magnetic moments. Noise due to fluctuating domains in the junction electrodes is found to play no significant role.Comment: 9 pages, 7 figure

Deafening silence? Marxism, international historical sociology and the spectre of Eurocentrism

Approaching the centenary of its establishment as a formal discipline, International Relations today challenges the ahistorical and aspatial frameworks advanced by the theories of earlier luminaries. Yet, despite a burgeoning body of literature built on the transdisciplinary efforts bridging International Relations and its long-separated nomothetic relatives, the new and emerging conceptual frameworks have not been able to effectively overcome the challenge posed by the ‘non-West’. The recent wave of international historical sociology has highlighted possible trajectories to problematise the myopic and unipolar conceptions of the international system; however, the question of Eurocentrism still lingers in the developing research programmes. This article interjects into the ongoing historical materialist debate in international historical sociology by: (1) conceptually and empirically challenging the rigid boundaries of the extant approaches; and (2) critically assessing the postulations of recent theorising on ‘the international’, capitalist states-system/geopolitics and uneven and combined development. While the significance of the present contributions in international historical sociology should not be understated, it is argued that the ‘Eurocentric cage’ still occupies a dominant ontological position which essentially silences ‘connected histories’ and conceals the role of inter-societal relations in the making of the modern states-system and capitalist geopolitics

Josephson array of mesoscopic objects. Modulation of system properties through the chemical potential

The phase diagram of a two-dimensional Josephson array of mesoscopic objects is examined. Quantum fluctuations in both the modulus and phase of the superconducting order parameter are taken into account within a lattice boson Hubbard model. Modulating the average occupation number $n_0$ of the sites in the system leads to changes in the state of the array, and the character of these changes depends significantly on the region of the phase diagram being examined. In the region where there are large quantum fluctuations in the phase of the superconducting order parameter, variation of the chemical potential causes oscillations with alternating superconducting (superfluid) and normal states of the array. On the other hand, in the region where the bosons interact weakly, the properties of the system depend monotonically on $n_0$. Lowering the temperature and increasing the particle interaction force lead to a reduction in the width of the region of variation in $n_0$ within which the system properties depend weakly on the average occupation number. The phase diagram of the array is obtained by mapping this quantum system onto a classical two-dimensional XY model with a renormalized Josephson coupling constant and is consistent with our quantum Path-Integral Monte Carlo calculations.Comment: 12 pages, 8 Postscript figure

Drivers and outcomes of work alienation: reviving a concept

This article sheds new light on an understudied construct in mainstream management theory, namely, work alienation. This is an important area of study because previous research indicates that work alienation is associated with important individual and organizational outcomes. We tested four antecedents of work alienation: decision-making autonomy, task variety, task identity, and social support. Moreover, we examined two outcomes of alienation: deviance and performance, the former measured 1 year after the independent variables were measured, and the latter as rated by supervisors. We present evidence from a sample of 283 employees employed at a construction and consultancy organization in the United Kingdom. The results supported the majority of our hypotheses, indicating that alienation is a worthy concept of exploration in the management sciences

Quantum Computation by Communication

We present a new approach to scalable quantum computing--a ``qubus computer''--which realises qubit measurement and quantum gates through interacting qubits with a quantum communication bus mode. The qubits could be ``static'' matter qubits or ``flying'' optical qubits, but the scheme we focus on here is particularly suited to matter qubits. There is no requirement for direct interaction between the qubits. Universal two-qubit quantum gates may be effected by schemes which involve measurement of the bus mode, or by schemes where the bus disentangles automatically and no measurement is needed. In effect, the approach integrates together qubit degrees of freedom for computation with quantum continuous variables for communication and interaction.Comment: final published versio

Beyond the Jaynes-Cummings model: circuit QED in the ultrastrong coupling regime

In cavity quantum electrodynamics (QED), light-matter interaction is probed at its most fundamental level, where individual atoms are coupled to single photons stored in three-dimensional cavities. This unique possibility to experimentally explore the foundations of quantum physics has greatly evolved with the advent of circuit QED, where on-chip superconducting qubits and oscillators play the roles of two-level atoms and cavities, respectively. In the strong coupling limit, atom and cavity can exchange a photon frequently before coherence is lost. This important regime has been reached both in cavity and circuit QED, but the design flexibility and engineering potential of the latter allowed for increasing the ratio between the atom-cavity coupling rate and the cavity transition frequency above the percent level. While these experiments are well described by the renowned Jaynes-Cummings model, novel physics is expected in the ultrastrong coupling limit. Here, we report on the first experimental realization of a superconducting circuit QED system in the ultrastrong coupling limit and present direct evidence for the breakdown of the Jaynes-Cummings model.Comment: 5 pages, 3 figure

Control of microwave signals using circuit nano-electromechanics

Waveguide resonators are crucial elements in sensitive astrophysical detectors [1] and circuit quantum electrodynamics (cQED) [2]. Coupled to artificial atoms in the form of superconducting qubits [3, 4], they now provide a technologically promising and scalable platform for quantum information processing tasks [2, 5-8]. Coupling these circuits, in situ, to other quantum systems, such as molecules [9, 10], spin ensembles [11, 12], quantum dots [13] or mechanical oscillators [14, 15] has been explored to realize hybrid systems with extended functionality. Here, we couple a superconducting coplanar waveguide resonator to a nano-coshmechanical oscillator, and demonstrate all-microwave field controlled slowing, advancing and switching of microwave signals. This is enabled by utilizing electromechanically induced transparency [16-18], an effect analogous to electromagnetically induced transparency (EIT) in atomic physics [19]. The exquisite temporal control gained over this phenomenon provides a route towards realizing advanced protocols for storage of both classical and quantum microwave signals [20-22], extending the toolbox of control techniques of the microwave field.Comment: 9 figure