Full counting statistics for transport through a molecular quantum dot magnet

Full counting statistics (FCS) for the transport through a molecular quantum dot magnet is studied theoretically in the incoherent tunneling regime. We consider a model describing a single-level quantum dot, magnetically coupled to an additional local spin, the latter representing the total molecular spin s. We also assume that the system is in the strong Coulomb blockade regime, i.e., double occupancy on the dot is forbidden. The master equation approach to FCS introduced in Ref. [12] is applied to derive a generating function yielding the FCS of charge and current. In the master equation approach, Clebsch-Gordan coefficients appear in the transition probabilities, whereas the derivation of generating function reduces to solving the eigenvalue problem of a modified master equation with counting fields. To be more specific, one needs only the eigenstate which collapses smoothly to the zero-eigenvalue stationary state in the limit of vanishing counting fields. We discovered that in our problem with arbitrary spin s, some quartic relations among Clebsch-Gordan coefficients allow us to identify the desired eigenspace without solving the whole problem. Thus we find analytically the FCS generating function in the following two cases: i) both spin sectors lying in the bias window, ii) only one of such spin sectors lying in the bias window. Based on the obtained analytic expressions, we also developed a numerical analysis in order to perform a similar contour-plot of the joint charge-current distribution function, which have recently been introduced in Ref. [13], here in the case of molecular quantum dot magnet problem.Comment: 17 pages, 5 figure

Nonequilibrium Kondo Effect in a Quantum Dot Coupled to Ferromagnetic Leads

We study the Kondo effect in the electron transport through a quantum dot coupled to ferromagnetic leads, using a real-time diagrammatic technique which provides a systematic description of the nonequilibrium dynamics of a system with strong local electron correlations. We evaluate the theory in an extension of the `resonant tunneling approximation', introduced earlier, by introducing the self-energy of the off-diagonal component of the reduced propagator in spin space. In this way we develop a charge and spin conserving approximation that accounts not only for Kondo correlations but also for the spin splitting and spin accumulation out of equilibrium. We show that the Kondo resonances, split by the applied bias voltage, may be spin polarized. A left-right asymmetry in the coupling strength and/or spin polarization of the electrodes significantly affects both the spin accumulation and the weight of the split Kondo resonances out of equilibrium. The effects are observable in the nonlinear differential conductance. We also discuss the influence of decoherence on the Kondo resonance in the frame of the real-time formulation.Comment: 13 pages, 13 figure

Structure-Free Validation of Residual Dipolar Coupling and Paramagnetic Relaxation Enhancement Measurements of Disordered Proteins.

Residual dipolar couplings (RDCs) and paramagnetic relaxation enhancements (PREs) have emerged as valuable parameters for defining the structures and dynamics of disordered proteins by nuclear magnetic resonance (NMR) spectroscopy. Procedures for their measurement, however, may lead to conformational perturbations because of the presence of the alignment media necessary for recording RDCs, or of the paramagnetic groups that must be introduced for measuring PREs. We discuss here experimental methods for quantifying these effects by considering the case of the 40-residue isoform of the amyloid β peptide (Aβ40), which is associated with Alzheimer's disease. By conducting RDC measurements over a range of concentrations of certain alignment media, we show that perturbations arising from transient binding of Aβ40 can be characterized, allowing appropriate corrections to be made. In addition, by using NMR experiments sensitive to long-range interactions, we show that it is possible to identify relatively nonperturbing sites for attaching nitroxide radicals for PRE measurements. Thus, minimizing the conformational perturbations introduced by RDC and PRE measurements should facilitate their use for the rigorous determination of the conformational properties of disordered proteins.This is the author accepted manuscript. The final version is available from ACS via http://dx.doi.org/10.1021/acs.biochem.5b0067

Correlation effects and the high-frequency spin susceptibility of an electron liquid: Exact limits

Spin correlations in an interacting electron liquid are studied in the high-frequency limit and in both two and three dimensions. The third-moment sum rule is evaluated and used to derive exact limiting forms (at both long- and short-wavelengths) for the spin-antisymmetric local-field factor, $\lim_{\omega \to \infty}G_-({\bf q, \omega})$. In two dimensions $\lim_{\omega \to \infty}G_-({\bf q, \omega})$ is found to diverge as $1/q$ at long wavelengths, and the spin-antisymmetric exchange-correlation kernel of time-dependent spin density functional theory diverges as $1/q^2$ in both two and three dimensions. These signal a failure of the local-density approximation, one that can be redressed by alternative approaches.Comment: 5 page

Pressure evolution of electronic and crystal structure of non-centrosymmetric EuCoGe3_3

We report on the pressure evolution of the electronic and crystal structures of the noncentrosymmetric antiferromagnet EuCoGe3. Using a diamond anvil cell, we performed high pressure fluorescence detected near-edge x-ray absorption spectroscopy at the Eu L3, Co K, and Ge K edges and synchrotron powder x-ray diffraction. In the Eu L3 spectrum, both divalent and trivalent Eu peaks are observed from the lowest pressure measurement (~2 GPa). By increasing pressure, the relative intensity of the trivalent Eu peak increases, and an average Eu valence continuously increases from 2.2 at 2 GPa to 2.31 at~50 GPa. On the other hand, no discernible changes are observed in the Co K and Ge K spectra as a function of pressure. With the increase in pressure, lattice parameters continuously decrease without changing I4mm symmetry. Our study revealed a robust divalent Eu state and an unchanged crystal symmetry of EuCoGe3 against pressure.Comment: Accepted in PRB https://journals.aps.org/prb/accepted/b2073O6fL9e1ca40307905b1de5bf05de12d8fc1

Purification, crystallization and preliminary crystallographic analysis of soybean mature glycinin A1bB2.

Glycinin is one of the most abundant storage-protein molecules in soybean seeds and is composed of five subunits (A1aB1b, A1bB2, A2B1a, A3B4 and A5A4B3). A1bB2 was purified from a mutant soybean cultivar containing glycinin composed of only A5A4B3 and A1bB2. At 281 K the protein formed hexagonal, rectangular and rod-shaped crystals in the first [0.1 M imidazole pH 8.0, 0.2 M MgCl2, 35%(v/v) MPD], second [0.1 M sodium citrate pH 5.6, 0.2 M ammonium acetate, 30%(v/v) MPD] and third (0.1 M phosphate-citrate pH 4.2, 2.0 M ammonium sulfate) crystallization conditions, respectively. X-ray diffraction data were collected to resolutions of 1.85, 1.85 and 2.5 Å from crystals of the three different shapes. The crystals belonged to space groups P6322, P21 and P1, with unit-cell parameters a = b = 143.60, c = 84.54 Å, a = 114.54, b = 105.82, c = 116.67 Å, β = 94.99° and a = 94.45, b = 94.96, c = 100.66 Å, α = 107.02, β = 108.44, γ = 110.71°, respectively. One, six and six subunits of A1bB2 were estimated to be present in the respective asymmetric units. The three-dimensional structure of the A1bB2 hexamer is currently being determined

The Kr85 s-process Branching and the Mass of Carbon Stars

We present new spectroscopic observations for a sample of C(N)-type red giants. These objects belong to the class of Asymptotic Giant Branch stars, experiencing thermal instabilities in the He-burning shell (thermal pulses). Mixing episodes called third dredge-up enrich the photosphere with newly synthesized C12 in the He-rich zone, and this is the source of the high observed ratio between carbon and oxygen (C/O > 1 by number). Our spectroscopic abundance estimates confirm that, in agreement with the general understanding of the late evolutionary stages of low and intermediate mass stars, carbon enrichment is accompanied by the appearance of s-process elements in the photosphere. We discuss the details of the observations and of the derived abundances, focusing in particular on rubidium, a neutron-density sensitive element, and on the s-elements Sr, Y and Zr belonging to the first s-peak. The critical reaction branching at Kr85, which determines the relative enrichment of the studied species, is discussed. Subsequently, we compare our data with recent models for s-processing in Thermally Pulsing Asymptotic Giant Branch stars, at metallicities relevant for our sample. A remarkable agreement between model predictions and observations is found. Thanks to the different neutron density prevailing in low and intermediate mass stars, comparison with the models allows us to conclude that most C(N) stars are of low mass (M < 3Mo). We also analyze the C12/C13 ratios measured, showing that most of them cannot be explained by canonical stellar models. We discuss how this fact would require the operation of an ad hoc additional mixing, currently called Cool Bottom Process, operating only in low mass stars during the first ascent of the red giant branch and, perhaps, also during the asymptotic giant branch.Comment: 54 pages + 6 figures + 6 tables. ApJ accepte

Ultrafast charge transfer processes accompanying KLL Auger decay in aqueous KCl solution

X-ray photoelectron spectroscopy (XPS) and KLL Auger spectra of aqueous KCl solution were measured for the K$^+$ and Cl$^-$ edges. While the XPS spectra of potassium and chloride have similar structures, both exhibiting only weak satellite structures near the main line, the Auger spectra of these isoelectronic ions differ dramatically. A very strong satellite peak was found in the K$^+$ KLL Auger spectrum at the low kinetic energy side of the $^1$D state. Using equivalent core models and ab initio calculations this spectral structure was assigned to electron transfer processes from solvent water molecules to the solvated K$^+$ cation. Contrary to the potassium case, no extra peak was found in the KLL Auger spectrum of solvated Cl$^-$ indicating on a strong dependence of the underlying processes on ionic charge. The observed charge transfer processes are suggested to play an important role in charge redistribution following single and multiple core-hole creation in atomic and molecular systems placed into an environment