Magnetic properties of single-crystalline CeCuGa3

The magnetic behavior of single-crystalline CeCuGa3 has been investigated. The compound forms in a tetragonal BaAl4-type structure consisting of rare-earth planes separated by Cu-Ga layers. If the Cu-Ga site disorder is reduced, CeCuGa3 adopts the related, likewise tetragonal BaNiSn3-type structure, in which the Ce ion are surrounded by different Cu and Ga layers and the inversion symmetry is lost. In the literature conflicting reports about the magnetic order of CeCuGa3 have been published. Single crystals with the centrosymmetric structure variant exhibit ferromagnetic order below approx. 4 K with a strong planar anisotropy. The magnetic behavior above the transition temperature can be well understood by the crystal-field splitting of the 4f Hund's rule ground-state multiplet of the Ce ions

Finite-Temperature Transition in the Spin-Dimer Antiferromagnet BaCuSi2O6

We consider a classical XY-like Hamiltonian on a body-centered tetragonal lattice, focusing on the role of interlayer frustration. A three-dimensional (3D) ordered phase is realized via thermal fluctuations, breaking the mirror-image reflection symmetry in addition to the XY symmetry. A heuristic field-theoretical model of the transition has a decoupled fixed point in the 3D XY universality, and our Monte Carlo simulation suggests that there is such a temperature region where long-wavelength fluctuations can be described by this fixed point. However, it is shown using scaling arguments that the decoupled fixed point is unstable against a fluctuation-induced biquadratic interaction, indicating that a crossover to nontrivial critical phenomena with different exponents appears as one approaches the critical point beyond the transient temperature region. This new scenario clearly contradicts the previous notion of the 3D XY universality.Comment: 16 pages, 7 figure

Structural Phase Transition in the 2D Spin Dimer Compound SrCu2(BO3)2

A displacive, 2nd order structural phase transition at Ts=395 K from space group I`4 2 m below Ts to I 4/m c m above Ts has been discovered in the two-dimensional spin dimer compound SrCu2(BO3)2. The temperature evolution of the structure in both phases has been studied by X-ray diffraction and Raman scattering, supplemented by differential scanning calorimetry and SQUID magnetometry. The implications of this transition and of the observed phonon anomalies in Raman scattering for spin-phonon and interlayer coupling in this quantum spin system will be discussed.Comment: 13pages, 13 figure

X-Band ESR Determination of Dzyaloshinsky-Moriya Interaction in 2D SrCu2_2(BO3_3)2_2 System

X-band ESR measurements on a single crystal of SrCu$_2$(BO$_3$)$_2$ system in a temperature range between 10 K and 580 K are presented. The temperature and angular dependence of unusually broad ESR spectra can be explained by the inclusion of antisymmetric Dzyaloshinsky-Moriya (DM) interaction, which yields by far the largest contribution to the linewidth. However, the well-accepted picture of only out-of-plane interdimer DM vectors is not sufficient for explanation of the observed angular dependence. In order to account for the experimental linewidth anisotropy we had to include sizable in-plane components of interdimer as well as intradimer DM interaction in addition to the out-of-plane interdimer one. The nearest-neighbor DM vectors lie perpendicular to crystal anisotropy c-axis due to crystal symmetry. We also emphasize that above the structural phase transition occurring at 395 K dynamical mechanism should be present allowing for instantaneous DM interactions. Moreover, the linewidth at an arbitrary temperature can be divided into two contributions; namely, the first part arising from spin dynamics governed by the spin Hamiltonian of the system and the second part due to significant spin-phonon coupling. The nature of the latter mechanism is attributed to phonon-modulation of the antisymmetric interaction, which is responsible for the observed linear increase of the linewidth at high temperatures.Comment: 17 pages, 4 figures, submitted to PR

Prefrontal cortex output circuits guide reward seeking through divergent cue encoding

The prefrontal cortex is a critical neuroanatomical hub for controlling motivated behaviours across mammalian species. In addition to intra-cortical connectivity, prefrontal projection neurons innervate subcortical structures that contribute to reward-seeking behaviours, such as the ventral striatum and midline thalamus. While connectivity among these structures contributes to appetitive behaviours, how projection-specific prefrontal neurons encode reward-relevant information to guide reward seeking is unknown. Here we use in vivo two-photon calcium imaging to monitor the activity of dorsomedial prefrontal neurons in mice during an appetitive Pavlovian conditioning task. At the population level, these neurons display diverse activity patterns during the presentation of reward-predictive cues. However, recordings from prefrontal neurons with resolved projection targets reveal that individual corticostriatal neurons show response tuning to reward-predictive cues, such that excitatory cue responses are amplified across learning. By contrast, corticothalamic neurons gradually develop new, primarily inhibitory responses to reward-predictive cues across learning. Furthermore, bidirectional optogenetic manipulation of these neurons reveals that stimulation of corticostriatal neurons promotes conditioned reward-seeking behaviour after learning, while activity in corticothalamic neurons suppresses both the acquisition and expression of conditioned reward seeking. These data show how prefrontal circuitry can dynamically control reward-seeking behaviour through the opposing activities of projection-specific cell populations

Accurate Treatment of Large Supramolecular Complexes by Double-Hybrid Density Functionals Coupled with Nonlocal van der Waals Corrections

In this work, we present a thorough assessment of the performance of some representative double-hybrid density functionals (revPBE0-DH-NL and B2PLYP-NL) as well as their parent hybrid and GGA counterparts, in combination with the most modern version of the nonlocal (NL) van der Waals correction to describe very large weakly interacting molecular systems dominated by noncovalent interactions. Prior to the assessment, an accurate and homogeneous set of reference interaction energies was computed for the supramolecular complexes constituting the L7 and S12L data sets by using the novel, precise, and efficient DLPNO-CCSD(T) method at the complete basis set limit (CBS). The correction of the basis set superposition error and the inclusion of the deformation energies (for the S12L set) have been crucial for obtaining precise DLPNO-CCSD(T)/CBS interaction energies. Among the density functionals evaluated, the double-hybrid revPBE0-DH-NL and B2PLYP-NL with the three-body dispersion correction provide remarkably accurate association energies very close to the chemical accuracy. Overall, the NL van der Waals approach combined with proper density functionals can be seen as an accurate and affordable computational tool for the modeling of large weakly bonded supramolecular systems.Financial support by the “Ministerio de Economía y Competitividad” (MINECO) of Spain and European FEDER funds through projects CTQ2011-27253 and CTQ2012-31914 is acknowledged. The support of the Generalitat Valenciana (Prometeo/2012/053) is also acknowledged. J.A. thanks the EU for the FP7-PEOPLE-2012-IEF-329513 grant. J.C. acknowledges the “Ministerio de Educación, Cultura y Deporte” (MECD) of Spain for a predoctoral FPU grant

Urocortin-1 within the Centrally-Projecting Edinger-Westphal Nucleus Is Critical for Ethanol Preference

Converging lines of evidence point to the involvement of neurons of the centrally projecting Edinger-Westphal nucleus (EWcp) containing the neuropeptide Urocortin-1 (Ucn1) in excessive ethanol (EtOH) intake and EtOH sensitivity. Here, we expanded these previous findings by using a continuous-access, two-bottle choice drinking paradigm (3%, 6%, and 10% EtOH vs. tap water) to compare EtOH intake and EtOH preference in Ucn1 genetic knockout (KO) and wild-type (WT) mice. Based on previous studies demonstrating that electrolytic lesion of the EWcp attenuated EtOH intake and preference in high-drinking C57BL/6J mice, we also set out to determine whether EWcp lesion would differentially alter EtOH consumption in Ucn1 KO and WT mice. Finally, we implemented well-established place conditioning procedures in KO and WT mice to determine whether Ucn1 and the corticotropin-releasing factor type-2 receptor (CRF-R2) were involved in the rewarding and aversive effects of EtOH (2 g/kg, i.p.). Results from these studies revealed that (1) genetic deletion of Ucn1 dampened EtOH preference only in mice with an intact EWcp, but not in mice that received lesion of the EWcp, (2) lesion of the EWcp dampened EtOH intake in Ucn1 KO and WT mice, but dampened EtOH preference only in WT mice expressing Ucn1, and (3) genetic deletion of Ucn1 or CRF-R2 abolished the conditioned rewarding effects of EtOH, but deletion of Ucn1 had no effect on the conditioned aversive effects of EtOH. The current findings provide strong support for the hypothesis that EWcp-Ucn1 neurons play an important role in EtOH intake, preference, and reward

Resolving the neural circuits of anxiety

Although anxiety disorders represent a major societal problem demanding new therapeutic targets, these efforts have languished in the absence of a mechanistic understanding of this subjective emotional state. While it is impossible to know with certainty the subjective experience of a rodent, rodent models hold promise in dissecting well-conserved limbic circuits. The application of modern approaches in neuroscience has already begun to unmask the neural circuit intricacies underlying anxiety by allowing direct examination of hypotheses drawn from existing psychological concepts. This information points toward an updated conceptual model for what neural circuit perturbations could give rise to pathological anxiety and thereby provides a roadmap for future therapeutic development.National Institute of Diabetes and Digestive and Kidney Diseases (U.S.) (NIH Director’s New Innovator Award DP2-DK-102256-01)National Institute of Mental Health (U.S.) (NIH) R01-MH102441-01)JPB Foundatio

Computational Treatment of Metalloproteins

Metalloproteins present a considerable challenge for modeling, especially when the starting point is far from thermodynamic equilibrium. Examples include formidable problems such as metalloprotein folding and structure prediction upon metal addition, removal, or even just replacement; metalloenzyme design, where stabilization of a transition state of the catalyzed reaction in the specific binding pocket around the metal needs to be achieved; docking to metal-containing sites and design of metalloenzyme inhibitors. Even more conservative computations, such as elucidations of the mechanisms and energetics of the reaction catalyzed by natural metalloenzymes, are often nontrivial. The reason is the vast span of time and length scales over which these proteins operate, and thus the resultant difficulties in estimating their energies and free energies. It is required to perform extensive sampling, properly treat the electronic structure of the bound metal or metals, and seamlessly merge the required techniques to assess energies and entropies, or their changes, for the entire system. Additionally, the machinery needs to be computationally affordable. Although a great advancement has been made over the years, including some of the seminal works resulting in the 2013 Nobel Prize in chemistry, many aforementioned exciting applications remain far from reach. We review the methodology on the forefront of the field, including several promising methods developed in our lab that bring us closer to the desired modern goals. We further highlight their performance by a few examples of applications