Fronts and stationary domains during electrochemical H2 oxidation on Pt: The impact of the position of the reference electrode on the spatiotemporal behaviour

We studied the local potential distribution in front of a rotating Pt ring-electrode during hydrogen oxidation in sulfuric acid for three different positions of the reference electrode. The potential distribution was measured with a potential micro-probe. The experiments were carried out in the bistable region of the system. For large and medium distances between the reference (RE) and the working electrode (WE), transitions between the two homogeneous states occurred through nucleation and growth of the globally stable state from the initially metastable one. The transition time was considerably longer for the intermediate distance between the RE and the WE. For the closest distance used, stationary patterns formed, consisting of two domains with high and low current densities, respectively. The difference in the double layer potential of the two domains amounted to more than 1 V. The low-current density domain was covered with Pt-O whereas in the high current density domain the electrode surface consisted of 'bare' Pt. The existence of these stationary non-equilibrium structures as well as the difference of the front behaviour for the other two electrode arrangements can be traced back to the existence of a negative global coupling for intermediate and close distances between the WE and the RE

Quasiparticle Interactions for f2^2-Impurity Anderson Model with Crystalline-Electric-Field: Numerical Renormalization Group Study

The aspect of the quasiparticle interaction of a local Fermi liquid, the impurity version of f$^2$-based heavy fermions, is studied by the Wilson numerical renormalization group method. In particular, the case of the f$^2$-singlet crystalline-electric-field ground state is investigated assuming the case of UPt$_3$ with the hexagonal symmetry. It is found that the interorbital interaction becomes larger than the intraorbital one in contrast to the case of the bare Coulomb interaction for the parameters relevant to UPt$_3$. This result offers us a basis to construct a microscopic theory of the superconductivity of UPt$_3$ where the interorbital interactions are expected to play important roles.Comment: 9 pages, 5 figure

Breathing Current Domains in Globally Coupled Electrochemical Systems: A Comparison with a Semiconductor Model

Spatio-temporal bifurcations and complex dynamics in globally coupled intrinsically bistable electrochemical systems with an S-shaped current-voltage characteristic under galvanostatic control are studied theoretically on a one-dimensional domain. The results are compared with the dynamics and the bifurcation scenarios occurring in a closely related model which describes pattern formation in semiconductors. Under galvanostatic control both systems are unstable with respect to the formation of stationary large amplitude current domains. The current domains as well as the homogeneous steady state exhibit oscillatory instabilities for slow dynamics of the potential drop across the double layer, or across the semiconductor device, respectively. The interplay of the different instabilities leads to complex spatio-temporal behavior. We find breathing current domains and chaotic spatio-temporal dynamics in the electrochemical system. Comparing these findings with the results obtained earlier for the semiconductor system, we outline bifurcation scenarios leading to complex dynamics in globally coupled bistable systems with subcritical spatial bifurcations.Comment: 13 pages, 11 figures, 70 references, RevTex4 accepted by PRE http://pre.aps.or

Magnetic state in URu2Si2, UPd2Al3 and UNi2Al3 probed by point contacts

The antiferromagnetic (AFM) state has been investigated in the three heavy-fermion compounds URu2Si2, UPd2Al3, and UNi2Al3 by measuring dV/dI(V) curves of point contacts at different temperatures (1.5-20 K) and magnetic fields (0-28 T). The zero-bias maximum in dV/dI(V) for URu2Si2 points to a partially gapped Fermi-surface related to the itinerant nature of the AFM state contrary to UPd2Al3 where analogous features have not been found. The AFM state in UNi2Al3 has more similarities with URu2Si2. For URu2Si2, the same critical field of about 40 T along the easy c axis is found for all features in dV/dI(V) corresponding to the Neel temperature, the gap in the electronic density of states, and presumably the ordered moments.Comment: 10 pages incl. 5 figures, LaTex 2

Quasiparticle spin susceptibility in heavy-fermion superconductors : An NMR study compared with specific heat results

Quasi-particle spin susceptibility ($\chi^{qp}$) for various heavy-fermion (HF) superconductors are discussed on the basis of the experimental results of electronic specific heat ($\gamma_{el}$), NMR Knight shift ($K$) and NMR relaxation rate ($1/T_1$) within the framework of the Fermi liquid model for a Kramers doublet crystal electric field (CEF) ground state. $\chi^{qp}_{\gamma}$ is calculated from the enhanced Sommerfeld coefficient $\gamma_{el}$ and $\chi^{qp}_{T_1}$ from the quasi-particle Korringa relation $T_1T(K^{qp}_{T_1})^2=const.$ via the relation of $\chi^{qp}_{T_1}=(N_A\mu_B/A_{hf})K^{qp}_{T_1}$ where $A_{hf}$ is the hyperfine coupling constant, $N_A$ the Abogadoro's number and $\mu_B$ the Bohr magneton. For the even-parity (spin-singlet) superconductors CeCu$_2$Si$_2$, CeCoIn$_5$ and UPd$_2$Al$_3$, the fractional decrease in the Knight shift, $\delta K^{obs}$, below the superconducting transition temperature ($T_c$) is due to the decrease of the spin susceptibility of heavy quasi-particle estimated consistently from $\chi^{qp}_{\gamma}$ and $\chi^{qp}_{T_1}$. This result allows us to conclude that the heavy quasi-particles form the spin-singlet Cooper pairs in CeCu$_2$Si$_2$, CeCoIn$_5$ and UPd$_2$Al$_3$. On the other hand, no reduction in the Knight shift is observed in UPt$_3$ and UNi$_2$Al$_3$, nevertheless the estimated values of $\chi^{qp}_{\gamma}$ and $\chi^{qp}_{T_1}$ are large enough to be probed experimentally. The odd-parity superconductivity is therefore concluded in these compounds. The NMR result provides a convincing way to classify the HF superconductors into either even- or odd- parity paring together with the identification for the gap structure, as long as the system has Kramers degeneracy.Comment: 11 pages, 3 tables, 5 figures, RevTex4(LaTex2e

On the thermoelectricity of correlated electrons in the zero-temperature limit

The Seebeck coefficient of a metal is expected to display a linear temperature-dependence in the zero-temperature limit. To attain this regime, it is often necessary to cool the system well below 1K. We put under scrutiny the magnitude of this term in different families of strongly-interacting electronic systems. For a wide range of compounds (including heavy-fermion, organic and various oxide families) a remarkable correlation between this term and the electronic specific heat is found. We argue that a dimensionless ratio relating these two signatures of mass renormalisation contains interesting information about the ground state of each system. The absolute value of this ratio remains close to unity in a wide range of strongly-correlated electron systems.Comment: 15 pages, including two figure

Optogenetic acidification of synaptic vesicles and lysosomes

Acidification is required for the function of many intracellular organelles, but methods to acutely manipulate their intraluminal pH have not been available. Here we present a targeting strategy to selectively express the light-driven proton pump Arch3 on synaptic vesicles. Our new tool, pHoenix, can functionally replace endogenous proton pumps, enabling optogenetic control of vesicular acidification and neurotransmitter accumulation. Under physiological conditions, glutamatergic vesicles are nearly full, as additional vesicle acidification with pHoenix only slightly increased the quantal size. By contrast, we found that incompletely filled vesicles exhibited a lower release probability than full vesicles, suggesting preferential exocytosis of vesicles with high transmitter content. Our subcellular targeting approach can be transferred to other organelles, as demonstrated for a pHoenix variant that allows light-activated acidification of lysosomes