Free-carrier relaxation and lattice heating in photoexcited bismuth thin films

We report ultrafast surface pump and interface probe experiments on photoexcited carrier transport across single crystal bismuth films on sapphire. The film thickness is sufficient to separate carrier dynamics from lattice heating and strain, allowing us to investigate the time-scales of momentum relaxation, heat transfer to the lattice and electron-hole recombination. The measured electron-hole ($e-h$) recombination time is 12--26 ps and ambipolar diffusivity is 18--40 cm$^{2}$/s for carrier excitation up to $\sim 10^{19} \text{cm}^{-3}$. By comparing the heating of the front and back sides of the film, we put lower limits on the rate of heat transfer to the lattice, and by observing the decay of the plasma at the back of the film, we estimate the timescale of electron-hole recombination. We interpret each of these timescales within a common framework of electron-phonon scattering and find qualitative agreement between the various relaxation times observed. We find that the carrier density is not determined by the $e-h$ plasma temperature after a few picoseconds. The diffusion and recombination become nonlinear with initial excitation $\gtrsim 10^{20} \text{cm}^{-3}$

Sodium vacancy ordering and the co-existence of localized spins and itinerant charges in NaxCoO2

The sodium cobaltate family (NaxCoO2) is unique among transition metal oxides because the Co sits on a triangular lattice and its valence can be tuned over a wide range by varying the Na concentration x. Up to now detailed modeling of the rich phenomenology (which ranges from unconventional superconductivity to enhanced thermopower) has been hampered by the difficulty of controlling pure phases. We discovered that certain Na concentrations are specially stable and are associated with superlattice ordering of the Na clusters. This leads naturally to a picture of co-existence of localized spins and itinerant charge carriers. For x = 0.84 we found a remarkably small Fermi energy of 87 K. Our picture brings coherence to a variety of measurements ranging from NMR to optical to thermal transport. Our results also allow us to take the first step towards modeling the mysterious ``Curie-Weiss'' metal state at x = 0.71. We suggest the local moments may form a quantum spin liquid state and we propose experimental test of our hypothesis.Comment: 16 pages, 5 figure

The first products made in space: Monodisperse latex particles

The preparation of large particle size 3 to 30 micrometer monodisperse latexes in space confirmed that original rationale unequivocally. The flight polymerizations formed negligible amounts of coagulum as compared to increasing amounts for the ground-based polymerizations. The number of offsize large particles in the flight latexes was smaller than in the ground-based latexes. The particle size distribution broadened and more larger offsize particles were formed when the polymerizations of the partially converted STS-4 latexes were completed on Earth. Polymerization in space also showed other unanticipated advantages. The flight latexes had narrower particle size distributions than the ground-based latexes. The particles of the flight latexes were more perfect spheres than those of the ground-based latexes. The superior uniformity of the flight latexes was confirmed by the National Bureau of Standards acceptance of the 10 micrometer STS-6 latex and the 30 micrometer STS-11 latexes as Standard Reference Materials, the first products made in space for sale on Earth. The polymerization rates in space were the same as those on Earth within experimental error. Further development of the ground-based polymerization recipes gave monodisperse particles as large as 100 micrometer with tolerable levels of coagulum, but their uniformity was significantly poorer than the flight latexes. Careful control of the polymerization parameters gave uniform nonspherical particles: symmetrical and asymmetrical doublets, ellipsoids, egg-shaped, ice cream cone-shaped, and popcorn-shaped particles

Magnetothermopower and Magnetoresistivity of RuSr2Gd1-xLaxCu2O8 (x=0, 0.1)

We report measurements of magnetothermopower and magnetoresistivity as a function of temperature on RuSr2Gd1-xLaxCu2O8 (x = 0, 0.1). The normal-state thermopower shows a dramatic decrease after applying a magnetic field of 5 T, whereas the resistivity shows only a small change after applying the same field. Our results suggest that RuO2 layers are conducting and the magnetic field induced decrease of the overall thermopower is caused by the decrease of partial thermopower decrease associated with the spin entropy decrease of the carriers in the RuO2 layers.Comment: 21 pages, 6 figure

An Empirical Charge Transfer Potential with Correct Dissociation Limits

The empirical valence bond (EVB) method [J. Chem. Phys. 52, 1262 (1970)] has always embodied charge transfer processes. The mechanism of that behavior is examined here and recast for use as a new empirical potential energy surface for large-scale simulations. A two-state model is explored. The main features of the model are: (1) Explicit decomposition of the total system electron density is invoked; (2) The charge is defined through the density decomposition into constituent contributions; (3) The charge transfer behavior is controlled through the resonance energy matrix elements which cannot be ignored; and (4) A reference-state approach, similar in spirit to the EVB method, is used to define the resonance state energy contributions in terms of "knowable" quantities. With equal validity, the new potential energy can be expressed as a nonthermal ensemble average with a nonlinear but analytical charge dependence in the occupation number. Dissociation to neutral species for a gas-phase process is preserved. A variant of constrained search density functional theory is advocated as the preferred way to define an energy for a given charge.Comment: Submitted to J. Chem. Phys. 11/12/03. 14 pages, 8 figure

Cerebral blood flow links insulin resistance and baroreflex sensitivity

Insulin resistance confers risk for diabetes mellitus and associates with a reduced capacity of the arterial baroreflex to regulate blood pressure. Importantly, several brain regions that comprise the central autonomic network, which controls the baroreflex, are also sensitive to the neuromodulatory effects of insulin. However, it is unknown whether peripheral insulin resistance relates to activity within central autonomic network regions, which may in turn relate to reduced baroreflex regulation. Accordingly, we tested whether resting cerebral blood flow within central autonomic regions statistically mediated the relationship between insulin resistance and an indirect indicator of baroreflex regulation; namely, baroreflex sensitivity. Subjects were 92 community-dwelling adults free of confounding medical illnesses (48 men, 30-50 years old) who completed protocols to assess fasting insulin and glucose levels, resting baroreflex sensitivity, and resting cerebral blood flow. Baroreflex sensitivity was quantified by measuring the magnitude of spontaneous and sequential associations between beat-by-beat systolic blood pressure and heart rate changes. Individuals with greater insulin resistance, as measured by the homeostatic model assessment, exhibited reduced baroreflex sensitivity (b = -0.16, p < .05). Moreover, the relationship between insulin resistance and baroreflex sensitivity was statistically mediated by cerebral blood flow in central autonomic regions, including the insula and cingulate cortex (mediation coefficients < -0.06, p-values < .01). Activity within the central autonomic network may link insulin resistance to reduced baroreflex sensitivity. Our observations may help to characterize the neural pathways by which insulin resistance, and possibly diabetes mellitus, relates to adverse cardiovascular outcomes. © 2013 Ryan et al