779 research outputs found
Inter-valley dark trion states with spin lifetimes of 150 ns in WSe
We demonstrate long trion spin lifetimes in a WSe monolayer of up to 150
ns at 5 K. Applying a transverse magnetic field in time-resolved Kerr-rotation
measurements reveals a complex composition of the spin signal of up to four
distinct components. The Kerr rotation signal can be well described by a model
which includes inhomogeneous spin dephasing and by setting the trion spin
lifetimes to the measured excitonic recombination times extracted from
time-resolved reflectivity measurements. We observe a continuous shift of the
Kerr resonance with the probe energy, which can be explained by an
adsorbate-induced, inhomogeneous potential landscape of the WSe flake. A
further indication of extrinsic effects on the spin dynamics is given by a
change of both the trion spin lifetime and the distribution of g-factors over
time. Finally, we detect a Kerr rotation signal from the trion's higher-energy
triplet state when the lower-energy singlet state is optically pumped by
circularly polarized light. We explain this by the formation of dark trion
states, which are also responsible for the observed long trion spin lifetimes.Comment: 23 pages, 13 figure
Analytical considerations for accurately capturing the relevant species contributing to vitamin D status in liquid chromatography-tandem mass spectrometry assays
This tutorial review focuses on analytical challenges encountered with the liquid chromatography-tandem mass spectrometry determination of 25-hydroxyvitamin D, which is currently still considered the metabolite that is most representative of vitamin D status. It describes how multiple binding states of circulating 25-hydroxyvitamin D (phase II metabolites, epimers, free/bioavailable/protein-bound species) can influence the accuracy of the analytical determination. It also summarizes important chemical species that can inadvertently contribute to vitamin D status and thus cause systematic errors. These interfering endogenous and exogenous compounds might be isomers of vitamin D, constitutional isomers or isobars and the article outlines techniques to eliminate or minimize these interferences, including chromatographic separations, ion mobility spectrometry, and high-resolution mass spectrometry.Peer Reviewe
Geometrical Frustration: A Study of 4d Hard Spheres
The smallest maximum kissing-number Voronoi polyhedron of 3d spheres is the
icosahedron and the tetrahedron is the smallest volume that can show up in
Delaunay tessalation. No periodic lattice is consistent with either and hence
these dense packings are geometrically frustrated. Because icosahedra can be
assembled from almost perfect tetrahedra, the terms "icosahedral" and
"polytetrahedral" packing are often used interchangeably, which leaves the true
origin of geometric frustration unclear. Here we report a computational study
of freezing of 4d hard spheres, where the densest Voronoi cluster is compatible
with the symmetry of the densest crystal, while polytetrahedral order is not.
We observe that, under otherwise comparable conditions, crystal nucleation in
4d is less facile than in 3d. This suggest that it is the geometrical
frustration of polytetrahedral structures that inhibits crystallization.Comment: 4 pages, 3 figures; revised interpretatio
Phase-field crystal modelling of crystal nucleation, heteroepitaxy and patterning
We apply a simple dynamical density functional theory, the
phase-field-crystal (PFC) model, to describe homogeneous and heterogeneous
crystal nucleation in 2d monodisperse colloidal systems and crystal nucleation
in highly compressed Fe liquid. External periodic potentials are used to
approximate inert crystalline substrates in addressing heterogeneous
nucleation. In agreement with experiments in 2d colloids, the PFC model
predicts that in 2d supersaturated liquids, crystalline freezing starts with
homogeneous crystal nucleation without the occurrence of the hexatic phase. At
extreme supersaturations crystal nucleation happens after the appearance of an
amorphous precursor phase both in 2d and 3d. We demonstrate that contrary to
expectations based on the classical nucleation theory, corners are not
necessarily favourable places for crystal nucleation. Finally, we show that
adding external potential terms to the free energy, the PFC theory can be used
to model colloid patterning experiments.Comment: 21 pages, 16 figure
Hard sphere crystallization gets rarer with increasing dimension
We recently found that crystallization of monodisperse hard spheres from the
bulk fluid faces a much higher free energy barrier in four than in three
dimensions at equivalent supersaturation, due to the increased geometrical
frustration between the simplex-based fluid order and the crystal [J.A. van
Meel, D. Frenkel, and P. Charbonneau, Phys. Rev. E 79, 030201(R) (2009)]. Here,
we analyze the microscopic contributions to the fluid-crystal interfacial free
energy to understand how the barrier to crystallization changes with dimension.
We find the barrier to grow with dimension and we identify the role of
polydispersity in preventing crystal formation. The increased fluid stability
allows us to study the jamming behavior in four, five, and six dimensions and
compare our observations with two recent theories [C. Song, P. Wang, and H. A.
Makse, Nature 453, 629 (2008); G. Parisi and F. Zamponi, Rev. Mod. Phys, in
press (2009)].Comment: 15 pages, 5 figure
Nanosecond spin lifetimes in single- and few-layer graphene-hBN heterostructures at room temperature
We present a new fabrication method of graphene spin-valve devices which
yields enhanced spin and charge transport properties by improving both the
electrode-to-graphene and graphene-to-substrate interface. First, we prepare
Co/MgO spin injection electrodes onto Si/SiO. Thereafter, we
mechanically transfer a graphene-hBN heterostructure onto the prepatterned
electrodes. We show that room temperature spin transport in single-, bi- and
trilayer graphene devices exhibit nanosecond spin lifetimes with spin diffusion
lengths reaching 10m combined with carrier mobilities exceeding 20,000
cm/Vs.Comment: 15 pages, 5 figure
Homogeneous nucleation of colloidal melts under the influence of shearing fields
We study the effect of shear flow on homogeneous crystal nucleation, using
Brownian Dynamics simulations in combination with an umbrella sampling like
technique. The symmetry breaking due to shear results in anisotropic radial
distribution functions. The homogeneous shear rate suppresses crystal
nucleation and leads to an increase of the size of the critical nucleus. These
observations can be described by a simple, phenomenological extension of
classical nucleation theory. In addition, we find that nuclei have a
preferential orientation with respect to the direction of shear. On average the
longest dimension of a nucleus is along the vorticity direction, while the
shortest dimension is preferably perpendicular to that and slightly tilted with
respect to the gradient direction.Comment: 10 pages, 8 figures, Submitted to J. Phys.: Condens. Matte
Static Friction between Elastic Solids due to Random Asperities
Several workers have established that the Larkin domains for two three
dimensional nonmetallic elastic solids in contact with each other at a
disordered interface are enormously large. This implies that there should be
negligible static friction per unit area in the macroscopic solid limit.
The present work argues that the fluctuations in the heights of the random
asperities at the interface that occur in the Greenwood-Williamson model can
account for static friction.Comment: Contains some improvements in the treatment of the subjec
Collective Behavior of Asperities in Dry Friction at Small Velocities
We investigate a simple model of dry friction based on extremal dynamics of
asperities. At small velocities, correlations develop between the asperities,
whose range becomes infinite in the limit of infinitely slow driving, where the
system is self-organized critical. This collective phenomenon leads to
effective aging of the asperities and results in velocity dependence of the
friction force in the form .Comment: 7 pages, 8 figures, revtex, submitted to Phys. Rev.
Simulation of fluid-solid coexistence in finite volumes: A method to study the properties of wall-attached crystalline nuclei
The Asakura-Oosawa model for colloid-polymer mixtures is studied by Monte
Carlo simulations at densities inside the two-phase coexistence region of fluid
and solid. Choosing a geometry where the system is confined between two flat
walls, and a wall-colloid potential that leads to incomplete wetting of the
crystal at the wall, conditions can be created where a single nanoscopic
wall-attached crystalline cluster coexists with fluid in the remainder of the
simulation box. Following related ideas that have been useful to study
heterogeneous nucleation of liquid droplets at the vapor-liquid coexistence, we
estimate the contact angles from observations of the crystalline clusters in
thermal equilibrium. We find fair agreement with a prediction based on Young's
equation, using estimates of interface and wall tension from the study of flat
surfaces. It is shown that the pressure versus density curve of the finite
system exhibits a loop, but the pressure maximum signifies the "droplet
evaporation-condensation" transition and thus has nothing in common with a van
der Waals-like loop. Preparing systems where the packing fraction is deep
inside the two-phase coexistence region, the system spontaneously forms a "slab
state", with two wall-attached crystalline domains separated by (flat)
interfaces from liquid in full equilibrium with the crystal in between;
analysis of such states allows a precise estimation of the bulk equilibrium
properties at phase coexistence
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