925 research outputs found
X-ray Scattering Study of the spin-Peierls transition and soft phonon behavior in TiOCl
We have studied the S=1/2 quasi-one-dimensional antiferromagnet TiOCl using
single crystal x-ray diffraction and inelastic x-ray scattering techniques. The
Ti ions form staggered spin chains which dimerize below Tc1 = 66 K and have an
incommensurate lattice distortion between Tc1 and Tc2 = 92 K. Based on our
measurements of the intensities, wave vectors, and harmonics of the
incommensurate superlattice peaks, we construct a model for the incommensurate
modulation. The results are in good agreement with a soliton lattice model,
though some quantitative discrepancies exist near Tc2. The behavior of the
phonons has been studied using inelastic x-ray scattering with ~2 meV energy
resolution. For the first time, a zone boundary phonon which softens at the
spin-Peierls temperature Tsp has been observed. Our results show reasonably
good quantitative agreement with the Cross-Fisher theory for the phonon
dynamics at wave vectors near the zone boundary and temperatures near Tsp.
However, not all aspects of the data can be described, such as the strong
overdamping of the soft mode above Tsp. Overall, our results show that TiOCl is
a good realization of a spin-Peierls system, where the phonon softening allows
us to identify the transition temperature as Tsp=Tc2=92 KComment: 14 pages, 14 figure
Crystallization in suspensions of hard spheres: A Monte Carlo and Molecular Dynamics simulation study
The crystallization of a metastable melt is one of the most important non
equilibrium phenomena in condensed matter physics, and hard sphere colloidal
model systems have been used for several decades to investigate this process by
experimental observation and computer simulation. Nevertheless, there is still
an unexplained discrepancy between simulation data and experimental nucleation
rate densities. In this paper we examine the nucleation process in hard spheres
using molecular dynamics and Monte Carlo simulation. We show that the
crystallization process is mediated by precursors of low orientational
bond-order and that our simulation data fairly match the experimental data
sets
Evidence of short time dynamical correlations in simple liquids
We report a molecular dynamics (MD) study of the collective dynamics of a
simple monatomic liquid -interacting through a two body potential that mimics
that of lithium- across the liquid-glass transition. In the glassy phase we
find evidences of a fast relaxation process similar to that recently found in
Lennard-Jones glasses. The origin of this process is ascribed to the
topological disorder, i.e. to the dephasing of the different momentum
Fourier components of the actual normal modes of vibration of the disordered
structure. More important, we find that the fast relaxation persists in the
liquid phase with almost no temperature dependence of its characteristic
parameters (strength and relaxation time). We conclude, therefore, that in the
liquid phase well above the melting point, at variance with the usual
assumption of {\it un-correlated} binary collisions, the short time particles
motion is strongly {\it correlated} and can be described via a normal mode
expansion of the atomic dynamics.Comment: 7 pages, 7 .eps figs. To appear in Phys. Rev.
Cluster Dynamical Mean-field calculations for TiOCl
Based on a combination of cluster dynamical mean field theory (DMFT) and
density functional calculations, we calculated the angle-integrated spectral
density in the layered quantum magnet TiOCl. The agreement with recent
photoemission and oxygen K-edge X-ray absorption spectroscopy experiments is
found to be good. Th e improvement achieved with this calculation with respect
to previous single-site DMFT calculations is an indication of the correlated
nature and low-dimensionality of TiOCl.Comment: 9 pages, 3 figures, improved version as publishe
Fluorescent Nanozeolite Receptors for the Highly Selective and Sensitive Detection of Neurotransmitters in Water and Biofluids
The design and preparation of synthetic binders (SBs) applicable for small biomolecule sensing in aqueous media remains very challenging. SBs designed by the lock-and-key principle can be selective for their target analyte but usually show an insufficient binding strength in water. In contrast, SBs based on symmetric macrocycles with a hydrophobic cavity can display high binding affinities but generally suffer from indiscriminate binding of many analytes. Herein, a completely new and modular receptor design strategy based on microporous hybrid materials is presented yielding zeolite-based artificial receptors (ZARs) which reversibly bind the neurotransmitters serotonin and dopamine with unprecedented affinity and selectivity even in saline biofluids. ZARs are thought to uniquely exploit both the non-classical hydrophobic effect and direct non-covalent recognition motifs, which is supported by in-depth photophysical, and calorimetric experiments combined with full atomistic modeling. ZARs are thermally and chemically robust and can be readily prepared at gram scales. Their applicability for the label-free monitoring of important enzymatic reactions, for (two-photon) fluorescence imaging, and for high-throughput diagnostics in biofluids is demonstrated. This study showcases that artificial receptor based on microporous hybrid materials can overcome standing limitations of synthetic chemosensors, paving the way towards personalized diagnostics and metabolomics
Evidence of two viscous relaxation processes in the collective dynamics of liquid lithium
New inelastic X-ray scattering experiments have been performed on liquid
lithium in a wide wavevector range. With respect to the previous measurements,
the instrumental resolution, improved up to 1.5 meV, allows to accurately
investigate the dynamical processes determining the observed shape of the the
dynamic structure factor, . A detailed analysis of the lineshapes
shows the co-existence of relaxation processes with both a slow and a fast
characteristic timescales, and therefore that pictures of the relaxation
mechanisms based on a simple viscoelastic model must be abandoned.Comment: 5 pages, 4 .PS figure
Inelastic X-ray scattering study of the collective dynamics in liquid sodium
Inelastic X-ray scattering data have been collected for liquid sodium at
T=390 K, i.e. slightly above the melting point. Owing to the very high
instrumental resolution, pushed up to 1.5 meV, it has been possible to
determine accurately the dynamic structure factor, , in a wide
wavevector range, nm, and to investigate on the dynamical
processes underlying the collective dynamics. A detailed analysis of the
lineshape of , similarly to other liquid metals, reveals the
co-existence of two different relaxation processes with slow and fast
characteristic timescales respectively. The present data lead to the conclusion
that: i) the picture of the relaxation mechanism based on a simple viscoelastic
model fails; ii) although the comparison with other liquid metals reveals
similar behavior, the data do not exhibit an exact scaling law as the principle
of corresponding state would predict.Comment: RevTex, 7 pages, 6 eps figures. Accepted by Phys. Rev.
Interaction of photons with plasmas and liquid metals: photoabsorption and scattering
Formulas to describe the photoabsorption and the photon scattering by a
plasma or a liquid metal are derived in a unified manner with each other. It is
shown how the nuclear motion, the free-electron motion and the core-electron
behaviour in each ion in the system determine the structure of photoabsorption
and scattering in an electron-ion mixture. The absorption cross section in the
dipole approximation consists of three terms which represent the absorption
caused by the nuclear motion, the absorption owing to the free-electron motion
producing optical conductivity or inverse Bremsstrahlung, and the absorption
ascribed to the core-electron behaviour in each ion with the Doppler
correction. Also, the photon scattering formula provides an analysis method for
experiments observing the ion-ion dynamical structure factor (DSF), the
electron-electron DSF giving plasma oscillations, and the core-electron DSF
yielding the X-ray Raman (Compton) scattering with a clear definition of the
background scattering for each experiment, in a unified manner. A formula for
anomalous X-ray scattering is also derived for a liquid metal. At the same
time, Thomson scattering in plasma physics is discussed from this general point
of view.Comment: LaTeX file: 18 pages without figur
Density fluctuations and single-particle dynamics in liquid lithium
The single-particle and collective dynamical properties of liquid lithium
have been evaluated at several thermodynamic states near the triple point. This
is performed within the framework of mode-coupling theory, using a
self-consistent scheme which, starting from the known static structure of the
liquid, allows the theoretical calculation of several dynamical properties.
Special attention is devoted to several aspects of the single-particle
dynamics, which are discussed as a function of the thermodynamic state. The
results are compared with those of Molecular Dynamics simulations and other
theoretical approaches.Comment: 31 pages (in preprint format), 14 figures. Submitted to Phys. Rev.
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