517 research outputs found
Mechanism of structural phase transitions in KCrF3
We study the origin of the cubic to tetragonal and tetragonal to monoclinic
structural transitions in KCrF3, and the associated change in orbital order,
paying particular attention to the relevance of super-exchange in both phases.
We show that super-exchange is not the main mechanism driving these
transitions. Specifically, it is not strong enough to be responsible for the
high-temperature cubic to tetragonal transition and does not yield the type of
orbital order observed in the monoclinic phase. The energy difference between
the tetragonal and the monoclinic structure is tiny, and most likely results
from the interplay between volume, covalency, and localization effects. The
transition is rather driven by Slater exchange than super-exchange.
Nevertheless, once the monoclinic distortions are present, super-exchange helps
in stabilizing the low symmetry structure. The orbital order we obtain for this
monoclinic phase is consistent with the magnetic transition at 80 K.Comment: 8 pages, 6 figure
Dominant Reaction Pathways in High Dimensional Systems
This paper is devoted to the development of a theoretical and computational
framework to efficiently sample the statistically significant thermally
activated reaction pathways, in multi-dimensional systems obeying Langevin
dynamics. We show how to obtain the set of most probable reaction pathways and
compute the corrections due to quadratic thermal fluctuations around such
trajectories. We discuss how to obtain predictions for the evolution of
arbitrary observables and how to generate conformations which are
representative of the transition state ensemble. We present an illustrative
implementation of our method by studying the diffusion of a point particle in a
2-dimensional funneled external potential.Comment: 18 pages, 7 figures. Improvement in the text and in the figures.
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Altermagnetic surface states: towards the observation and utilization of altermagnetism in thin films, interfaces and topological materials
The altermagnetism influences the electronic states allowing the presence of
non-relativistic spinsplittings. Since altermagnetic spin-splitting is present
along specific k-paths of the 3D Brillouin zone, we expect that the
altermagnetic surface states will be present on specific surface orientations.
We unveil the properties of the altermagnetic surface states considering three
representative space groups: tetragonal, orthorhombic and hexagonal. We
calculate the 2D projected Brillouin zone from the 3D Brillouin zone. We study
the surfaces with their respective 2D Brillouin zones establishing where the
spin-splittings with opposite sign merge annihilating the altermagnetic
properties and on which surfaces the altermagnetism is preserved. Looking at
the three principal surface orientations, we find that for several cases two
surfaces are blind to the altermagnetism, while the altermagnetism survives for
one surface orientation. Which surface preserves the altermagnetism depends
also on the magnetic order. We show that an electric field orthogonal to the
blind surface can activate the altermagnetism. Our results predict which
surfaces to cleave in order to preserve altermagnetism in surfaces or
interfaces and this paves the way to observe non-relativistic altermagnetic
spin-splitting in thin films via spin-resolved ARPES and to interface the
altermagnetism with other collective modes. We open future perspectives for the
study of altermagnetic effects on the trivial and topological surface states.Comment: 8 pages, 10 figure
Puckering Free Energy of Pyranoses: an NMR and Metadynamics--Umbrella Sampling Investigation
We present the results of a combined metadynamics--umbrella sampling
investigation of the puckered conformers of pyranoses described using the
gromos 45a4 force field. The free energy landscape of Cremer--Pople puckering
coordinates has been calculated for the whole series of alpha and beta
aldohexoses, showing that the current force field parameters fail in
reproducing proper puckering free energy differences between chair conformers.
We suggest a modification to the gromos 45a4 parameter set which improves
considerably the agreement of simulation results with theoretical and
experimental estimates of puckering free energies. We also report on the
experimental measurement of altrose conformers populations by means of NMR
spectroscopy, which show good agreement with the predictions of current
theoretical models
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