645 research outputs found
A multideterminant assessment of mean field methods for the description of electron transfer in the weak coupling regime
Multideterminant calculations have been performed on model systems to
emphasize the role of many-body effects in the general description of charge
quantization experiments. We show numerically and derive analytically that a
closed-shell ansatz, the usual ingredient of mean-field methods, does not
properly describe the step-like electron transfer characteristic in weakly
coupled systems. With the multideterminant results as a benchmark, we have
evaluated the performance of common ab initio mean field techniques, such as
Hartree Fock (HF) and Density Functional Theory (DFT) with local and hybrid
exchange correlation functionals, with a special focus on spin-polarization
effects. For HF and hybrid DFT, a qualitatively correct open-shell solution
with distinct steps in the electron transfer behaviour can be obtained with a
spin-unrestricted (i.e., spin-polarized) ansatz though this solution differs
quantitatively from the multideterminant reference. We also discuss the
relationship between the electronic eigenvalue gap and the onset of charge
transfer for both HF and DFT and relate our findings to recently proposed
practical schemes for calculating the addition energies in the Coulomb blockade
regime for single molecule junctions from closed-shell DFT within the local
density approximation
Anisotropy of the Mobility of Pentacene from Frustration
The bandstructure of pentacene is calculated using first-principles density
functional theory. A large anisotropy of the hole and electron effective masses
within the molecular planes is found. The band dispersion of the HOMO and the
LUMO is analyzed with the help of a tight-binding fit. The anisotropy is shown
to be intimately related to the herringbone structure.Comment: Accepted for publication in Synthetic Metal
Electric-Field-Induced Mott Insulating States in Organic Field-Effect Transistors
We consider the possibility that the electrons injected into organic
field-effect transistors are strongly correlated. A single layer of acenes can
be modelled by a Hubbard Hamiltonian similar to that used for the
kappa-(BEDT-TTF)(2)X family of organic superconductors. The injected electrons
do not necessarily undergo a transition to a Mott insulator state as they would
in bulk crystals when the system is half-filled. We calculate the fillings
needed for obtaining insulating states in the framework of the slave-boson
theory and in the limit of large Hubbard repulsion, U. We also suggest that
these Mott states are unstable above some critical interlayer coupling or
long-range Coulomb interaction.Comment: 9 pages, 7 figure
Plasmacytoid dendritic cells migrate in afferent skin lymph (Correction: vol 180, pg 5963, 2008)
Psychometric properties of the transaddiction craving triggers questionnaire in alcohol use disorder.
We aimed to develop the transaddiction craving triggers questionnaire (TCTQ), which assesses the propensity of specific situations and contexts to trigger craving and to test its psychometric properties in alcohol use disorder (AUD).
This study included a sample of 111 AUD outpatients. We performed exploratory factor analysis (EFA) and calculated item-dimension correlations. Internal consistency was measured with Cronbach's alpha coefficient. Construct validity was assessed through Spearman correlations with craving, emotional symptoms, impulsivity, mindfulness, and drinking characteristics.
The EFA suggested a 3-factor solution: unpleasant affect, pleasant affect, and cues and related thoughts. Cronbach's coefficient alpha ranged from .80 to .95 for the three factors and the total score. Weak positive correlations were identified between the TCTQ and drinking outcomes, and moderate correlation were found between the TCTQ and craving strength, impulsivity, anxiety, depression, and impact of alcohol on quality of life.
The 3-factor structure is congruent with the well-established propensity of emotions and cues to trigger craving. Construct validity is supported by close relations between the TCTQ and psychological well-being rather than between the TCTQ and drinking behaviors. Longitudinal validation is warranted to assess sensitivity to change of the TCTQ and to explore its psychometric properties in other addictive disorders
A New Photomechanical Molecular Switch Based on a Linear {\pi}-Conjugated System
We report the electronic transport properties of a new photo-addressable
molecular switch. The switching process relies on a new concept based on linear
{\pi}-conjugated dynamic systems, in which the geometry and hence the
electronic properties of an oligothiophene chain can be reversibly modified by
the photochemical trans-cis isomerization of an azobenzene unit fixed in a
lateral loop. Electron transport measurements through self-assembled monolayers
on gold, contacted with eGaIn top contact, show switching with a conductance
ratio up to 1E3. Ab initio calculations have been used to identify the most
energetically stable conformations of the molecular switch, the corresponding
calculated conductances qualitatively explain the trend observed in the
photo-switching experiments.Comment: Full manuscript and supporting information, J. Phys. Chem.
C,published on line (2017
A New Photomechanical Molecular Switch Based on a Linear {\pi}-Conjugated System
We report the electronic transport properties of a new photo-addressable
molecular switch. The switching process relies on a new concept based on linear
{\pi}-conjugated dynamic systems, in which the geometry and hence the
electronic properties of an oligothiophene chain can be reversibly modified by
the photochemical trans-cis isomerization of an azobenzene unit fixed in a
lateral loop. Electron transport measurements through self-assembled monolayers
on gold, contacted with eGaIn top contact, show switching with a conductance
ratio up to 1E3. Ab initio calculations have been used to identify the most
energetically stable conformations of the molecular switch, the corresponding
calculated conductances qualitatively explain the trend observed in the
photo-switching experiments.Comment: Full manuscript and supporting information, J. Phys. Chem.
C,published on line (2017
Has probation any impact in terms of reparation to victims and communities? Complicating a simple question
A DNA-Modified Live Vaccine Prime-Boost Strategy Broadens the T-Cell Response and Enhances the Antibody Response against the Porcine Reproductive and Respiratory Syndrome Virus.
The Porcine Reproductive and Respiratory Syndrome Virus (PRRSV) induces reproductive disorders in sows and respiratory illnesses in growing pigs and is considered as one of the main pathogenic agents responsible for economic losses in the porcine industry worldwide. Modified live PRRSV vaccines (MLVs) are very effective vaccine types against homologous strains but they present only partial protection against heterologous viral variants. With the goal to induce broad and cross-protective immunity, we generated DNA vaccines encoding B and T antigens derived from a European subtype 1 strain that include T-cell epitope sequences known to be conserved across strains. These antigens were expressed either in a native form or in the form of vaccibodies targeted to the endocytic receptor XCR1 and CD11c expressed by different types of antigen-presenting cells (APCs). When delivered in skin with cationic nanoparticles and surface electroporation, multiple DNA vaccinations as a stand-alone regimen induced substantial antibody and T-cell responses, which were not promoted by targeting antigens to APCs. Interestingly, a DNA-MLV prime-boost strategy strongly enhanced the antibody response and broadened the T-cell responses over the one induced by MLV or DNA-only. The anti-nucleoprotein antibody response induced by the DNA-MLV prime-boost was clearly promoted by targeting the antigen to CD11c and XCR1, indicating a benefit of APC-targeting on the B-cell response. In conclusion, a DNA-MLV prime-boost strategy, by enhancing the potency and breadth of MLV vaccines, stands as a promising vaccine strategy to improve the control of PRRSV in infected herds
Excited States of Ladder-type Poly-p-phenylene Oligomers
Ground state properties and excited states of ladder-type paraphenylene
oligomers are calculated applying semiempirical methods for up to eleven
phenylene rings. The results are in qualitative agreement with experimental
data. A new scheme to interpret the excited states is developed which reveals
the excitonic nature of the excited states. The electron-hole pair of the
S1-state has a mean distance of approximately 4 Angstroem.Comment: 24 pages, 21 figure
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