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Highly charged interface trap states in PbS1âx govern electro-thermal transport
This work describes our discovery of the dominant role of highly charged interfaces on the electrothermal transport properties of PbS, along with a method to reduce the barrier potential for charge carriers by an order of magnitude. High temperature thermoelectrics such as PbS are inevitably exposed to elevated temperatures during postsynthesis treatment as well as operation. However, we observed that as the material was heated, large concentrations of sulfur vacancy (VS..) sites were formed at temperatures as low as 266 degrees C. This loss of sulfur doped the PbS n-type and increased the carrier concentration, where these excess electrons were trapped and immobilized at interfacial defect sites in polycrystalline PbS with an abundance of grain boundaries. Sulfur deficient PbS0.81 exhibited a large barrier potential for charge carriers of 0.352 eV, whereas annealing the material under a sulfur-rich environment prevented VS.. formation and lowered the barrier by an order of magnitude to 0.046 eV. Through ab initio calculations, the formation of VS.. was found to be more favorable on the surface compared to the bulk of the material with a 1.72 times lower formation energy barrier. These observations underline the importance of controlling interface-vacancy effects in the preparation of bulk materials comprised of nanoscale constituents.U. S. National Science Foundation [CAREER-1553987, REU-1560098]; UConn Research Foundation [PD17-0137]; U.S. Department of Energy Office of Science [89233218CNA000001]; GE Graduate Fellowship for Innovation; XSEDE through the computational resource allocation [TG-DMR170031]Open access journalThis item from the UA Faculty Publications collection is made available by the University of Arizona with support from the University of Arizona Libraries. If you have questions, please contact us at [email protected]
Opening the Black Box of Family-Based Treatments: an artificial intelligence Framework to Examine therapeutic alliance and therapist Empathy
The evidence-based treatment (EBT) movement has primarily focused on core intervention content or treatment fidelity and has largely ignored practitioner skills to manage interpersonal process issues that emerge during treatment, especially with difficult-to-treat adolescents (delinquent, substance-using, medical non-adherence) and those of color. A chief complaint of real world practitioners about manualized treatments is the lack of correspondence between following a manual and managing microsocial interpersonal processes (e.g. negative affect) that arise in treating real world clients. Although family-based EBTs share core similarities (e.g. focus on family interactions, emphasis on practitioner engagement, family involvement), most of these treatments do not have an evidence base regarding common implementation and treatment process problems that practitioners experience in delivering particular models, especially in mid-treatment when demands on families to change their behavior is greatest in treatment - a lack that characterizes the field as a whole. Failure to effectively address common interpersonal processes with difficult-to-treat families likely undermines treatment fidelity and sustained use of EBTs, treatment outcome, and contributes to treatment dropout and treatment nonadherence. Recent advancements in wearables, sensing technologies, multivariate time-series analyses, and machine learning allow scientists to make significant advancements in the study of psychotherapy processes by looking under the skin of the provider-client interpersonal interactions that define therapeutic alliance, empathy, and empathic accuracy, along with the predictive validity of these therapy processes (therapeutic alliance, therapist empathy) to treatment outcome. Moreover, assessment of these processes can be extended to develop procedures for training providers to manage difficult interpersonal processes while maintaining a physiological profile that is consistent with astute skills in psychotherapeutic processes. This paper argues for opening the black box of therapy to advance the science of evidence-based psychotherapy by examining the clinical interior of evidence-based treatments to develop the next generation of audit- and feedback- (i.e., systemic review of professional performance) supervision systems
Coherent Spin-Phonon Coupling in the Layered Ferrimagnet Mn3Si2Te6
We utilize ultrafast photoexcitation to drive coherent lattice oscillations
in the layered ferrimagnetic crystal Mn3Si2Te6, which significantly stiffen
below the magnetic ordering temperature. We suggest that this is due to an
exchange-mediated contraction of the lattice, stemming from strong
magneto-structural coupling in this material. Additionally, simulations of the
transient incoherent dynamics reveal the importance of spin relaxation channels
mediated by optical and acoustic phonon scattering. Our findings highlight the
importance of spin-lattice coupling in van der Waals magnets and a promising
route for their dynamic optical control through their intertwined electronic,
lattice, and spin degrees of freedom
Sensitivity analysis of a hybrid-electric aircraft powertrain based on Sobol indices
This paper presents a sensitivity analysis based on the Sobol indices which is an essential step âon the road of system optimizationâ. Such analysis focuses on electrical propeller subsystem (propellers, gearbox, electric motors) including surrogate design models. A previous study [1] has shown that electromechanical actuators (electric generators and electric motors) involve more than 30% of hybrid electric propulsion system weight. Furthermore, most of the variables used for the electric machine design. The electric motor design model is detailed with the related constraints. A physical analysis based on design parameter sensitivity and parameter couplings are described. This study will permit to remove insensitive variables in view of simplifying the global optimization process to be achieved at the whole powertrain level
Surface Effects on Anisotropic Photoluminescence in One-Dimensional Organic Metal Halide Hybrids
One-dimensional (1D) organic metal halide hybrids exhibit strongly
anisotropic optical properties, highly efficient light emission, and large
Stokes shift, holding promises for novel photodetection and lighting
applications. However, the fundamental mechanisms governing their unique
optical properties and in particular the impacts of surface effects are not
understood. Here, we investigate 1D C4N2H14PbBr4 by polarization-dependent
time-averaged and time-resolved photoluminescence (TRPL) spectroscopy, as a
function of photoexcitation energy. Surprisingly, we find that the emission
under photoexcitation polarized parallel to the 1D metal halide chains can be
either stronger or weaker than that under perpendicular polarization, depending
on the excitation energy. We attribute the excitation-energy-dependent
anisotropic emission to fast surface recombination, supported by
first-principles calculations of optical absorption in this material. The fast
surface recombination is directly confirmed by TRPL measurements, when the
excitation is polarized parallel to the chains. Our comprehensive studies
provide a more complete picture for a deeper understanding of the optical
anisotropy in 1D organic metal halide hybrids
Controllable Strain-driven Topological Phase Transition and Dominant Surface State Transport in High-Quality HfTe5 Samples
Controlling materials to create and tune topological phases of matter could
potentially be used to explore new phases of topological quantum matter and to
create novel devices where the carriers are topologically protected. It has
been demonstrated that a trivial insulator can be converted into a topological
state by modulating the spin-orbit interaction or the crystal lattice. However,
there are limited methods to controllably and efficiently tune the crystal
lattice and at the same time perform electronic measurements at cryogenic
temperatures. Here, we use large controllable strain to demonstrate the
topological phase transition from a weak topological insulator phase to a
strong topological insulator phase in high-quality HfTe5 samples. After
applying high strain to HfTe5 and converting it into a strong topological
insulator, we found that the sample's resistivity increased by more than two
orders of magnitude (24,000%) and that the electronic transport is dominated by
the topological surface states at cryogenic temperatures. Our findings show
that HfTe5 is an ideal material for engineering topological properties, and it
could be generalized to study topological phase transitions in van der Waals
materials and heterostructures. These results can pave the way to create novel
devices with applications ranging from spintronics to fault-tolerant
topologically protected quantum computers
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