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6%), which include the hassle of wearing the device (38%) and dislike of device on the body (33%). Adolescents who endorsed more barriers also reported more diabetes distress (P = 0.003), family conflict (P = 0.003), and depressive symptoms (P = 0.014). Pump and CGM discontinuers both endorsed more barriers and more negative perceptions of technology than current users, but reported no difference from device users in diabetes distress, family conflict, or depression. Gender was not related to the perceptions of devices. Conclusions Clinicians can proactively assess attitudes toward diabetes technology and perceptions of benefits/burdens to encourage device uptake and potentially prevent device discontinuation among adolescents.Humans have a unique ability to perceive shape in different ways. Although we naturally estimate objective (physical) shape in our daily interactions with the world, we are also capable of estimating projective (retinal) shape, especially when attempting to accurately draw objects and scenes. In four experiments, we demonstrated robust effects of 3D context on shape perception. Using a binocular stereo paradigm, we presented rectangular surfaces of varying widths alone or embedded in a polyhedron. We investigated how context, judgment type, and angle affected width estimates. see more We found that the presence of even a small amount of 3D context aids objective judgments but hinders projective judgments, whereas a lack of context had the opposite effect. Context facilitated objective shape assessments by improving estimates of surface orientation. These results demonstrate that the typical presence of 3D context aids shape perception (shape constancy) while simultaneously making the projective judgments necessary for realistic drawing more difficult.The separation of charge-transfer states into free charges at the donor/acceptor (D/A) interfaces plays a central role in organic solar cells (OSCs). Because of strong Coulomb attraction, the separation mechanisms are elusive, particularly for the high-efficiency non-fullerene (NF) OSCs with low exciton-dissociation driving forces. Here, we demonstrate that the Coulomb barriers can be substantially overcome by electronic polarization for OSCs based on a series of A-D-A acceptors (ITIC, IT-4F, and Y6). In contrast to fullerene-based D/A heterojunctions, the polarization energies for both donor holes and acceptor electrons are remarkably increased from the interfaces to pure regions in the NF heterojunctions because of strong stabilization on electrons but destabilization on holes by electrostatic interactions in the A-D-A acceptors. In particular, upon incorporation of fluorine substituents and electron-poor cores into ITIC, the increased polarization energies can completely compensate for the Coulomb attraction in the IT-4F- and Y6-based heterojunctions, leading to barrierless charge separation.Nickel(I) metalloradicals bear great potential for the reductive activation of challenging substrates but are often too unstable to be isolated. Similar chemistry may be enabled by nickel(II) hydrides that store the reducing equivalents in hydride bonds and reductively eliminate H2 upon substrate binding. Here we present a pyrazolate-based bis(β-diketiminato) ligand [LPh]3- with bulky m-terphenyl substituents that can host two Ni-H units in close proximity. Complexes [LPh(NiII-H)2]- (3) are prone to intramolecular reductive H2 elimination, and an equilibrium between 3 and orthometalated dinickel(II) monohydride complexes 2 is evidenced. 2 is shown to form via intramolecular metal-metal cooperative phenyl group C(sp2)-H oxidative addition to the dinickel(I) intermediate [LPhNiI2]- (4). While NiI species have been implicated in catalytic C-H functionalization, discrete activation of C-H bonds at NiI complexes has rarely been described. The reversible H2 and C-H reductive elimination/oxidative addition equilibrium smoothly unmasks the powerful 2-electron reductant 4 from either 2 or 3, which is demonstrated by reaction with benzaldehyde. link2 A dramatic cation effect is observed for the rate of interconversion of 2 and 3 and also for subsequent thermally driven formation of a twice orthometalated dinickel(II) complex 6. X-ray crystallographic and NMR titration studies indicate distinct interaction of the Lewis acidic cation with 2 and 3. The present system allows for the unmasking of a highly reactive [LPhNiI2]- intermediate 4 either via elimination of H2 from dihydride 3 or via reductive C-H elimination from monohydride 2. The latter does not release any H2 byproduct and adds a distinct platform for metal-metal cooperative two-electron substrate reductions while circumventing the isolation of any unstable superreduced form of the bimetallic scaffold.A full-dimensional global potential energy surface for the KRb + KRb → K2 + Rb2 reaction is developed from 20 759 ab initio points calculated using a coupled cluster singles, doubles, and perturbative triples (CCSD(T)) method with effective core potentials, extrapolated to the complete basis set limit. The ab initio points are represented with high fidelity (root-mean-square error of 1.86 cm-1) using the permutation-invariant polynomial-neural network method, which enforces the permutation invariance of the potential with respect to exchange of identical nuclei. The potential energy surface features two D2h minima and one Cs minimum connected by the isomerization saddle points. The Rice-Ramsperger-Kassel-Marcus lifetime of the K2Rb2 reaction intermediate estimated using the potential energy surface is 227 ns, in reasonable agreement with the latest experimental measurement.Bicelles are submicrometer-sized disc-shaped molecular self-assemblies that can be obtained in aqueous solution by dispersing mixtures of certain amphiphiles. Although phospholipid bicelle and phospholipid vesicle assemblies adopt similar lipid bilayer structures, the differences in bilayer characteristics, especially physicochemical properties such as bilayer fluidity, are not clearly understood. Herein, we report the lipid ordering properties of bicelle bilayer membranes based on induced circular dichroism (ICD) and fluorescence polarization analyses using 1,6-diphenyl-1,3,5-hexatriene (DPH) as a probe. Bicelles were prepared by using 1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC) and 1,2-dihexanoyl-sn-glycero-3-phosphocholine (DHPC), while pure DMPC vesicles and pure DHPC micelles were used as references. At temperatures below the phase transition temperature of DMPC, the bicelles showed lower membrane fluidities, whereas DHPC micelles showed higher membrane fluidity, suggesting no significant differences in bilayer fluidity between the bicelle and vesicle assemblies. The ICD signals of DPH were induced only when the membrane was in ordered (solid-ordered or ripple-gel) phases. In the bicelle systems, the ICD of DPH was more significant than that of the DMPC vesicle. The induced chirality of DPH was dependent on the chirality of the bilayer lipid. Compared to that of the DMPC/DHPC bicelle, the ICD of the 1,2-dipalmitoyl-sn-glycero-3-phosphocholine/DHPC bicelle was higher, while that of the bovine sphingomyelin/DHPC bicelle was lower. Because the lipids are tightly packed in the ordered phase, the ICD intensity reflects the molecular ordering state of the lipids in the bicelle bilayer.We present a consistent theory of energy balance and conversion in a single-molecule junction with strong interactions between electrons on the molecular linker (dot) and phonons in the nuclear environment where the Marcus-type electron hopping processes predominate in the electron transport. It is shown that the environmental reorganization and relaxation that accompany electron hopping energy exchange between the electrodes and the nuclear (molecular and solvent) environment may bring a moderate local cooling of the latter in biased systems. The effect of a periodically driven dot level on the heat transport and power generated in the system is analyzed, and energy conservation is demonstrated both within and beyond the quasistatic regime. Finally, a simple model of atomic scale engine based on a Marcus single-molecule junction with a driven electron level is suggested and discussed.A simple model of a nanofluidic transistor consisting of a uniformly charged central section between a pair of plane parallel walls is considered. The linearized Poisson-Boltzmann equation corresponding to weak surface charge is solved exactly, and the solution is presented as an infinite series. The problem is characterized by three dimensionless parameters, namely the normalized surface charge, the ratio of the channel width to the Debye length, and the length-to-width aspect ratio of the charged section. The first of these parameters is presumed small, but the other two are arbitrary. The dependence of the exclusion-enrichment effect on these three parameters is discussed.The increased demand for electronic devices, combined with a desire to minimize the environmental impact, necessitates the development of new eco-friendly materials. One promising approach is the incorporation of renewable and green materials that possess the desired mechanical and electrical properties while allowing for more ecologically friendly disposal of these devices. The addition of low-weight percentages (0.25-0.75 wt %) of cellulose nanocrystals (CNCs) was investigated as an environmentally friendly additive in aqueous dispersions of poly(vinyl alcohol) (PVA). It was found that these low CNC loadings were sufficient to induce a favorable increase in viscosity, which in turn dramatically enhanced the film quality of the PVA blends through an improvement in the critical radius of the spun film, overall film thickness, and homogeneity of the thin film. This corresponded to an increase in the number of functioning organic electronic devices that could be fabricated by spin coating, including metal-insulator-metal (MIM) capacitors and organic thin-film transistors (OTFTs). link3 Most importantly, the incorporation of CNCs into PVA did not significantly alter the native dielectric properties of the polymer thin films when incorporated into both MIM capacitors and OTFTs.In this work, using ab initio many-body theory and inspired by an idea suggested by G. D. Mahan for an abstract N-dimensional chain composed of s-type atoms ( Phys. Rev. Lett. 2009, 102, 016801), we propose a functional topological spin-charge gearbox based on the real synthesized Co3Ni(EtOH) cluster driven with laser pulses. We analyze the implications arising from the use of a real molecule with d-character functional orbitals rather than an extended system and discuss the role of the point group symmetry of the system and the transferability of the electronic and spin density between different many-body states using specially designed laser pulses. We thus find that first-row transition-metal elements can host unpaired yet correlated d electrons and thus act as sites for spin information carriers, while designated laser pulses induce symmetry operations leading to a realizable spin-charge gearbox.Organic-inorganic perovskites have attracted increasing attention in recent years owing to their excellent optoelectronic properties and photovoltaic performance. In this work, the prototypical hybrid perovskite CH3NH3PbI3 is turned into a ferromagnetic material by doping Mn, which enables simultaneous control of both charge and spin of electrons. The room-temperature ferromagnetism originates from the double exchange interaction between Mn2+-I--Mn3+ ions. Furthermore, it is discovered that the magnetic field can effectively modulate the photovoltaic properties of Mn-doped perovskite films. The photocurrent of Mn-doped perovskite solar cells increases by 0.5% under a magnetic field of 1 T, whereas the photocurrent of undoped perovskite decreases by 3.3%. These findings underscore the potential of Mn-doped perovskites as novel solution-processed ferromagnetic material and promote their application in multifunctional photoelectric-magnetic devices.