Communication: An adaptive configuration interaction approach for strongly correlated electrons with tunable accuracy
We introduce a new procedure for iterative selection of determinant spaces capable of describing highly correlated systems. This adaptive configuration interaction (ACI) determines an optimal basis by an iterative procedure in which the determinant space is expanded and coarse grained until self-consistency. Two importance criteria control the selection process and tune the ACI to a user-defined level of accuracy. The ACI is shown to yield potential energy curves of N2 with nearly constant errors, and it predicts singlet-triplet splittings of acenes up to decacene that are in good agreement with the density matrix renormalization group.
Effect of ethanol concentrations on temperature driven structural changes of chymotrypsin inhibitor 2
A series of atomistic molecular dynamics (MD) simulations of a small enzymatic protein Chymotrypsin Inhibitor 2 (CI2) in water-ethanol mixed solutions were carried out to explore the underlying mechanism of ethanol driven conformational changes of the protein. Efforts have been made to probe the influence of ethanol concentrations ranging from 0% to 75% (v/v) at ambient condition (300 K (T1)) and at elevated temperatures (375 K (T2) and 450 K (T3)) to investigate the temperature induced conformational changes of the protein further. Our study showed that the effect of varying ethanol concentrations on protein’s structure is almost insignificant at T1 and T2 temperatures whereas at T3 temperature, partial unfolding of CI2 in 10% ethanol solution followed by full unfolding of the protein at ethanol concentrations above 25% occurs. However, interestingly, at T3 temperature CI2’s native structure was found to be retained in pure water (0% ethanol solution) indicating that the cosolvent ethanol do play an important role in thermal denaturation of CI2. Such observations were quantified in the light of root-mean-square deviations (RMSDs) and radius of gyration. Although higher RMSD values of β-sheet over α-helix indicate complete destruction of the β-structure of CI2 at high ethanol concentrations, the associated time scale showed that the faster melting of α-helix happens over β-sheet. Around 60%-80% of initial native contacts of the protein were found broken with the separation of hydrophobic core consisting eleven residues at ethanol concentrations greater than 25%. This leads protein to expand with the increase in solvent accessible surface area. The interactions between protein and solvent molecules showed that protein’s solvation shell preferred to accommodate ethanol molecules as compared to water thereby excluded water molecules from CI2’s surface. Further, concentration dependent differential self-aggregation behavior of ethanol is likely to regulate the replacement of relatively fast diffused water by low diffused ethanol molecules from protein’s surface during the unfolding process.
The impact of the solvent on the photodissociation of embedded molecules has been intensively investigated in the last decades. Collisions of photofragments with the solvating atoms or molecules can change their kinetic energy distribution or even lead to the de-excitation of the dissociating molecule to a bound electronic state quenching the dissociation. In this article we show that this cage effect is strongly enhanced if interatomic Coulombic decay (ICD) of the excited state becomes allowed. Ab initio calculations in H2O–Cl− cluster show that the ultra-fast dissociation of water in the Ãexcited state is strongly quenched by ICD. We found that this very efficient quenching is due to two factors. First, the lifetimes of the Ã state due to ICD are short ranging between 6 and 30 fs. Second, nuclear dynamics is dominated by the chattering motion of the H atom between O and Cl− allowing ICD to act for longer times. We hope that this work will be an important first step in clarifying the impact of ICD on photodissociation of embedded molecules.
This paper presents a novel piezoelectric energy harvester, which is a MEMS-based device. This piezoelectric energy harvester uses a bifurcate-shape. The derivation of the mathematical modeling is based on the Euler-Bernoulli beam theory, and the main mechanical and electrical parameters of this energy harvester are analyzed and simulated. The experiment result shows that the maximum output voltage can achieve 3.3V under an acceleration of 1g at 292.11Hz of frequency, and the output power can be up to 0.155mW under the load of 0.4MΩ. The power density is calculated as 496.79μWmm−3. Besides that, it is demonstrated efficiently at output power and voltage and adaptively in practical vibration circumstance. This energy harvester could be used for low-power electronic devices.
Link between hopping models and percolation scaling laws for charge transport in mixtures of small molecules
Mixed host compositions that combine chargetransportmaterials with luminescent dyes offer superior control over exciton formation and chargetransport in organic light emitting devices (OLEDs). Two approaches are typically used to optimize the fraction of chargetransportmaterials in a mixed host composition: either an empirical percolative model, or a hopping transport model. We show that these two commonly-employed models are linked by an analytic expression which relates the localization length to the percolation threshold and critical exponent. The relation is confirmed both numerically and experimentally through measurements of the relative conductivity of Tris(4-carbazoyl-9-ylphenyl)amine (TCTA) :1,3-bis(3,5-dipyrid-3-yl-phenyl)benzene (BmPyPb) mixtures with different concentrations, where the TCTA plays a role as hole conductor and the BmPyPb as hole insulator. The analytic relation may allow the rational design of mixed layers of small molecules for high-performance OLEDs.
The nonlinear Vlasov equation contains the full nonlinear dynamics and collective effects of a given Hamiltonian system. The linearized approximation is not valid for a variety of interesting systems, nor is it simple to extend to higher order. It is also well-known that the linearized approximation to the Vlasov equation is invalid for long times, due to its inability to correctly capture fine phase space structures. We derive a perturbation theory for the Vlasov equation based on the underlying Hamiltonian structure of the phase space evolution. We obtain an explicit perturbation series for a dressed Hamiltonian applicable to arbitrary systems whose dynamics can be described by the nonlinear Vlasov equation.
We prove that the bound state energies of the two-dimensional massive Dirac operator with dipole type potentials accumulate with exponential rate at the band edge. In fact we prove a corresponding formula of De Martino et al. [Phys. Rev. Lett. 112(18), 186603 (2014)].