Search for: All records

We perform first-principles calculations to explore the electronic, thermodynamic and dielectric properties of two-dimensional (2D) layered, alkaline-earth hydroxides Ca(OH)2 and Mg(OH)2. We calculate the lattice parameters, exfoliation energies and phonon spectra of monolayers and also investigate the thermal properties of these monolayers, such as the Helmholtz free energy, heat capacity at constant volume and entropy as a function of temperature. We employ Density Functional Perturbation Theory (DFPT) to calculate the in-plane and out-of-plane static dielectric constant of the bulk and monolayer samples. We compute the bandgap and electron affinity values using the HSE06 functional and estimate the leakage current density of transistors with monolayer Ca(OH)2 and Mg(OH)2 as dielectrics when combined with HfS2 and WS2, respectively. Our results show that bilayer Mg(OH)2 (EOT∼0.60 nm) with a lower solubility in water offers higher out-of-plane dielectric constants and lower leakage currents than does bilayer Ca(OH)2 (EOT∼0.56 nm). Additionally, the out-of-plane dielectric constant, leakage current and EOT of Mg(OH)2 outperform bilayer h-BN. We verify the applicability of Anderson’s rule and conclude that bilayers of Ca(OH)2 and Mg(OH)2, respectively, paired with lattice-matched monolayer HfS2 and WS2, are effective structural combinations that could lead to the development of innovative multi-functional Field Effect Transistors (FETs). 

Topological insulators open many avenues for designing future electronic devices. Using the Bardeen transfer Hamiltonian method, we calculate the current density of electron tunneling between two slabs of Bi2Se3. 3D TI tunnel diode current-voltage characteristics are calculated for different doping concentrations, tunnel barrier height and thickness, and 3D TI bandgap. The difference in the Fermi levels of the slabs determines the peak and trough voltages. The tunnel barrier width and height affect the magnitude of the current without affecting the shape of the current-voltage characteristics. The bandgap of the 3D TI determines the magnitude of the tunnel current, albeit at a lesser rate than the tunnel barrier potential, thus the device characteristics are robust under changing TI material. The high peak-to-trough ratio of 3D TI tunnel diodes, the controllabilty of the trough current location, and the simple construction provide advantages over other NDR devices. 

We study the magnetic properties of platinum diselenide (PtSe2) intercalated with Ti, V, Cr, and Mn, using first-principle density functional theory (DFT) calculations and Monte Carlo (MC) simulations. First, we present the equilibrium position of intercalants in PtSe2 obtained from the DFT calculations. Next, we present the magnetic groundstates for each of the intercalants in PtSe2 along with their critical temperature. We show that Ti intercalants result in an in-plane AFM and out-of-plane FM groundstate, whereas Mn intercalant results in in-plane FM and out-of-plane AFM. V intercalants result in an FM groundstate both in the in-plane and the out-of-plane direction, whereas Cr results in an AFM groundstate both in the in-plane and the out-of-plane direction. We find a critical temperature of <0.01 K, 111 K, 133 K, and 68 K for Ti, V, Cr, and Mn intercalants at a 7.5% intercalation, respectively. In the presence of Pt vacancies, we obtain critical temperatures of 63 K, 32 K, 221 K, and 45 K for Ti, V, Cr, and Mn-intercalated PtSe2, respectively. We show that Pt vacancies can change the magnetic groundstate as well as the critical temperature of intercalated PtSe2, suggesting that the magnetic groundstate in intercalated PtSe2 can be controlled via defect engineering. 

Although cyclic voltammetry (CV) measurements in solution have been widely used to determine the highest occupied molecular orbital energy (E_HOMO) of semiconducting organic molecules, an understanding of the experimentally observed discrepancies due to the solvent used is lacking. To explain these differences, we investigate the solvent effects onE_HOMOby combining density functional theory and molecular dynamics calculations for four donor molecules with a common backbone moiety. We compare the experimentalE_HOMOvalues to the calculated values obtained from either implicit or first solvation shell theories. We find that the first solvation shell method can capture theE_HOMOvariation arising from the functional groups in solution, unlike the implicit method. We further applied the first solvation shell method to other semiconducting organic molecules measured in solutions for different solvents. We find that theE_HOMOobtained using an implicit method is insensitive to solvent choice. The first solvation shell, however, producesE_HOMOvalues that are sensitive to solvent choices and agrees with published experimental results. The solvent sensitivity arises from a hierarchy of three effects: (1) the solute electronic state within a surrounding dielectric continuum, (2) ambient temperature or solvent atoms changing the solute geometry, and (3) electronic interactions between the solute and solvents. The implicit method, on the other hand, only captures the effect of a dielectric environment. Our findings suggest thatE_HOMOobtained by CV measurements should account for the influence of solvent when the results are reported, interpreted, or compared to other molecules.