Determining the adsorption potential of adsorbed ions in the field of computational electrocatalysis is of great interest to study their interaction with the electrode material and the solvent, and... Show moreDetermining the adsorption potential of adsorbed ions in the field of computational electrocatalysis is of great interest to study their interaction with the electrode material and the solvent, and to map out surface phase diagrams and reaction pathways. Calculating the adsorption potentials of ions with density functional theory and comparing across various ions requires an accurate reference energy of the ion in solution and electrons at the same electrochemical scale. Here we highlight a previously used method for determining the reference free energy of solution phase ions using a simple electrochemical thermodynamic cycle, which allows this free energy to be calculated from that of a neutral gas-phase or solid species and an experimentally measured equilibrium potential, avoiding the need to model solvent around the solution phase ion in the electronic structure calculations. While this method is not new, we describe its use and utility in detail and show that this same method can be used to find the free energy of any ion from any reaction, as long as the half-cell equilibrium potential is known, even for reactions that do not transfer the same number of protons and electrons. To illustrate its usability, we compare the adsorption potentials obtained with DFT of I*, Br*, Cl*, and SO4 * on Pt(111) and Au(111) and OH* and Ag* on Pt(111) with those measured experimentally and find that this simple and computationally affordable method reproduces the experimental trends. Show less
Lebedev, N.; Stehno, M.; Rana, A.; Gauquelin, N.; Verbeeck, J.; Brinkman, A.; Aarts, J. 2020
We have studied the transport properties of LaTiO3/SrTiO3 (LTO/STO) heterostructures. In spite of 2D growth observed in reflection high energy electron diffraction, transmission electron microscopy... Show moreWe have studied the transport properties of LaTiO3/SrTiO3 (LTO/STO) heterostructures. In spite of 2D growth observed in reflection high energy electron diffraction, transmission electron microscopy images revealed that the samples tend to amorphize. Still, we observe that the structures are conducting, and some of them exhibit high conductance and/or superconductivity. We established that conductivity arises mainly on the STO side of the interface, and shows all the signs of the two-dimensional electron gas usually observed at interfaces between STO and LTO or LaAlO3, including the presence of two electron bands and tunability with a gate voltage. Analysis of magnetoresistance (MR) and superconductivity indicates the presence of spatial fluctuations of the electronic properties in our samples. That can explain the observed quasilinear out-of-plane MR, as well as various features of the in-plane MR and the observed superconductivity. Show less
Bossoni, L.; Grand Moursel, L.; Bulk, M.; Simon, B.G.; Webb, A.; Weerd, L. van der; ... ; Oosterkamp, T.H. 2017
Amorphous materials as diverse as foams, emulsions, colloidal suspensions and granular media can jam into a rigid, disordered state where they withstand finite shear stresses before yielding. Here... Show moreAmorphous materials as diverse as foams, emulsions, colloidal suspensions and granular media can jam into a rigid, disordered state where they withstand finite shear stresses before yielding. Here we review the current understanding of the transition to jamming and the nature of the jammed state for disordered packings of particles that act through repulsive contact interactions and are at zero temperature and zero shear stress. We first discuss the breakdown of affine assumptions that underlies the rich mechanics near jamming. We then extensively discuss jamming of frictionless soft spheres. At the jamming point, these systems are marginally stable (isostatic) in the sense of constraint counting, and many geometric and mechanical properties scale with distance to this jamming point. Finally, we discuss current explorations of jamming of frictional and non-spherical (ellipsoidal) particles. Both friction and asphericity tune the contact number at jamming away from the isostatic limit, but in opposite directions. This allows one to disentangle the distance to jamming and the distance to isostaticity. The picture that emerges is that most quantities are governed by the contact number and scale with the distance to isostaticity, while the contact number itself scales with the distance to jamming. Show less