LOBSTER: Local Orbital Projections, Atomic Charges, and Chemical Bonding Analysis from Projector-Augmented-Wave-Based DFT

Abstract

<jats:p>We present an update on recently developed methodology and functionality in the computer program LOBSTER (Local Orbital Basis Suite Towards Electronic-Structure Reconstruction) for chemical-bonding analysis in periodic systems. LOBSTER is based on an analytic projection from projector-augmented wave (PAW) densityfunctional theory (DFT) computations [J. Comput. Chem. 2013, 34, 2557], reconstructing chemical information in terms of local, auxiliary atomic orbitals and thereby opening the output of PAW-based DFT codes to chemical interpretation. We demonstrate how LOBSTER has been improved by taking into account time reversal symmetry, thereby speeding up the DFT and LOBSTER calculations by a factor of 2. Over the recent years, the functionalities have also been continually expanded, including accurate projected densities of states (DOS), crystal orbital Hamilton population (COHP) analysis, atomic and orbital charges, gross populations, and the recently introduced 𝒌-dependent COHP. The software is offered free-of-charge for non-commercial research.</jats:p>

The Hydrogen Evolution Activity of BaZrS3, BaTiS3, and BaVS3 Chalcogenide Perovskites

“…Our analysis is inspired by a computational study examining correlations between bulk and surface properties of cubic strontium perovskite oxides carried out by Fung and coworkers. [43] By plotting COHP [40][41][42] and estimating ICOHP for the perovskite oxides, they show that the reactivity of oxygen is correlated with ICOHP -increasing as the number of delectrons increases (Ti!Zn) or going up a group (Zr!Ti). This is because the metal-oxygen bond weakens, reflected in the increasing antibonding population in COHP and consequently higher (more positive) value of ICOHP.…”

“…where DE DFT is the electronic energy, DE ZPE is the zero point energy obtained from vibrational analysis, DU is the internal energy corresponding to the vibrational enthalpy contributions excluding the zero point energies, and TDS is calculated at 298 K, and accounts for the loss of translational and rotational degrees of freedom from the gas phase upon adsorption of H 2 . [7,39] We calculate the crystal orbital Hamilton population (COHP), [40][41][42] a product of the DOS and the overlap Hamiltonian element, to probe potential correlations between bulk properties and surface chemistry of these materials. [43]…”

Graph neural network with classification accelerating the discovery of Heusler catalysts for nitrogen reduction reaction

“…As depicted in Fig. 6d, when N2 is adsorbed on Ru, the Integrated Crystal Orbital Hamilton Population (ICOHP) 49 between N and Hf is close to zero, indicating no significant bonding or anti-bonding interactions. In this case, N2 activation primarily arises from the filling of the anti-bonding 𝜋 2𝑝 * orbitals of N by Ru.…”

Co-alloying of Sn and Te enables high thermoelectric performance in Ag9GaSe6

“…The plane wave energy cutoff was set to 400 eV for all calculations. The projected crystal orbital Hamilton population (pCOHP) was calculated through the LOBSTER code 41 based on a ground state self-consistent calculation from VASP. The Brillouin zone was sampled by 3 × 3 × 3 G-centered k mesh for structural relaxations and charge density calculations, and by 9 × 9 × 9 G-centered k mesh for COHP calculations.…”