We have performed electronic structure calculations of the interaction of potassium and oxygen with graphite (GR), individually and as coadsorbates. We use up to three graphite planes to represent the graphite surface, but we show that the main physics is correctly described by a single graphite layer. At low coverage the potassium–graphite bond is largely ionic, and the variation of the K–GR bond energy with the lateral position of the K atom in the graphite unit cell is very small. We study the interaction between atomic oxygen and graphite. We find that O binds strongest at the bridge site, but the barrier for diffusion is rather small. The frequency for the perpendicular O–graphite vibrational mode is remarkably low (53 meV), reflecting the relative slow variation of the O–graphite interaction energy with the separation z between the O atom and the graphite surface. We consider the adsorption of O2 on a clean graphite surface and on a graphite surface with a low concentration of potassium. On the clean surface the O2–graphite interaction is found to be repulsive (the weak attractive van der Waals interaction is not included in our theoretical method), in accordance with the extremely low sticking coefficient observed for O2 on clean graphite. When potassium is adsorbed on the graphite surface, O2 chemisorbs at the potassium sites which is consistent with the large sticking coefficient observed for O2 on a potassium covered surface. The energy barrier towards dissociation of O2 on the clean graphite surface is estimated to be similar to that of gas phase O2. For O2 on K/graphite we find that O2 chemisorbs “side-on” K, and that the barrier for dissociation is much smaller than in the gas phase or on the clean graphite surface.

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Solar-energy plays an important role in solving serious environmental problems and meeting highenergy demand. However, the lack of suitable materials hinders further progress of this technology. Here, we present the largest inorganic solar-cell material search to date using density functional theory (DFT) and machine-learning approaches. We calculated the spectroscopic limited maximum efficiency (SLME) using Tran-Blaha modified Becke-Johnson potential for 5097 non-metallic materials and identified 1997 candidates with an SLME higher than 10%, including 934 candidates with suitable convex-hull stability and effective carrier mass. Screening for 2D-layered cases, we found 58 potential materials and performed G0W0 calculations on a subset to estimate the prediction-uncertainty. As the above DFT methods are still computationally expensive, we developed a high accuracy machine learning model to pre-screen efficient materials and applied it to over a million materials. Our results provide a general framework and universal strategy for the design of high-efficiency solar cell materials. The data and tools are publicly 2 distributed at:

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For two model systems, a dimer of N,N‘-dimethyl thiacarbocyanine and a dimer of C.I. Pigment Yellow 12, we compare results of several approaches to calculation of the exciton interaction energy. The sum over Coulombic interactions between atomic transition charges is compared to the point-dipole and extended-dipole approximations and to the direct evaluation of the Coulomb interaction integral over transition charge densities, for a range of dimer configurations. Calculations are carried out at semiempirical, ab initio Hartree−Fock, and ab initio configuration interaction−singles levels. Finally, we discuss the relation of these interaction energies to those calculated using a supermolecular approach. We conclude that for the materials studied, semiempirical methods are adequate to describe the excitonic shift.

Fulfillment of the promise of transparent electronics has been hindered until now largely by the lack of semiconductors that can be doped p-type in a stable way, and that at the same time present high hole mobility and are highly transparent in the visible spectrum. Here, a high-throughput study based on first-principles methods reveals four oxides, namely X2SeO2, with X = La, Pr, Nd, and Gd, which are unique in that they exhibit excellent characteristics for transparent electronic device applications – i.e., a direct band gap larger than 3.1 eV, an average hole effective mass below the electron rest mass, and good p-type dopability. Furthermore, for La2SeO2 it is explicitly shown that Na impurities substituting La are shallow acceptors in moderate to strong anion-rich growth conditions, with low formation energy, and that they will not be compensated by anion vacancies VO or VSe.

We present electronic band structures of transparent oxides calculated using the Tran-Blaha modified Becke-Johnson (TB-mBJ) potential. We studied the basic n-type conducting binary oxides In(2)O(3), ZnO, CdO and SnO(2) along with the p-type conducting ternary oxides delafossite CuXO(2) (X=Al, Ga, In) and spinel ZnX(2)O(4) (X=Co, Rh, Ir). The results are presented for calculated band gaps and effective electron masses. We discuss the improvements in the band gap determination using TB-mBJ compared to the standard generalized gradient approximation (GGA) in density functional theory (DFT) and also compare the electronic band structure with available results from the quasiparticle GW method. It is shown that the calculated band gaps compare well with the experimental and GW results, although the electron effective mass is generally overestimated.