Efficient first-principles calculation of phonon assisted photocurrent in large-scale solar cell devices

We present a straightforward and computationally cheap method to obtain the phonon-assisted photocurrent in large-scale devices from first-principles transport calculations. The photocurrent is calculated using nonequilibrium Green's function with light-matter interaction from the first-order Born approximation while electron-phonon coupling (EPC) is included through special thermal displacements (STD). We apply the method to a silicon solar cell device and demonstrate the impact of including EPC in order to properly describe the current due to the indirect band-to-band transitions. The first-principles results are successfully compared to experimental measurements of the temperature and light intensity dependence of the open-circuit voltage of a silicon photovoltaic module. Our calculations illustrate the pivotal role played by EPC in photocurrent modelling to avoid underestimation of the open-circuit voltage, short-circuit current and maximum power. This work represents a recipe for computational characterization of future photovoltaic devices including the combined effects of light-matter interaction, phonon-assisted tunneling and the device potential at finite bias from the level of first-principles simulations

Electron-phonon scattering from Green's function transport combined with Molecular Dynamics: Applications to mobility predictions

We present a conceptually simple method for treating electron-phonon scattering and phonon limited mobilities. By combining Green's function based transport calculations and molecular dynamics (MD), we obtain a temperature dependent transmission from which we evaluate the mobility. We validate our approach by comparing to mobilities and conductivies obtained by the Boltzmann transport equation (BTE) for different bulk and one-dimensional systems. For bulk silicon and gold we successfully compare against experimental values. We discuss limitations and advantages of each of the computational approaches.Comment: 8 pages, 8 figure

Unravelling the role of inelastic tunneling into pristine and defected graphene

We present a first principles method for calculating the inelastic electron tunneling spectroscopy (IETS) on gated graphene. We reproduce experiments on pristine graphene and point out the importance of including several phonon modes to correctly estimate the local doping from IETS. We demonstrate how the IETS of typical imperfections in graphene can yield characteristic fingerprints revealing e.g. adsorbate species or local buckling. Our results show how care is needed when interpreting STM images of defects due to suppression of the elastic tunneling on graphene

First-principles electron transport with phonon coupling: Large scale at low cost

Phonon-assisted tunneling plays a crucial role for electronic device performance and even more so with future size down-scaling. We show how one can include this effect in large-scale first-principles calculations using a single "special thermal displacement" (STD) of the atomic coordinates at almost the same cost as elastic transport calculations. We apply the method to ultra-scaled silicon devices and demonstrate the importance of phonon-assisted band-to-band and source-to-drain tunneling. In a diode the phonons lead to a rectification ratio suppression in good agreement with experiments, while in an ultra-thin body transistor the phonons increase off-currents by four orders of magnitude, and the subthreshold swing by a factor of four, in agreement with perturbation theory

Interface band gap narrowing behind open circuit voltage losses in Cu₂ZnSnS₄ solar cells

We present evidence that band gap narrowing at the heterointerface may be a major cause of the large open circuit voltage deficit of Cu$_2$ZnSnS$_4$/CdS solar cells. Band gap narrowing is caused by surface states that extend the Cu$_2$ZnSnS$_4$ valence band into the forbidden gap. Those surface states are consistently found in Cu$_2$ZnSnS$_4$, but not in Cu$_2$ZnSnSe$_4$, by first-principles calculations. They do not simply arise from defects at surfaces but are an intrinsic feature of Cu$_2$ZnSnS$_4$ surfaces. By including those states in a device model, the outcome of previously published temperature-dependent open circuit voltage measurements on Cu$_2$ZnSnS$_4$ solar cells can be reproduced quantitatively without necessarily assuming a cliff-like conduction band offset with the CdS buffer layer. Our first-principles calculations indicate that Zn-based alternative buffer layers are advantageous due to the ability of Zn to passivate those surface states. Focusing future research on Zn-based buffers is expected to significantly improve the open circuit voltage and efficiency of pure-sulfide Cu$_2$ZnSnS$_4$ solar cells.Comment: Accepted at Applied Physics Letter

Stacked Janus Device Concepts: Abrupt pn-Junctions and Cross-Plane Channels

Janus transition metal dichalcogenides with a built-in structural cross-plane (cp) asymmetry have recently emerged as a new class of two-dimensional materials with a large cp dipole. Using first-principles calculations, and a tailored transport method, we demonstrate that stacking graphene and MoSSe Janus structures result in record high homogeneous doping of graphene and abrupt, atomically thin, cross-plane pn-junctions. We show how graphene in contrast to metals can act as electrodes to Janus stacks without screening the cp dipole and predict a large photocurrent response dominated by a cp transport channel in a few-layer stacked device. The photocurrent is above that of a corresponding thin-film silicon device illustrating the great potential of Janus stacks, for example, in photovoltaic devices

QuantumATK: An integrated platform of electronic and atomic-scale modelling tools

QuantumATK is an integrated set of atomic-scale modelling tools developed since 2003 by professional software engineers in collaboration with academic researchers. While different aspects and individual modules of the platform have been previously presented, the purpose of this paper is to give a general overview of the platform. The QuantumATK simulation engines enable electronic-structure calculations using density functional theory or tight-binding model Hamiltonians, and also offers bonded or reactive empirical force fields in many different parametrizations. Density functional theory is implemented using either a plane-wave basis or expansion of electronic states in a linear combination of atomic orbitals. The platform includes a long list of advanced modules, including Green's-function methods for electron transport simulations and surface calculations, first-principles electron-phonon and electron-photon couplings, simulation of atomic-scale heat transport, ion dynamics, spintronics, optical properties of materials, static polarization, and more. Seamless integration of the different simulation engines into a common platform allows for easy combination of different simulation methods into complex workflows. Besides giving a general overview and presenting a number of implementation details not previously published, we also present four different application examples. These are calculations of the phonon-limited mobility of Cu, Ag and Au, electron transport in a gated 2D device, multi-model simulation of lithium ion drift through a battery cathode in an external electric field, and electronic-structure calculations of the composition-dependent band gap of SiGe alloys.Comment: Submitted to Journal of Physics: Condensed Matte