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Register a new userHigh-accuracy large-scale DFT calculations using localized orbitals in complex electronic systems: The case of graphene-metal interfaces
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Over many years, computational simulations based on Density Functional Theory (DFT) have been used extensively to study many different materials at the atomic scale. However, its application is restricted by system size, leaving a number of interesting systems without a high-accuracy quantum description. In this work, we calculate the electronic and structural properties of a graphene-metal system significantly larger than in previous plane-wave calculations with the same accuracy. For this task we use a localised basis set with the textsc{Conquest} code, both in their primitive, pseudo-atomic orbital form, and using a recent multi-site approach. This multi-site scheme allows us to maintain accuracy while saving computational time and memory requirements, even in our exemplar complex system of graphene grown on Rh(111) with and without intercalated atomic oxygen. This system offers a rich scenario that will serve as a benchmark, demonstrating that highly accurate simulations in cells with over 3000 atoms are feasible with modest computational resources.
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Using large-scale DFT calculations, we have investigated the structural and electronic properties of both armchair and zigzag graphdiyne nanotubes as a function of size. To provide insight in these properties, we present new detailed calculations of the structural relaxation energy, effective electron/hole mass, and size-scaling of the bandgap as a function of size and chirality using accurate screened-exchange DFT calculations. These calculations provide a systematic evaluation of the structural and electronic properties of the largest graphdiyne nanotubes to date - up to 1,296 atoms and 23,328 basis functions. Our calculations find that zigzag graphdiyne nanotubes (GDNTs) are structurally more stable compared to armchair GDNTs of the same size. Furthermore, these large-scale calculations allow us to present simple analytical formulae to guide future experimental efforts for estimating the fundamental bandgaps of these unique nanotubes as a function of chirality and diameter. While the bandgaps for both the armchair and zigzag GDNTs can be tuned as a function of size, the conductivity in each of these two different chiralities is markedly different. Zigzag GDNTs have wider valence and conduction bands and are expected to have a higher electron- and hole-mobility than their armchair counterparts.
We present an efficient, linear-scaling implementation for building the (screened) Hartree-Fock exchange (HFX) matrix for periodic systems within the framework of numerical atomic orbital (NAO) basis functions. Our implementation is based on the localized resolution of the identity approximation by which two-electron Coulomb repulsion integrals can be obtained by only computing two-center quantities -- a feature that is highly beneficial to NAOs. By exploiting the locality of basis functions and efficient prescreening of the intermediate three- and two-index tensors, one can achieve a linear scaling of the computational cost for building the HFX matrix with respect to the system size. Our implementation is massively parallel, thanks to a MPI/OpenMP hybrid parallelization strategy for distributing the computational load and memory storage. All these factors add together to enable highly efficient hybrid functional calculations for large-scale periodic systems. In this work we describe the key algorithms and implementation details for the HFX build as implemented in the ABACUS code package. The performance and scalability of our implementation with respect to the system size and the number of CPU cores are demonstrated for selected benchmark systems up to 4096 atoms.
We investigate the effect of charge self-consistency (CSC) in density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations compared to simpler one-shot calculations for materials where interaction effects lead to a strong redistribution of electronic charges between different orbitals or between different sites. We focus on two systems close to a metal-insulator transition, for which the importance of CSC is currently not well understood. Specifically, we analyze the strain-related orbital polarization in the correlated metal CaVO$_3$ and the spontaneous electronic charge disproportionation in the rare-earth nickelate LuNiO$_3$. In both cases, we find that the CSC treatment reduces the charge redistribution compared to cheaper one-shot calculations. However, while the MIT in CaVO$_3$ is only slightly shifted due to the reduced orbital polarization, the effect of the site polarization on the MIT in LuNiO$_3$ is more subtle. Furthermore, we highlight the role of the double-counting correction in CSC calculations containing different inequivalent sites.
The semiconductor-metal junction is one of the most critical factors for high performance electronic devices. In two-dimensional (2D) semiconductor devices, minimizing the voltage drop at this junction is particularly challenging and important. Despite numerous studies concerning contact resistance in 2D semiconductors, the exact nature of the buried interface under a three-dimensional (3D) metal remains unclear. Herein, we report the direct measurement of electrical and optical responses of 2D semiconductor-metal buried interfaces using a recently developed metal-assisted transfer technique to expose the buried interface which is then directly investigated using scanning probe techniques. We characterize the spatially varying electronic and optical properties of this buried interface with < 20 nm resolution. To be specific, potential, conductance and photoluminescence at the buried metal/MoS2 interface are correlated as a function of a variety of metal deposition conditions as well as the type of metal contacts. We observe that direct evaporation of Au on MoS2 induces a large strain of ~5% in the MoS2 which, coupled with charge transfer, leads to degenerate doping of the MoS2 underneath the contact. These factors lead to improvement of contact resistance to record values of 138 kohm-um, as measured using local conductance probes. This approach was adopted to characterize MoS2-In/Au alloy interfaces, demonstrating contact resistance as low as 63 kohm-um. Our results highlight that the MoS2/Metal interface is sensitive to device fabrication methods, and provides a universal strategy to characterize buried contact interfaces involving 2D semiconductors.
Novel electronic systems forming at oxide interfaces comprise a class of new materials with a wide array of potential applications. A high mobility electron system forms at the LaAlO$_3$/SrTiO$_3$ interface and, strikingly, both superconducts and displays indications of hysteretic magnetoresistance. An essential step for device applications is establishing the ability to vary the electronic conductivity of the electron system by means of a gate. We have fabricated metallic top gates above a conductive interface to vary the electron density at the interface. By monitoring capacitance and electric field penetration, we are able to tune the charge carrier density and establish that we can completely deplete the metallic interface with small voltages. Moreover, at low carrier densities, the capacitance is significantly enhanced beyond the geometric capacitance for the structure. In the same low density region, the metallic interface overscreens an external electric field. We attribute these observations to a negative compressibility of the electronic system at the interface. Similar phenomena have been observed previously in semiconducting two-dimensional electronic systems. The observed compressibility result is consistent with the interface containing a system of mobile electrons in two dimensions.
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