Quality assessment of graphene： Continuity, uniformity, and accuracy of mobility measurements

With the increasing availability of large-area graphene, the ability to rapidly and accurately assess the quality of the electrical properties has become critically important. For practical applications, spatial variability in carrier density and carrier mobility must be controlled and minimized. We present a simple framework for assessing the quality and homogeneity of large-area graphene devices. The field effect in both exfoliated graphene devices encapsulated in hexagonal boron nitride and chemical vapor-deposited （CVD） devices was measured in dual current-voltage configurations and used to derive a single, gate-dependent effective shape factor, t, for each device, β is a sensitive indicator of spatial homogeneity that can be obtained from samples of arbitrary shape. All 50 devices investigated in this study show a variation （up to tenfold） in β as a function of the gate bias. Finite element simulations suggest that spatial doping inhomogeneity, rather than mobility inhomogeneity, is the primary cause of the gate dependence of β, and that measurable variations of β can be caused by doping variations as small as 10^10 cm^-2. Our results suggest that local variations in the position of the Dirac point alter the current flow and thus the effective sample shape as a function of the gate bias. We also found that such variations lead to systematic errors in carrier mobility calculations, which can be revealed by inspecting the corresponding β factor.

Beyond the RPA and GW methods with adiabatic xc-kernels for accurate ground state and quasiparticle energies

We review the theory and application of adiabatic exchange–correlation(xc)-kernels for ab initio calculations of ground state energies and quasiparticle excitations within the frameworks of the adiabatic connection fluctuation dissipation theorem and Hedin’s equations,respectively.Various different xc-kernels,which are all rooted in the homogeneous electron gas,are introduced but hereafter we focus on the specific class of renormalized adiabatic kernels,in particular the rALDA and rAPBE.The kernels drastically improve the description of short-range correlations as compared to the random phase approximation(RPA),resulting in significantly better correlation energies.This effect greatly reduces the reliance on error cancellations,which is essential in RPA,and systematically improves covalent bond energies while preserving the good performance of the RPA for dispersive interactions.For quasiparticle energies,the xc-kernels account for vertex corrections that are missing in the GW self-energy.In this context,we show that the short-range correlations mainly correct the absolute band positions while the band gap is less affected in agreement with the known good performance of GW for the latter.The renormalized xc-kernels offer a rigorous extension of the RPA and GW methods with clear improvements in terms of accuracy at little extra computational cost.

Exploring and machine learning structural instabilities in 2D materials

We address the problem of predicting the zero-temperature dynamical stability (DS) of a periodic crystal without computing its fullphonon band structure. Here we report the evidence that DS can be inferred with good reliability from the phonon frequencies atthe center and boundary of the Brillouin zone (BZ). This analysis represents a validation of the DS test employed by theComputational 2D Materials Database (C2DB). For 137 dynamically unstable 2D crystals, we displace the atoms along an unstablemode and relax the structure. This procedure yields a dynamically stable crystal in 49 cases. The elementary properties of these newstructures are characterized using the C2DB workflow, and it is found that their properties can differ significantly from those of theoriginal unstable crystals, e.g., band gaps are opened by 0.3 eV on average. All the crystal structures and properties are available inthe C2DB. Finally, we train a classification model on the DS data for 3295 2D materials in the C2DB using a representation encodingthe electronic structure of the crystal. We obtain an excellent receiver operating characteristic (ROC) curve with an area under thecurve (AUC) of 0.90, showing that the classification model can drastically reduce computational efforts in high-throughput studies.

Shift current photovoltaic efficiency of 2D materials

Shift current photovoltaic devices are potential candidates for future cheap,sustainable,and efficient electricity generation.In the present work,we calculate the solar-generated shift current and efficiencies in 326 different 2D materials obtained from the computational database C2DB.We apply,as metrics,the efficiencies of monolayer and multilayer samples.The monolayer efficiencies are generally found to be low,while the multilayer efficiencies of infinite stacks show great promise.Furthermore,the out-of-plane shift current response is considered,and material candidates for efficient out-of-plane shift current devices are identified.Among the screened materials,MXY Janus and MX_(2) transition metal dichalchogenides(TMDs)constitute a prominent subset,with chromium based MXY Janus TMDs holding particular promise.Finally,in order to explain the band gap dependence of the PV efficiency,a simple gapped graphene model with a variable band gap is established and related to the calculated efficiencies.

Towards fully automated GW band structure calculations:What we can learn from 60.000 self-energy evaluationsTowards fully automated GW band structure calculations:What we can learn from 60.000 self-energy evaluations

We analyze a data set comprising 370 GW band structures of two-dimensional(2D)materials covering 14 different crystal structures and 52 chemical elements.The band structures contain a total of 61716 quasiparticle(QP)energies obtained from plane-wavebased one-shot G0W0@PBE calculations with full frequency integration.We investigate the distribution of key quantities,like the QP self-energy corrections and QP weights,and explore their dependence on chemical composition and magnetic state.The linear QP approximation is identified as a significant error source and we propose schemes for controlling and drastically reducing this error at low computational cost.We analyze the reliability of the 1/N basis set extrapolation and find that is well-founded with a narrow distribution of coefficients of determination(r^(2))peaked very close to 1.Finally,we explore the accuracy of the scissors operator approximation and conclude that its validity is very limited.Our work represents a step towards the development of automatized workflows for high-throughput G0W0 band structure calculations for solids.