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Title: Combined subsampling and analytical integration for efficient large-scale GW calculations for 2D systems
Abstract

Accurate and efficient predictions of the quasiparticle properties of complex materials remain a major challenge due to the convergence issue and the unfavorable scaling of the computational cost with respect to the system size. QuasiparticleGWcalculations for two-dimensional (2D) materials are especially difficult. The unusual analytical behaviors of the dielectric screening and the electron self-energy of 2D materials make the conventional Brillouin zone (BZ) integration approach rather inefficient and require an extremely densek-grid to properly converge the calculated quasiparticle energies. In this work, we present a combined nonuniform subsampling and analytical integration method that can drastically improve the efficiency of the BZ integration in 2DGWcalculations. Our work is distinguished from previous work in that, instead of focusing on the intricate dielectric matrix or the screened Coulomb interaction matrix, we exploit the analytical behavior of various terms of the convolved self-energy Σ(q) in the smallqlimit. This method, when combined with another acceleratedGWmethod that we developed recently, can drastically speed up (by over three orders of magnitude)GWcalculations for 2D materials. Our method allows fully convergedGWcalculations for complex 2D systems at a fraction of computational cost, facilitating future high throughput screening of the quasiparticle properties of 2D semiconductors for various applications. To demonstrate the capability and performance of our new method, we have carried out fully convergedGWcalculations for monolayer C2N, a recently discovered 2D material with a large unit cell, and investigate its quasiparticle band structure in detail.

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NSF-PAR ID:
10181473
Author(s) / Creator(s):
; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
npj Computational Materials
Volume:
6
Issue:
1
ISSN:
2057-3960
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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    References

    Lee, D. H.; Park, H.; Clevenger, M.; Kim, H.; Kim, C. S.; Liu, M.; Kim, G.; Song, H. W.; No, K.; Kim, S. Y.; Ko, D.-K.; Lucietto, A.; Park, H.; Lee, S., High-Performance Oxide-Based p–n Heterojunctions Integrating p-SnOx and n-InGaZnO.ACS Applied Materials & Interfaces2021,13(46), 55676-55686.

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    Yim, K.; Youn, Y.; Lee, M.; Yoo, D.; Lee, J.; Cho, S. H.; Han, S., Computational discovery of p-type transparent oxide semiconductors using hydrogen descriptor.npj Computational Materials2018,4(1), 17.

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