Please use this identifier to cite or link to this item: https://doi.org/10.1021/acs.jctc.9b00229
Title: Quasiparticle Levels at Large Interface Systems from Many-Body Perturbation Theory: The XAF-GW Method
Authors: Xuan, Fengyuan 
Chen, Yifeng 
Quek, Su Ying 
Keywords: Science & Technology
Physical Sciences
Chemistry, Physical
Physics, Atomic, Molecular & Chemical
Chemistry
Physics
MONOLAYER
RENORMALIZATION
THICKNESS
ALIGNMENT
AU(111)
AG(111)
BANDGAP
PTCDA
Issue Date: 1-Jun-2019
Publisher: AMERICAN CHEMICAL SOCIETY
Citation: Xuan, Fengyuan, Chen, Yifeng, Quek, Su Ying (2019-06-01). Quasiparticle Levels at Large Interface Systems from Many-Body Perturbation Theory: The XAF-GW Method. JOURNAL OF CHEMICAL THEORY AND COMPUTATION 15 (6) : 3824-3835. ScholarBank@NUS Repository. https://doi.org/10.1021/acs.jctc.9b00229
Abstract: © 2019 American Chemical Society. We present a fully ab initio approach based on many-body perturbation theory in the GW approximation to compute the quasiparticle levels of large interface systems without significant covalent interactions between the different components of the interface (meaning that the different components can be separated without the creation of dangling bonds). The only assumption in our approach is that the polarizability matrix (chi) of the interface can be given by the sum of the polarizability matrices of individual components of the interface. We show analytically, using a two-state hybridized model, that this assumption is valid even in the presence of interface hybridization to form bonding and antibonding states up to first order in the overlap matrix elements involved in the hybridization. We validate our approach by showing that the band structure obtained in our method is almost identical to that obtained using a regular GW calculation for bilayer black phosphorus, where interlayer hybridization is significant. Significant savings in computational time and memory are obtained by computing chi only for the smallest subunit cell of each component and expanding (unfolding) the chi matrix to that in the unit cell of the interface. To treat interface hybridization, the full wave functions of the interface are used in computing the self-energy. We thus call the method XAF-GW (X, eXpand-chi; A, Add-chi; F, Full wave functions). Compared to GW-embedding type approaches in the literature, the XAF-GW approach is not limited to specific screening environments or to nonhybridized interface systems. XAF-GW can also be applied to systems with different dimensionalities, as well as to Moire superlattices such as in twisted bilayers. We illustrate the generality and usefulness of our approach by applying it to self-assembled PTCDA monolayers on Au(111) and Ag(111) and PTCDA monolayers on graphite-supported monolayer WSe2. In all cases, the predicted HOMO and LUMO levels agree well with experimental measurements.
Source Title: JOURNAL OF CHEMICAL THEORY AND COMPUTATION
URI: https://scholarbank.nus.edu.sg/handle/10635/170971
ISSN: 15499618
15499626
DOI: 10.1021/acs.jctc.9b00229
Appears in Collections:Staff Publications
Elements

Show full item record
Files in This Item:
File Description SizeFormatAccess SettingsVersion 
1903.01847v1.pdf1.56 MBAdobe PDF

OPEN

Post-printView/Download

SCOPUSTM   
Citations

10
checked on Mar 3, 2021

Page view(s)

58
checked on Mar 5, 2021

Download(s)

2
checked on Mar 5, 2021

Google ScholarTM

Check

Altmetric


Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.