Please use this identifier to cite or link to this item: https://doi.org/10.1021/acs.jpcc.7b00715
Title: Energy Level Alignment at Hybridized Organic-Metal Interfaces: The Role of Many-Electron Effects
Authors: Chen, Yifeng 
Tamblyn, Isaac
Quek, Su Ying 
Keywords: Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
SELF-ASSEMBLED MONOLAYERS
SINGLE-MOLECULE CIRCUITS
QUASI-PARTICLE
CHARGE-TRANSPORT
CONDUCTANCE
1ST-PRINCIPLES
JUNCTIONS
Issue Date: 22-Jun-2017
Publisher: AMERICAN CHEMICAL SOCIETY
Citation: Chen, Yifeng, Tamblyn, Isaac, Quek, Su Ying (2017-06-22). Energy Level Alignment at Hybridized Organic-Metal Interfaces: The Role of Many-Electron Effects. JOURNAL OF PHYSICAL CHEMISTRY C 121 (24) : 13125-13134. ScholarBank@NUS Repository. https://doi.org/10.1021/acs.jpcc.7b00715
Abstract: © 2017 American Chemical Society. Hybridized molecule/metal interfaces are ubiquitous in molecular and organic devices. The energy level alignment (ELA) of frontier molecular levels relative to the metal Fermi level (EF) is critical to the conductance and functionality of these devices. However, a clear understanding of the ELA that includes many-electron self-energy effects is lacking. Here, we investigate the many-electron effects on the ELA using state-of-the-art, benchmark GW calculations on prototypical chemisorbed molecules on Au(111), in eleven different geometries. The GW ELA is in good agreement with photoemission for monolayers of benzene diamine on Au(111). We find that in addition to static image charge screening, the frontier levels in most of these geometries are renormalized by additional screening from substrate-mediated intermolecular Coulomb interactions. For weakly chemisorbed systems, such as amines and pyridines on Au, this additional level renormalization (∼1.5 eV) comes solely from static screened exchange energy, allowing us to suggest computationally more tractable schemes to predict the ELA at such interfaces. However, for more strongly chemisorbed thiolate layers, dynamical effects are present. Our ab initio results constitute an important step toward the understanding and manipulation of functional molecular/organic systems for both fundamental studies and applications.
Source Title: JOURNAL OF PHYSICAL CHEMISTRY C
URI: https://scholarbank.nus.edu.sg/handle/10635/170973
ISSN: 19327447
19327455
DOI: 10.1021/acs.jpcc.7b00715
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