Range-separated hybrid functionals for mixed dimensional heterojunctions: Application to phthalocyanines/MoS2

Zhou, Qunfei; Liu, Zhen-Fei; Marks, Tobin J.; Darancet, Pierre

doi:10.1063/5.0052619

Title: Range-separated hybrid functionals for mixed dimensional heterojunctions: Application to phthalocyanines/MoS₂

Journal Article · Mon Dec 20 00:00:00 EST 2021 · APL Materials

DOI:https://doi.org/10.1063/5.0052619· OSTI ID:1886391

^[1];

^[2]; Marks, Tobin J. ^[3];

^[4]

Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Wayne State Univ., Detroit, MI (United States)
Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

We analyze the electronic structure and level alignment of transition-metal phthalocyanine (MPc) molecules adsorbed on two-dimensional MoS₂ employing density functional theory (DFT) calculations. We develop a procedure for multi-objective optimal tuning of parameters of range-separated hybrid functionals in these mixed-dimensional systems. Using this procedure, which leads to the asymptotically-correct exchange-correlation potential between molecule and two-dimensional material, we obtain electronic structures consistent with experimental photoemission results for both energy level alignment and electronic bandgaps, representing a significant advance compared to standard DFT methods. We elucidate the MoS₂ valence resonance with the transition-metal phthalocyanine non-frontier 3d orbitals and its dependence on the transition metal atomic number. Based on our calculations, we derive parameter-free, model self-energy corrections that quantitatively accounts for the effects of the heterogeneous dielectric environment on the electronic structure of these mixed-dimensional heterojunctions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357; DMR-1720139

OSTI ID:: 1886391

Alternate ID(s):: OSTI ID: 1836599

Journal Information:: APL Materials, Vol. 9, Issue 12; ISSN 2166-532X

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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