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

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

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

7 Scopus citations


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 molecules and two-dimensional materials, 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 account for the effects of the heterogeneous dielectric environment on the electronic structure of these mixed-dimensional heterojunctions.

Original languageEnglish (US)
Article number121112
JournalAPL Materials
Issue number12
StatePublished - Dec 1 2021

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)


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