Dependence of electron transfer dynamics on the number of graphene layers in π-stacked 2D materials: insights from <i>ab initio</i> nonadiabatic molecular dynamics

Mehdipour, Hamid; Smith, Brendan; Rezakhani, A. T.; Tafreshi, Saeedeh Sarabadani; Leeuw, Nora H. de; Prezhdo, Oleg V.; Moshfegh, A.Z.; Akimov, Alexey V.

doi:10.1039/c9cp04100a

Cited by 11 publications

(6 citation statements)

References 63 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The electrostatic doping or interfacial charge exchange between graphene and the underlying substrate most likely alters the affinity (i.e., strength of the interaction) between graphene and top adsorbates. This phenomenon has been reported by multiple molecular dynamics (MD) simulations studying other systems. − In the high ZnPc flux deposition regime, the preferential NW growth is observed either on graphene as-grown on Cu or on bare substrates which form quasi-vertical and nearly horizontal high-aspect-ratio crystallites, respectively. In the case of low ZnPc flux deposition regime, the ZnPc crystallites also prefer to adopt NW growth on graphene on Cu, while they prefer to form flat islands on other graphene-coated substrates as evidenced by the AFM images in Figure a–c.…”

Section: Resultsmentioning

confidence: 56%

Influence of the Underlying Substrate on the Physical Vapor Deposition of Zn-Phthalocyanine on Graphene

et al. 2021

View full text Add to dashboard Cite

Graphene shows great promise not only as a highly conductive flexible and transparent electrode for fabricating novel device architectures but also as an ideal synthesis platform for studying fundamental growth mechanisms of various materials. In particular, directly depositing metal phthalocyanines (MPc’s) on graphene is viewed as a compelling approach to improve the performance of organic photovoltaics and light-emitting diodes. In this work, we systematically investigate the ZnPc physical vapor deposition (PVD) on graphene either as-grown on Cu or as-transferred on various substrates including Si(100), C-plane sapphire, SiO2/Si, and h-BN. To better understand the effect of the substrate on the ZnPc structure and morphology, we also compare the ZnPc growth on highly crystalline single- and multilayer graphene. The experiments show that, for identical deposition conditions, ZnPc exhibits various morphologies such as high-aspect-ratio nanowires or a continuous film when changing the substrate supporting graphene. ZnPc morphology is also found to transition from a thin film to a nanowire structure when increasing the number of graphene layers. Our observations suggest that substrate-induced changes in graphene affect the adsorption, surface diffusion, and arrangement of ZnPc molecules. This study provides clear guidelines to control MPc crystallinity, morphology, and molecular orientations which drastically influence the (opto)electronic properties.

show abstract

Section: Resultsmentioning

confidence: 56%

Influence of the Underlying Substrate on the Physical Vapor Deposition of Zn-Phthalocyanine on Graphene

et al. 2021

View full text Add to dashboard Cite

show abstract

“…89 The ΔSCF method was also used to test the neglect of back-reaction (NBRA) approximation as applied to model the photoinduced interfacial charge transfer from zinc phthalocyanine to ultrathin graphene. 90 More applications of the ΔSCF approach for the NAMD of solid-state systems are expected with the development of software packages. [91][92][93] Despite the good performance of ΔSCF, there is no underlying theory to justify the method as used in applications.…”

Section: A the δScf Methodsmentioning

confidence: 99%

The ΔSCF method for non-adiabatic dynamics of systems in the liquid phase

Vandaele

Mališ

Luber

2022

The Journal of Chemical Physics

View full text Add to dashboard Cite

Computational studies of ultrafast photoinduced processes give valuable insights into the photochemical mechanisms of a broad range of compounds. In order to accurately reproduce, interpret, and predict experimental results, which are typically obtained in a condensed phase, it is indispensable to include the condensed phase environment in the computational model. However, most studies are still performed in vacuum due to the high computational cost of state-of-the-art non-adiabatic molecular dynamics (NAMD) simulations. The quantum mechanical/molecular mechanical (QM/MM) solvation method has been a popular model to perform photodynamics in the liquid phase. Nevertheless, the currently used QM/MM embedding techniques cannot sufficiently capture all solute–solvent interactions. In this Perspective, we will discuss the efficient ΔSCF electronic structure method and its applications with respect to the NAMD of solvated compounds, with a particular focus on explicit quantum mechanical solvation. As more research is required for this method to reach its full potential, some challenges and possible directions for future research are presented as well.

show abstract

“…This scheme has been widely used to explore the photoinduced carrier dynamics of periodic systems including carbon nanotubes and tetrapyrroles by our and other research groups. 23,[51][52][53][63][64][65][66][67][68][69][70][71] Other relevant theoretical backgrounds are put in the ESI. †…”

Section: Computational Detailsmentioning

confidence: 99%

Mechanistic insights into photoinduced energy and charge transfer dynamics between magnesium-centered tetrapyrroles and carbon nanotubes

Zhou,

Cheng,

Zhang

et al. 2023

Phys. Chem. Chem. Phys.

View full text Add to dashboard Cite

show abstract

Dependence of electron transfer dynamics on the number of graphene layers in π-stacked 2D materials: insights from ab initio nonadiabatic molecular dynamics

Abstract: Time-resolved simulation study has been carried out to explain anti-Fermi Golden rule order of charge transfer rates measured at the interfaces of Zn-phthalocyanine molecule with single-layer graphene and double-layer graphene.

Cited by 11 publications

References 63 publications

Influence of the Underlying Substrate on the Physical Vapor Deposition of Zn-Phthalocyanine on Graphene

Influence of the Underlying Substrate on the Physical Vapor Deposition of Zn-Phthalocyanine on Graphene

The ΔSCF method for non-adiabatic dynamics of systems in the liquid phase

Mechanistic insights into photoinduced energy and charge transfer dynamics between magnesium-centered tetrapyrroles and carbon nanotubes

Contact Info

Product

Resources

About