Electronic and Optical Excitations at the Pyridine/ZnO(101¯0) Hybrid Interface

Turkina, Olga; Nabok, Dmitrii; Guļāns, Andris; Cocchi, Caterina; Draxl, Claudia

doi:10.1002/adts.201800108

Cited by 16 publications

(21 citation statements)

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“…The renormalization of the ZnO band gap is only 0.03 eV in DFT but anyway 0.45 eV in G 0 W 0 . A qualitatively similar behavior has been recently observed in another hybrid system, consisting of pyridine molecules chemisorbed on the wurtzite ZnO(101̅0) surface …”

Section: Resultssupporting

confidence: 84%

Energy-Level Alignment at Organic/Inorganic Interfaces from First Principles: Example of Poly(para-phenylene)/Rock-Salt ZnO(100)

2019

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By means of full-potential all-electron density-functional theory and many-body perturbation theory, we compute the band alignment at a prototypical hybrid inorganic/organic interface. The electronic properties of a model system built of poly(para-phenylene) and rs-ZnO are studied in two different geometries, employing several approaches of increasing sophistication. To this extent, we explore models for predicting the level alignment, which are based on the knowledge of the electronic structure of the individual constituents and are commonly used for semiconductor interfaces. For their evaluation in the context of hybrid materials, we perform an ab-initio study of the entire system, including a quasiparticle description of the electronic stucture within the G0W0 approximation. Based on this, we quantify the impact of structure, charge redistribution, orbital hybridization, and molecular polarization on the band offsets and the alignment type. We highlight not only known limitations of predicting the level alignment at a hybrid inorganic/organic interface by simple models, but also demonstrate how structural details of the interface components impact the results. arXiv:1908.07293v1 [cond-mat.mtrl-sci]

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Section: Resultssupporting

confidence: 84%

Energy-Level Alignment at Organic/Inorganic Interfaces from First Principles: Example of Poly(para-phenylene)/Rock-Salt ZnO(100)

2019

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“…Also excitons localized solely on either component appear in the absorption spectrum of the pyridine-ZnO interface investigated in Ref. [63]. On account of the relative energy gaps of the inorganic and organic constituents, excitons confined on the ZnO layer appear in the low-energy region, while those localized only on the molecular monolayer are found at higher energies, in the ultraviolet band.…”

Section: Introductionmentioning

confidence: 93%

“…Upon photo-excitation, the charge transfer and the faceted electronic structure of hybrid systems give rise to new types of excitons, characterized by a specific amount of (de)localization on the individual components and/or across the interface [50,[56][57][58][59][60][61][62]. A meaningful example is given by a recent first-principles study on a hybrid inorganic/organic interface formed by a monolayer of pyridine molecules chemisorbed on a ZnO surface [63]. In such a system, where the hybridization between the electronic states of the organic and the inorganic sides is enhanced by the covalent bond, hybrid excitons coexist with charge-transfer ones.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast charge transfer and vibronic coupling in a laser-excited hybrid inorganic/organic interface

Jacobs

Krumland

Valencia

et al. 2020

Advances in Physics: X

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Hybrid interfaces formed by inorganic semiconductors and organic molecules are intriguing materials for opto-electronics. Interfacial charge transfer is primarily responsible for their peculiar electronic structure and optical response. Hence, it is essential to gain insight into this fundamental process also beyond the static picture. Ab initio methods based on real-time time-dependent density-functional theory coupled to the Ehrenfest molecular dynamics scheme are ideally suited for this problem. We investigate a laser-excited hybrid inorganic/organic interface formed by the electron acceptor molecule 2,3,5,6-tetrafluoro-7,7,8,8-tetracyano-quinodimethane (F4TCNQ) physisorbed on a hydrogenated silicon cluster, and we discuss the fundamental mechanisms of charge transfer in the ultrashort time window following the impulsive excitation. The considered interface is p-doped and exhibits charge transfer in the ground state. When it is excited by a resonant laser pulse, the charge transfer across the interface is additionally increased, but contrary to previous observations in allorganic donor/acceptor complexes, it is not further promoted by vibronic coupling. In the considered time window of 100 fs, the molecular vibrations are coupled to the electron dynamics and enhance intramolecular charge transfer. Our results highlight the complexity of the physics involved and demonstrate the ability of the adopted formalism to achieve a comprehensive understanding of ultrafast charge transfer in hybrid materials.

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“…2) and represent the contributions to a given electronic transition to the λ th solution of the BSE (see, for example, Refs. [54][55][56]). Both eigenenergies and eigenvectors of Eq.…”

Section: Theoretical Background and Computational Detailsmentioning

confidence: 99%

Electronic and optical excitations of two-dimensional ZrS2 and HfS2 and their heterostructure

Lau

Cocchi

Draxl

2019

Phys. Rev. Materials

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In a first-principles study based on density-functional theory and many-body perturbation theory, we investigate the electronic properties and the optical excitations of ZrS2 and HfS2 monolayers and their van der Waals heterostructure. Both materials have an indirect quasi-particle band gap, which amounts to about 2.8 eV in ZrS2 and to 2.6 eV in HfS2. In both systems the valence-band maximum is at Γ and the conduction-band minimum at M. Spin-orbit coupling induces a splitting of about 100 meV at the Γ point in the valence band, while it does not affect the conduction band. The optical absorption spectra are dominated by excitonic peaks, with binding energies between 0.6 eV and 0.8 eV. The ZrS2/HfS2 heterobilayer exhibits a peculiar type-I level alignment with a large degree of hybridization between the two monolayers in the valence band, while the conduction bands retain either ZrS2 or HfS2 character, respectively. As a consequence, both the electron and the hole components of the first exciton are localized in the ZrS2 monolayer with non-vanishing probability of finding the hole also in the HfS2 sheet.

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Electronic and Optical Excitations at the Pyridine/ZnO(101¯0) Hybrid Interface

Cited by 16 publications

References 50 publications

Energy-Level Alignment at Organic/Inorganic Interfaces from First Principles: Example of Poly(para-phenylene)/Rock-Salt ZnO(100)

Energy-Level Alignment at Organic/Inorganic Interfaces from First Principles: Example of Poly(para-phenylene)/Rock-Salt ZnO(100)

Ultrafast charge transfer and vibronic coupling in a laser-excited hybrid inorganic/organic interface

Electronic and optical excitations of two-dimensional ZrS2 and HfS2 and their heterostructure

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