Study of the cold charge transfer state separation at the TQ1/PC<sub>71</sub>BM interface

Volpi, Riccardo; Linares, Mathieu

doi:10.1002/jcc.24776

Cited by 3 publications

(2 citation statements)

References 62 publications

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“…The efficiency of separation and transference of the charge carriers are of critical importance to solar cell efficiency. 1 Today, it is still hard to achieve good efficiency when considering a single II-VI semiconductor, due to high recombination rates for the charge carriers and also because of photocorrosion. 2 Therefore, the combining of semiconductors receives a lot of attention due to the tunability of their electronic properties, leading to many relevant nanotechnology and optoelectronic applications.…”

Section: Introductionmentioning

confidence: 99%

Band alignment and charge transfer predictions of ZnO/ZnX (X = S, Se or Te) interfaces applied to solar cells: a PBE+Utheoretical study

Flores

Gouvêa

Piotrowski

et al. 2018

Phys. Chem. Chem. Phys.

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The engineering of semiconductor materials for the development of solar cells is of great importance today. Two topics are considered to be of critical importance for the efficiency of Grätzel-type solar cells, the efficiency of charge separation and the efficiency of charge carrier transfer. Thus, one research focus is the combination of semiconductor materials with the aim of reducing charge recombination, which occurs by spatial charge separation. From an experimental point of view, the combining of materials can be achieved by decorating a core with a shell of another material resulting in a core-shell system, which allows control of the desired photoelectronic properties. In this context, a computational simulation is mandatory for the atomistic understanding of possible semiconductor combinations and for the prediction of their properties. Considering the construction of ZnO/ZnX (X = S, Se or Te) interfaces, we seek to investigate the electronic influence of the shell (ZnX) on the core (ZnO) and, consequently, find out which of the interfaces would present the appropriate properties for (Grätzel-type) solar cell applications. To perform this study, we have employed density functional theory (DFT) calculations, considering the Perdew-Burke-Ernzerhof (PBE) functional. However, it is well-known that plain DFT fails to describe strong electronic correlated materials where, in general, an underestimation of the band gap is obtained. Thus, to obtain the correct description of the electronic properties, a Hubbard correction was employed, i.e. PBE+U calculations. The PBE+U methodology provided the correct electronic structure properties for bulk ZnO in good agreement with experimental values (99.4%). The ZnO/ZnX interfaces were built and were composed of six ZnO layers and two ZnX layers, which represents the decoration process. The core-shell band gap was 2.2 eV for ZnO/ZnS, ∼1.71 eV for ZnO/ZnSe and ∼0.95 eV for ZnO/ZnTe, which also exhibited a type-II band alignment. Bader charge analysis showed an accumulation of charges in the 6th layer of ZnO for the three ZnO/ZnX interfaces. On the basis of these results, we have proposed that ZnO/ZnS and ZnO/ZnSe core-shell structures can be applied as good candidates (with better efficiency) for photovoltaic devices.

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Section: Introductionmentioning

confidence: 99%

Band alignment and charge transfer predictions of ZnO/ZnX (X = S, Se or Te) interfaces applied to solar cells: a PBE+Utheoretical study

Flores

Gouvêa

Piotrowski

et al. 2018

Phys. Chem. Chem. Phys.

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“…Although the energetic disorder introduced by intermolecular electrostatic interactions, due to permanent and induced dipoles, can play a key role in improving charge separation at heterojunctions, [43][44][45] and charge-carrier localization [46], it was not included in this work because of the nonpolar nature of TFB, which implies low energetic disorder as confirmed by Malliaras et al [18].…”

Section: Charge Transport Modelmentioning

confidence: 99%

Energetic fluctuations in amorphous semiconducting polymers: Impact on charge-carrier mobility

Gali

D’Avino

Aurel

et al. 2017

The Journal of Chemical Physics

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We present a computational approach to model hole transport in an amorphous semiconducting fluorene-triphenylamine copolymer (TFB), which is based on the combination of molecular dynamics to predict the morphology of the oligomeric system and Kinetic Monte Carlo (KMC), parameterized with quantum chemistry calculations, to simulate hole transport. Carrying out a systematic comparison with available experimental results, we discuss the role that different transport parameters play in the KMC simulation and in particular the dynamic nature of positional and energetic disorder on the temperature and electric field dependence of charge mobility. It emerges that a semi-quantitative agreement with experiments is found only when the dynamic nature of the disorder is taken into account. This study establishes a clear link between microscopic quantities and macroscopic hole mobility for TFB and provides substantial evidence of the importance of incorporating fluctuations, at the molecular level, to obtain results that are in good agreement with temperature and electric field-dependent experimental mobilities. Our work makes a step forward towards the application of nanoscale theoretical schemes as a tool for predictive material screening.

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Theoretical description of photoinduced electron transfer in donor–acceptor supramolecular complexes based on carbon buckybowls

Rubert-Albiol,

Cerdá,

Calbo

et al. 2024

The Journal of Chemical Physics

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Herein, we explore, from a theoretical perspective, the nonradiative photoinduced processes (charge separation and energy transfer) within a family of donor–acceptor supramolecular complexes based on the electron-donor truxene-tetrathiafulvalene (truxTTF) derivative and a series of curved fullerene fragments (buckybowls) of different shapes and sizes (C30H12, C32H12, and C38H14) as electron acceptors that successfully combine with truxTTF via non-covalent interactions. The resulting supramolecular complexes (truxTTF·C30H12, truxTTF·C32H12, and truxTTF·C38H14) undergo charge-separation processes upon photoexcitation through charge-transfer states involving the donor and acceptor units. Despite the not so different size of the buckybowls, they present noticeable differences in the charge-separation efficiency owing to a complex decay post-photoexcitation mechanism involving several low-lying excited states of different natures (local and charge-transfer excitations), all closely spaced in energy. In this intricate scenario, we have adopted a theoretical approach combining electronic structure calculations at (time-dependent) density functional theory, a multistate multifragment diabatization method, the Marcus–Levitch–Jortner semiclassical rate expression, and a kinetic model to estimate the charge separation rate constants of the supramolecular heterodimers. Our outcomes highlight that the efficiency of the photoinduced charge-separation process increases with the extension of the buckybowl backbone. The supramolecular heterodimer with the largest buckybowl (truxTTF·C38H14) displays multiple and efficient electron-transfer pathways, providing a global photoinduced charge separation in the ultrafast time scale in line with the experimental findings. The study reported indicates that modifications in the shape and size of buckybowl systems can give rise to attractive novel acceptors for potential photovoltaic applications.

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Study of the cold charge transfer state separation at the TQ1/PC₇₁BM interface

Cited by 3 publications

References 62 publications

Band alignment and charge transfer predictions of ZnO/ZnX (X = S, Se or Te) interfaces applied to solar cells: a PBE+Utheoretical study

Band alignment and charge transfer predictions of ZnO/ZnX (X = S, Se or Te) interfaces applied to solar cells: a PBE+Utheoretical study

Energetic fluctuations in amorphous semiconducting polymers: Impact on charge-carrier mobility

Theoretical description of photoinduced electron transfer in donor–acceptor supramolecular complexes based on carbon buckybowls

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Study of the cold charge transfer state separation at the TQ1/PC71BM interface

Cited by 3 publications

References 62 publications

Band alignment and charge transfer predictions of ZnO/ZnX (X = S, Se or Te) interfaces applied to solar cells: a PBE+Utheoretical study

Band alignment and charge transfer predictions of ZnO/ZnX (X = S, Se or Te) interfaces applied to solar cells: a PBE+Utheoretical study

Energetic fluctuations in amorphous semiconducting polymers: Impact on charge-carrier mobility

Theoretical description of photoinduced electron transfer in donor–acceptor supramolecular complexes based on carbon buckybowls

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Study of the cold charge transfer state separation at the TQ1/PC₇₁BM interface