First-principles investigation of band offset and charge transfer characteristics at the PE/fluorinated layer interface

Chen, Xi; Guo, Guangzhi; Hao, Ying; Li, Jiaming; Li, Wendong; Deng, Junbo; Zhang, Guanjun; Zhai, Mingming

doi:10.1039/d0cp01992e

Cited by 4 publications

(7 citation statements)

References 51 publications

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“…The hopping time is calculated by eq . The hopping distance along the z axis and time of each step are recorded to calculate the charge mobility μ according to eq : P k = k k intra hop + + k intra hop − + k inter hop , where 0.25em k = k intra hop + , k intra hop − , or 0.25em k inter hop t k = 1 k intra hop + + k intra hop − + k inter hop μ = lim t → ∞ nobreak0em.25em⁡ μ ( t ) = lim t → ∞ nobreak0em.25em⁡ z ( t ) − z ( 0 ) t E …”

Section: Methodsmentioning

confidence: 99%

Origins of Charge Mobility Decreasing from Stretching–Releasing Cycles in Polymer Semiconductors

Chen,

Li,

Min

et al. 2023

Macromolecules

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Polymer semiconductors as a key component of electronic skin need to maintain the coexistence of stretchability and electrical functionalities. However, repeated stretching−compressing cycles inevitably lead to the charge mobilities decreasing and poor working performance of polymer semiconductors. Here, a method combining molecular dynamics (MD) simulations and charge transport theory was developed to obtain the morphology−mobility relationship of amorphous poly(3-hexylthiophene) (P3HT). The simulation results show that the hole mobility decreases by 6% along the strain direction after three stretching−compressing cycles with 80% strain. These results are due to the chain alignment change caused by the mechanical operations. The stretched P3HT material presents higher charge mobility due to its better chain alignment, while the compressed P3HT shows lower charge mobility because of the poor chain alignment. Repeated stretching−compressing cycles lead to the chain alignment parameters decreasing along the deformation direction with accumulation and saturation effects. The repeated cycles also result in the primitive path length decreasing, which indicates polymer chain spatial distribution is more localized after repeated deformations. Our findings provide microscale knowledge about the dependence of molecular morphology and charge mobility on stretching−compressing cycles, which can help to guide the design of polymer semiconductors with higher charge mobility under repeated stretching−compressing cycles.

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Section: Methodsmentioning

confidence: 99%

Origins of Charge Mobility Decreasing from Stretching–Releasing Cycles in Polymer Semiconductors

Chen,

Li,

Min

et al. 2023

Macromolecules

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“…Sato et al investigated the charge transport process for polyethylene (PE) with the aid of first-principles calculations within the framework of Marcus theory and a localized charge transport model. , They found that Marcus theory can reasonably predict the hole mobility, but it is not suitable for describing the electron transfer process in PE. Chen et al simulated the movement and accumulation of carriers in crystal poly(tetrafluoroethylene) (PTFE) based on classical Marcus theory . However, it is still uncertain as to whether the localized charge transport model can be applied to other polymeric dielectrics, especially to those with more complex structures.…”

Section: Introductionmentioning

confidence: 99%

“…Chen et al simulated the movement and accumulation of carriers in crystal poly(tetrafluoroethylene) (PTFE) based on classical Marcus theory. 22 However, it is still uncertain as to whether the localized charge transport model can be applied to other polymeric dielectrics, especially to those with more complex structures. Silicone rubber (SR) is a common insulation material used in high-voltage power cables and electrical insulators.…”

Section: Introductionmentioning

confidence: 99%

Multiscale Study of the Charge Transport Properties of Silicone Rubber Oligomers

et al. 2022

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Polymer dielectrics are widely used as insulation in electronic and electrical equipment. The charge transport process in polymer dielectrics under a high electric field, which is considered to result in electrical aging and even breakdown of equipment insulation, has attracted considerable attention. Based on a localized charge transfer model, the charge transport mechanism for typical silicone rubber (SR) insulating materials was studied by multiscale methods. A model of silicone rubber oligomers under standard conditions was generated by classical molecular dynamics. The frontier molecular orbitals and projected density of states for the SR oligomer were obtained via quantum chemistry methods. The electronic coupling, reorganization energy, and free energy difference for both electron and hole transfer processes between adjacent SR molecules in the molecular dynamics model were calculated. Both hole transfer and electron transfer in SR conform to an intermolecular hopping mechanism due to their high intramolecular reorganization energy and low intermolecular electronic coupling. The results of normal mode analysis for reorganization energy indicate that the high-temperature approximation holds for charge transport in SR around or above room temperature. The charge transfer trajectory and charge mobility in SR were simulated based on kinetic Monte Carlo simulations. The hole and electron mobilities at room temperature were calculated to be 7.24 × 10 −11 and 2.76 × 10 −9 cm 2 /Vs, respectively, which agrees with the experimental data. Both electron transport and hole transport in SR show thermal activation characteristics, with corresponding activation energies of 358 and 314 meV, respectively. This work suggests a physical model to describe the charge transport process in SR polymer dielectrics.

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“…The metallicity therefore is due to covalent bonding across the interface. To calculate the band alignment, the valence band offset (VBO) at the interface is determined as VBO = ( E perovskite + V perovskite ) – ( E MXene + V MXene ) + Δ V , where E perovskite and E MXene are the valence band maxima (VBMs) and V perovskite and V MXene are the macroscopic average electrostatic potentials of the component materials . Moreover, Δ V is the difference between the average electrostatic potentials on the two sides of the interface, as taken from Figure .…”

mentioning

confidence: 99%

“…To calculate the band alignment, the valence band offset (VBO) at the interface is determined as VBO = (E perovskite + V perovskite ) − (E MXene + V MXene ) + ΔV, where E perovskite and E MXene are the valence band maxima (VBMs) and V perovskite and V MXene are the macroscopic average electrostatic potentials of the component materials. 26 Moreover, ΔV is the difference between the average electrostatic potentials on the two sides of the interface, as taken from interface and thus aids the power conversion efficiency. 27 The type III band alignment leads to transfer of electrons from the valence band of Cs 2 NaBiI 6 to the conduction band of Sc 2 C(OH) 2 .…”

mentioning

confidence: 99%

Interfaces between Pb-Free Double Perovskite Cs₂NaBiI₆ and MXenes Sc₂CO₂ and Sc₂C(OH)₂

Albar

Schwingenschlögl

2022

J. Phys. Chem. Lett.

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First-principles calculations are used to explore the electronic properties of the interfaces between the Pb-free double perovskite Cs2NaBiI6 and the MXenes Sc2CO2 and Sc2C(OH)2. The effect of the termination group on the stability, ionization potential, electron affinity, and band alignment is investigated. We find a type II band alignment at the Cs2NaBiI6/Sc2CO2 interface, which permits charge transfer, and a type III band alignment at the Cs2NaBiI6/Sc2C(OH)2 interface, which results in electron–hole recombination. Sc2CO2 turns out to be highly promising for solar cell applications due to an almost ideal ionization potential difference to Cs2NaBiI6.

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First-principles investigation of band offset and charge transfer characteristics at the PE/fluorinated layer interface

Abstract: Polymers, especially polyethylene (PE) are widely employed as insulating material in electrical power transmission system. However, the insulation still faces the problem of space charge which will distort the electric...

Cited by 4 publications

References 51 publications

Origins of Charge Mobility Decreasing from Stretching–Releasing Cycles in Polymer Semiconductors

Origins of Charge Mobility Decreasing from Stretching–Releasing Cycles in Polymer Semiconductors

Multiscale Study of the Charge Transport Properties of Silicone Rubber Oligomers

Interfaces between Pb-Free Double Perovskite Cs₂NaBiI₆ and MXenes Sc₂CO₂ and Sc₂C(OH)₂

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First-principles investigation of band offset and charge transfer characteristics at the PE/fluorinated layer interface

Abstract: Polymers, especially polyethylene (PE) are widely employed as insulating material in electrical power transmission system. However, the insulation still faces the problem of space charge which will distort the electric...

Cited by 4 publications

References 51 publications

Origins of Charge Mobility Decreasing from Stretching–Releasing Cycles in Polymer Semiconductors

Origins of Charge Mobility Decreasing from Stretching–Releasing Cycles in Polymer Semiconductors

Multiscale Study of the Charge Transport Properties of Silicone Rubber Oligomers

Interfaces between Pb-Free Double Perovskite Cs2NaBiI6 and MXenes Sc2CO2 and Sc2C(OH)2

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Product

Resources

About

Interfaces between Pb-Free Double Perovskite Cs₂NaBiI₆ and MXenes Sc₂CO₂ and Sc₂C(OH)₂