Article
Chemistry, Multidisciplinary
Narayanaswamy Kamatham, Olzhas A. Ibraikulov, Pablo Durand, Jing Wang, Olivier Boyron, Benoit Heinrich, Thomas Heiser, Patrick Leveque, Nicolas Leclerc, Stephane Mery
Summary: This study reports the impact of functionalizing four different semiconducting polymer structures with linear siloxane-terminated side-chains, showing that the substitution of alkyl chains with siloxane chains significantly influences the properties of the polymers. The increase in pi-stacking overlap of the polymer backbones leads to enhanced charge mobility values. Additionally, different siloxane chains have distinct effects on the polymer structure.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Polymer Science
Alexey N. Lachinov, Danfis D. Karamov, Azat F. Galiev, Sergey N. Salazkin, Vera V. Shaposhnikova, Tatiana N. Kost, Alla B. Chebotareva
Summary: The mechanism of charge carrier transport in the ITO/polymer/Cu structure using copoly(arylene ether ketone) films is studied. The effects of polymer film thickness on the potential barrier, charge carrier concentration, and mobility are investigated. The study of this system is important due to its potential application in solar cells. Various characterizations and models are used to evaluate the parameters of the charge carriers and barrier height. The supramolecular structure and surface charge field of the polymer films are also discussed.
Article
Chemistry, Multidisciplinary
Yifei Jiang, Haobin Chen, Xiaoju Men, Zezhou Sun, Zhen Yuan, Xuanjun Zhang, Daniel T. Chiu, Changfeng Wu, Jason McNeill
Summary: A novel multimode superresolution method was developed to map the structure and measure the energy landscape of single carrier transport along conjugated polymer nanowires. By quenching of local emission and tracking the motion of a single photogenerated hole using blinking-assisted localization microscopy, the method successfully correlated structures with charge transport properties. The efficiency of inter- and intrachain hole transport inside the nanowires was compared, and the depth of carrier traps from torsional disorder and chemical defects was directly measured for the first time.
Article
Polymer Science
Gui-Sheng Jiao, Yuanshuo Zhang, He Cheng, Tongfei Shi, Zhi-Chao Yan
Summary: Charge transport in conjugated polymers is influenced by both static structure and dynamics of backbone segments. Molecular dynamics simulations are used to study regiorandom poly(3-alkylthiophenes) (P3ATs) with 6-12 alkyl carbons per side chain. The effect of temperature and side chain length on the static structure is investigated, revealing that the peak at q & SIM; 0.42 & ANGS;(-1) is due to edge-to-edge packing along the side-chain direction and shifts to lower q with longer side chains. The peak at q & SIM; 1.35 & ANGS;(-1) is contributed by intrachain side chain-side chain correlation and interchain correlation on the face-to-face stacking direction. Moreover, longer side chains result in faster backbone dynamics, with the carbon atoms farther from the backbone exhibiting faster motion. The last three atoms near the end of the alkyl side chain play a significant role in the faster motion of the backbone.
Review
Chemistry, Physical
Yang Zhou, Keke Zhang, Zhaoyang Chen, Haichang Zhang
Summary: Organic field-effect transistors (OFETs) have gained attention due to their performance in charge transport. Optimizing charge transport within the semiconductor layer and charge injection is crucial for improving OFETs' performance. Currently, the majority of conjugated materials belong to the p-type semiconductor category, lagging behind in research on n-type or ambipolar conjugated materials.
Article
Polymer Science
Yuchai Pan, Jianyao Huang, Dong Gao, Zhihui Chen, Weifeng Zhang, Gui Yu
Summary: Semiconducting polymers play a crucial role in both industrial and academic purposes, with ongoing research focusing on the structure-performance relationship. By improving structural engineering, new semiconducting polymers with enhanced properties can be developed. Through studying a series of diketopyrrolopyrrole-based polymers with different alkyl chain lengths, a strong correlation between electrical performance and alkyl side chain was observed, leading to a comprehensive understanding of design rules for high-performance semiconductor materials.
Article
Energy & Fuels
Armin Richter, Ralph Muller, Jan Benick, Frank Feldmann, Bernd Steinhauser, Christian Reichel, Andreas Fell, Martin Bivour, Martin Hermle, Stefan W. Glunz
Summary: Front- and back-junction silicon photovoltaics dominate the market due to lower manufacturing complexity, but achieving efficiency improvements remains challenging. An optimized design by Richter et al. has led to a 26.0%-efficient cell. While interdigitated back-contact cells offer the highest efficiency, both-sides-contacted cells are preferred in industrial production for their simplicity.
Article
Biochemistry & Molecular Biology
Gabriela Grzes, Karol Wolski, Tomasz Uchacz, Justyna Bala, Boris Louis, Ivan G. Scheblykin, Szczepan Zapotoczny
Summary: This report presents a synthetic route to prepare ladder-like polymer brushes with PProDOT-conjugated chains using a novel surface-initiated technique. Characterization and stability tests of these brushes demonstrate the remarkable stability of the obtained materials.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Physical
Tingxia Zhou, Xiaomei Wu, Tianqi Deng, Haoyuan Li, Zhibin Gao, Wen Shi
Summary: Recently, two-dimensional covalent organic framework-based materials have shown promising performance for potential thermoelectric applications. However, the systematic atomistic design strategies for enhancing the thermoelectric properties of these materials remain a challenging task. In this study, using ab initio computations on 17 representative two-dimensional covalent organic frameworks, an atomistic understanding is established to uncover the complex correlation between macroscopic thermoelectric properties, nontrivial transport processes, and basic chemical structures, and general materials design guidelines are presented. The study reveals that the ratio of contributions from linker and knot parts to the valence bands can serve as a strong predictor of the thermoelectric performance of covalent organic frameworks.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Materials Science, Multidisciplinary
Vivian Nketia-Yawson, Benjamin Nketia-Yawson, Jea Woong Jo
Summary: Using conjugated polyelectrolytes (CPEs) as interfacial work function modifiers significantly improves the hole carrier mobility in hybrid methylammonium lead iodide perovskite-conjugated polymer field-effect transistors (FETs).
ORGANIC ELECTRONICS
(2023)
Article
Chemistry, Multidisciplinary
Masahiro Funahashi
Summary: The study shows that a bulk photovoltaic effect can be achieved in a chiral smectic crystal phase doped with specific additives. The polarity of the photovoltaic effect can be adjusted by changing the polarization bias. Aggregation of fullerene derivatives into microcrystals promotes hole-electron dissociation, leading to high efficiency of photocurrent generation.
MATERIALS CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
Alexey N. N. Lachinov, Danfis D. Karamov, Azat F. Galiev, Alexey A. A. Lachinov, Azat R. Yusupov, Vera V. Shaposhnikova, Sergey N. Salazkin, Alla B. Chebotareva
Summary: This study investigates the current flow path in a multilayer sample by marking the polymer-polymer interface with a doping nanolayer of a Cu2O island film. The results show that doping the polymer-polymer interface with Cu2O particles strongly affects the transport of charge carriers, resulting in an increase in conductivity. It is concluded that the transport of charge carriers occurs along the polymer-polymer interface at the specified structure parameters in this study.
APPLIED SCIENCES-BASEL
(2023)
Article
Physics, Applied
Jiu-Xun Sun, Hong-Chun Yang, Yang Li, Hai-Juan Cui
Summary: Although the accurate solution of the drift-diffusion model has been a challenge in semiconductor physics, this study presents a new approach based on Fermi-Dirac statistics and a general mobility model. The results demonstrate noticeable differences between the accurate solution and other existing solutions, such as the Scharfetter-Gummel scheme and the Mott-Gurney equation.
PHYSICAL REVIEW APPLIED
(2023)
Article
Polymer Science
Xuran Wang, Shengzhen Liu, Chunxing Ren, Long Cao, Weimin Zhang, Ti Wu
Summary: In this study, a series of conjugated polymers with novel fluorine-containing branched side chains were synthesized and characterized for their performance in solution-processed organic field-effect transistors (OFETs). The results showed that these polymers exhibited high electron mobility, as well as good thermal and environmental stability in OFET devices.
Article
Polymer Science
Qianglong Lv, Cunbin An, Tao Zhang, Pengxin Zhou, Jianhui Hou
Summary: Optimizing side chains can maximize the photovoltaic performance of conjugated polymers, influencing aggregation behavior and phase separation, leading to improved power conversion efficiency in polymer solar cells.
Article
Multidisciplinary Sciences
Jiongzhao Li, Weicheng Cao, Yufei Shu, Haibing Zhang, Xudong Qian, Xueqian Kong, Linjun Wang, Xiaogang Peng
Summary: High-quality colloidal nanocrystals can be synthesized in hydrocarbon solvents with alkanoates as the common organic ligand. Water molecules with a similar number of surface alkanoate ligands are found at the inorganic-organic interface for all types of colloidal nanocrystals studied. Carboxylate ligands are coordinated to the surface metal ions, and the first monolayer of water molecules bonds to the carboxylate groups of alkanoate ligands through hydrogen bonds. Additional monolayer(s) of water molecules can be adsorbed through hydrogen bonds to the first monolayer of water molecules. The water-enriched structure of the inorganic-organic interface of high-quality colloidal nanocrystals plays a crucial role in their synthesis, processing, and properties.
NATIONAL SCIENCE REVIEW
(2022)
Article
Nanoscience & Nanotechnology
Zedong Wang, Jiawei Dong, Jing Qiu, Linjun Wang
Summary: The article introduces an efficient divide-and-conquer approach based on Wannier analysis and machine learning for nonadiabatic dynamics simulations of large systems. The method decomposes the system into small building blocks and constructs the system Hamiltonian using artificial neural networks. It successfully studies graphene nanoribbons with >10,000 atoms.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Liping Chen, Tao Liang, Linjun Wang
Summary: In this study, Morse clusters with up to 700 atoms were systematically studied using the unbiased fuzzy global optimization (FGO) method, resulting in the identification of new global minima with lower energies, as well as detailed growth patterns and magic clusters. Additionally, the presence of a central vacancy in Morse clusters with p=6 was discovered for the first time.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Materials Science, Multidisciplinary
Francesco Maria Bellussi, Otello Maria Roscioni, Edoardo Rossi, Annalisa Cardellini, Marina Provenzano, Luca Persichetti, Valeriya Kudryavtseva, Gleb Sukhorukov, Pietro Asinari, Marco Sebastiani, Matteo Fasano
Summary: The wetting properties of soft interfaces with different liquids are challenging to predict in surface engineering. In this article, a molecular dynamics simulations-based workflow is proposed to predict the wettability of polymer surfaces and tested against experimental contact angles of several liquids. The results show a discrepancy of less than 3% for water. This work represents the initial step towards predicting the wettability of more complex soft interfaces using an integrated multiscale framework.
Article
Chemistry, Physical
Guijie Li, Cancan Shao, Jiabo Xu, Linjun Wang
Summary: The paper introduces a unified framework of mixed quantum-classical dynamics called Branching-Corrected Surface Hopping and Mean Field (BCSHMF) method. Through benchmark testing on diverse scattering models, BCSHMF achieves high reliability and flexibility, indicating the compatibility between surface hopping and mean field, and the importance of trajectory branching in describing nonadiabatic dynamics.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Suryoday Prodhan, Rex Manurung, Alessandro Troisi
Summary: A model reduction scheme is proposed to compute intra-chain charge-carrier mobility from the monomer sequence in polymer semiconductors. The scheme can be combined with any quantum dynamics approach and assumes transport through incoherent hopping events between states of different degrees of delocalization. The correlation between charge localization characteristics and charge mobility is quantitatively established using 28 realistic polymers, providing insights into the relationship between inter-monomer coupling and mobility.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Otello Maria Roscioni, Matteo Ricci, Claudio Zannoni, Gabriele D'Avino
Summary: The quality of amorphous molecular morphologies obtained with a new coarse-grained model is compared with reference atomistic data. The study focuses on small-molecule organic semiconductors in their pristine and doped forms, analyzing their structural features and electronic properties. The results demonstrate that the accurate coarse-grained model produces molecular glasses that are highly similar to atomistic samples, with even better agreement after back-mapping. The electronic properties of the back-mapped morphologies are almost indistinguishable from the atomistic reference, supporting the feasibility of large-scale simulations of complex molecular systems at a reduced computational cost.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Yao Lu, Jiawei Dong, Linjun Wang
Summary: In this study, an importance sampling approach is proposed to calculate the electron distribution at general interfaces. The method is verified to be highly accurate, precise, and efficient through comparisons with other sampling approaches and non-adiabatic dynamics simulations. Factors such as the number of states, electronic couplings, reorganization energies, and energetic disorders are found to have significant impacts on the anomalous interfacial charge transfer across a high energy barrier. Additionally, a machine learning approach is proposed to predict interfacial charge transfer in extremely large systems based on data computed by importance sampling in relatively small but diverse systems.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Haiwei Lei, Liping Chen, Linjun Wang
Summary: This study presents a new global optimization method to obtain the lowest-energy structures of cadmium selenide clusters. The method combines atom-pair hopping, ultrafast shape recognition, and adaptive temperature techniques to enhance search efficiency. The results reveal the systematic structural evolution of cadmium selenide clusters from rings to stacked rings, cages, nanotubes, cage-wurtzite, cage-core, and finally wurtzite structures.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Physics, Condensed Matter
Zirui Wang, Jiawei Dong, Linjun Wang
Summary: In this study, a parameter-free full crossing corrected global flux surface hopping method was used to investigate charge transport in two-dimensional hexagonal molecular crystals. The results show that the signs of electronic couplings have a strong impact on charge mobility and delocalization strength, and can even lead to a transition from hopping to band-like transport. In contrast, such phenomena cannot be observed in extensively studied two-dimensional square systems.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2023)
Article
Chemistry, Multidisciplinary
Hairui Lei, Tenghui Li, Jiongzhao Li, Jie Zhu, Haibing Zhang, Haiyan Qin, Xueqian Kong, Linjun Wang, Xiaogang Peng
Summary: This study investigates facet reconstruction of colloidal wurtzite CdSe/CdS core/shell nanocrystals under typical synthetic conditions and reveals that two sets of facets with specific low-index facets can be reversibly reconstructed by switching the ligand system, indicating their thermodynamic stability. The atomic structures of the low-index facets of wurtzite nanocrystals are diverse, and each facet is paired with a common ligand in the solution. The results suggest that facet-controlled nanocrystals can be synthesized by optimal facet-ligand pairing, enabling the formation of semiconductor nanocrystals with size-dependent properties at an atomic level.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Multidisciplinary
Hairui Lei, Jiongzhao Li, Xueqian Kong, Linjun Wang, Xiaogang Peng
Summary: This article summarizes the properties of colloidal semiconducting nanocrystals with a single-crystalline structure, which are largely influenced by their surface structure at the atomic-molecular level. Although there is a lack of understanding and control over the surface structure, the three spatial zones of the nanocrystal surface (crystal facets, inorganic-ligands interface, and ligands monolayer) can be studied using advanced experimental techniques and theoretical calculations. The surface ligands and their bonding modes are facet-specific, and the solubility of nanocrystal-ligands complexes is determined by the ligands monolayer. The molecular environment surrounding each nanocrystal plays a critical role in their properties.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Physical
Cancan Shao, Zhecun Shi, Jiabo Xu, Linjun Wang
Summary: Surface hopping simulations have been improved by utilizing a machine learning assisted approach to optimize the decoherence time formulas. By using exact quantum dynamics as references and generating descriptor spaces through nuclear kinetic energy and adiabatic energy difference, we obtained new energy-based formulas. These formulas were benchmarked in various systems and models, showing high accuracy and efficiency in reproducing the exact quantum dynamics. This approach offers a promising avenue to enhance the accuracy of surface hopping simulations in complex systems based on quantum dynamics data.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Guijie Li, Zhecun Shi, Xin Guo, Linjun Wang
Summary: In the traditional Ehrenfest mean field approach, an effective wave packet is used to describe the nuclear motion in nonadiabatic dynamics. However, in the quantum picture, the wave packet components on different adiabatic potential energy surfaces separate in space due to different velocities and forces. In this study, we propose an auxiliary branching corrected mean field method that introduces trajectories of auxiliary wave packets on adiabatic surfaces. The method accurately captures the channel populations and time-dependent spatial distribution of population, revealing the important role of auxiliary wave packets in solving intrinsic problems of mean field description in nonadiabatic dynamics.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Qiong Chen, Zhaoyong Li, Ye Lei, Yixin Chen, Hua Tang, Guangcheng Wu, Bin Sun, Yuxi Wei, Tianyu Jiao, Songna Zhang, Feihe Huang, Linjun Wang, Hao Li
Summary: Controlling the self-assembly on noncovalent components is possible by suppressing entropy loss with templates but this is challenging for covalent components. Here the authors employed directing groups to endow purely covalent molecular building blocks with different conformations which favor the formation of specific self-assembled products.
NATURE COMMUNICATIONS
(2023)