Article
Materials Science, Multidisciplinary
Yizhong Guo, Jiao Teng, Guo Yang, Ang Li, Yao Deng, Chengpeng Yang, Lihua Wang, Xin Yan, Ze Zhang, Xiaoyan Li, En Ma, Xiaodong Han
Summary: Detailed monitoring of atomic-scale processes is crucial for understanding grain rotation in nanocrystalline metals. In this study, in situ atomic-resolution evidence reveals that the type of grain boundary plays a role in the atomic processes involved in grain rotation in nanocrystalline Pt. General GBs exhibit a combination of dislocation activities and atomic rearrangements, while tilt GBs mostly rely on dislocation activities. GB dislocation climb, glide, and reaction are often associated with Lomer-like dislocation formation and destruction.
Article
Multidisciplinary Sciences
Zheyi Lu, Yang Chen, Weiqi Dang, Lingan Kong, Quanyang Tao, Likuan Ma, Donglin Lu, Liting Liu, Wanying Li, Zhiwei Li, Xiao Liu, Yiliu Wang, Xidong Duan, Lei Liao, Yuan Liu
Summary: A dry dielectric integration strategy enables the transfer of wafer-scale and high-kappa dielectrics on top of 2D semiconductors. An ultra-thin buffer layer is used to pre-deposit sub-3 nm thin Al2O3 or HfO2 dielectrics, which are then mechanically dry-transferred on top of MoS2 monolayers. The transferred ultra-thin dielectric film exhibits wafer-scale flatness and uniformity without any cracks, showing high capacitance, low leakage currents, and excellent transistor properties.
NATURE COMMUNICATIONS
(2023)
Article
Engineering, Electrical & Electronic
Chieh Lo, Shu-Chieh Chang, Kun-Tao Lin, Chung-Kuang Chen, Chen-Feng Chang, Feng-Shuo Zhang, Zong-Han Lu, Tien-Sheng Chao
Summary: We fabricated FeRAM and FeFET devices using a bilayer HfxZr1-xO2 (HZO), consisting of 5-nm-thick antiferroelectric HZO and 5-nm-thick ferroelectric HZO. Grazing-incidence x-ray diffraction and TEM results showed higher orthorhombic phase and larger grain size. By employing low temperature atomic layer deposition, we improved the leakage current (<3 x 10(-5) A/cm(2) under +/- 2V), gate control ability, memory window (>1.5V) and endurance (>10(7) cycles), indicating the promising potential of low-temperature ALD for non-volatile memory devices.
IEEE ELECTRON DEVICE LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Mikko Nisula, Antti J. Karttunen, Eduardo Solano, Girish C. Tewari, Maarit Karppinen, Matthias Minjauw, Himanshu Sekhar Jena, Pascal Van der Voort, Dirk Poelman, Christophe Detavernier
Summary: The study explores the relationship between the electrical conductivity, structure, and oxidation state of one-dimensional coordination polymer thin films of N,N'-dimethyl dithiooxamidato-copper prepared by atomic/molecular layer deposition. The results indicate that the electrical conductivity of the films is highly dependent on the oxidation state, with a significant increase in conductivity upon partial reduction and the observed metallic behavior in the high-conductance state.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Konstantin G. Wirth, Jonas B. Hauck, Alexander Rothstein, Hristiyana Kyoseva, Dario Siebenkotten, Lukas Conrads, Lennart Klebl, Ammon Fischer, Bernd Beschoten, Christoph Stampfer, Dante M. Kennes, Lutz Waldecker, Thomas Taubner
Summary: In this study, ABCB stacked tetralayer graphene domains were identified and characterized using scattering-type scanning near-field optical microscopy and confocal Raman microscopy. By comparing experimental results with theoretical predictions, a reliable method for the recognition of ABCB domains in tetralayer graphene was established.
Article
Chemistry, Multidisciplinary
Hui Zhang, Yue Yu, Xinyue Dai, Jinshan Yu, Hua Xu, Shanshan Wang, Feng Ding, Jin Zhang
Summary: By combining aberration-corrected scanning transmission electron microscopy and density functional theory calculations, this study investigated the fracture mechanics of 2D rhenium disulfide, revealing distinctive crack behaviors at different grain boundaries. The results show that grain boundaries aligned with Re chains are more prone to brittle intergranular fracture, while those not aligned with Re chains exhibit high resistance to fracture, impeding crack propagation. These findings provide new insights for material reinforcement and controllable cutting through grain boundary engineering.
Article
Chemistry, Multidisciplinary
Robert M. Pankow, Alexandra Harbuzaru, Ding Zheng, Brendan Kerwin, Giacomo Forti, Isaiah D. D. Duplessis, Bryan Musolino, Rocio P. Ponce Ortiz, Antonio Facchetti, Tobin J. J. Marks
Summary: For the first time, we demonstrate the ability of a porous semiconducting polymer film to enable easy penetration of electrolyte through vertically stacked polymer layers, enabling electrochromic switching between different types of polymers. The fabricated films are extensively characterized and incorporated into single and multilayer electrochromic devices. These results provide a proof of concept for the development of new types of electrochromic devices with precise control over semiconductor film morphology and polymer electronic structure.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Eric R. R. Hoglund, De-Liang Bao, Andrew O'Hara, Thomas W. W. Pfeifer, Md Shafkat Bin Hoque, Sara Makarem, James M. M. Howe, Sokrates T. T. Pantelides, Patrick E. E. Hopkins, Jordan A. A. Hachtel
Summary: Grain boundaries are a common microstructural feature that greatly influence the functionality of various materials. Extensive experimental and theoretical studies have been conducted to understand the correlation between atomic-scale grain boundary structures and macroscopic properties. In this study, a SrTiO3 grain boundary was examined using advanced microscopy and spectroscopy techniques, along with density functional theory. The results provide insights into the impact of individual boundaries on macroscopic properties through the analysis of localized grain boundary vibrations.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Wenjie Li, Weimin Li, Guo Chen, Liyun Wu, Jun Zhang, Ming Chen, Guohua Zhong, Junyi Zhu, Ye Feng, Hao Zeng, Chunlei Yang
Summary: Conducting atomic force microscopy is used to investigate the mechanism behind the lower power conversion efficiency (PCE) of CZTS solar cells compared to CIGS solar cells. The difference in efficiency is attributed to the distinct band alignment at the grain boundaries and grain interior for the two materials. CZTS demonstrates type-I band alignment, leading to enhanced carrier recombination and decreased PCE.
Article
Chemistry, Multidisciplinary
Penghui Li, Yeqiang Bu, Linyan Wang, Chong Wang, Junquan Huang, Ke Tong, Yujun Chen, Julong He, Zhisheng Zhao, Bo Xu, Zhongyuan Liu, Guoying Gao, Anmin Nie, Hongtao Wang, Yongjun Tian
Summary: Fracture behaviors in perfect and twinned B4C crystals were studied via in situ TEM mechanical testing. It was found that cracks preferentially initiated at the twin boundaries (TBs) and propagated along them, resulting in the fracture of B4C. The theoretical calculations also showed a softening effect of TBs on B4C, with amorphous bands preferentially nucleated at the TBs. These findings clarify the atomic arrangement and the role of planar defects in the failure of B4C.
ADVANCED MATERIALS
(2022)
Article
Materials Science, Multidisciplinary
Xianming Yang, Weiguo Wang, Xinfu Gu
Summary: The study found that in BCC metals, grain boundaries with {0 1 1}/{0 1 1} inter-connections have higher forming ability and corrosion resistance, making them suitable as near singular boundaries. This discovery is significant for grain boundary design and control in BCC metals.
PHILOSOPHICAL MAGAZINE
(2022)
Article
Materials Science, Multidisciplinary
Snehanshu Pal, K. Vijay Reddy, Tingting Yu, Jianwei Xiao, Chuang Deng
Summary: The study reveals that in nanocrystalline Ni and Al models, the atomic excess volume and excess energy in grain boundaries exhibit a skew-normal distribution, and there is a weak inverse correlation between the two. The correlation between atomic excess volume and excess energy strongly depends on the type of grain boundary, indicating the absence of a universal trend between the two properties.
JOURNAL OF MATERIALS SCIENCE
(2021)
Review
Chemistry, Multidisciplinary
Liu Yang, Yanyan Wang, Xu Wang, Shareen Shafique, Fei Zheng, Like Huang, Xiaohui Liu, Jing Zhang, Yuejin Zhu, Chuanxiao Xiao, Ziyang Hu
Summary: This review focuses on the application of atomic force microscopy (AFM)-based scanning probing techniques in investigating the local properties of polycrystalline photovoltaic materials. By studying the optoelectronic heterogeneities at grain interiors (GIs) and grain boundaries (GBs), it is possible to understand their critical roles in device performance and guide optimization. The potential of these AFM-based techniques in developing next-generation photovoltaics and optoelectronics is also discussed.
Review
Chemistry, Multidisciplinary
Seong-Jun Yang, Min-Yeong Choi, Cheol-Joo Kim
Summary: This review discusses the importance and challenges of engineering boundary structures in 2D materials, and explores current techniques and future directions for structure control.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yuhui Ma, Yuanhang Cheng, Xiuwen Xu, Menglin Li, Chujun Zhang, Sin Hang Cheung, Zixin Zeng, Dong Shen, Yue-Min Xie, Ka Lok Chiu, Fen Lin, Shu Kong So, Chun-Sing Lee, Sai-Wing Tsang
Summary: While the passivation effect of polymers with large and small dipole moments on MAPbI(3) perovskite films is negligible, they can significantly improve the stability of photovoltaic devices under continuous light irradiation. The additives are able to strongly suppress ion migration, enhancing the electrical-field stress tolerance of perovskite solar cells.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Irena Senkovska, Volodymyr Bon, Leila Abylgazina, Matthias Mendt, Jan Berger, Gregor Kieslich, Petko Petkov, Jhonatan Luiz Fiorio, Jan-Ole Joswig, Thomas Heine, Larissa Schaper, Christopher Bachetzky, Rochus Schmid, Roland A. A. Fischer, Andreas Poeppl, Eike Brunner, Stefan Kaskel
Summary: Flexible porous frameworks are a cutting-edge area of materials research due to their ability to adaptively open and close pores induced by chemical and physical stimuli, offering a wide range of functions. However, the factors influencing the switchability are still poorly understood, including the role of building blocks, crystal size, defects, cooperativity, and host-guest interactions. This review discusses an integrated approach using idealized model materials to systematically investigate and understand the critical factors affecting framework dynamics, leading to progress in their understanding and application.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Eric Vogelsberg, Marco Moors, Anastasia S. Sorokina, Dmitry A. Ryndyk, Sebastian Schmitz, Jessica S. Freitag, Anastasia V. Subbotina, Thomas Heine, Bernd Abel, Kirill Yu. Monakhov
Summary: We present a chemically programmed design and switching characteristics of a functional metal-DNA-origami-polyoxometalate (POM) material synthesized through solution-processing. The DNA origami acts as a carrier structure, controlling the hybridization of six-helix bundle (6HB) positions with DNA-augmented POV6 units on a gold surface. The electron acceptance and injection into the non-conducting DNA structure and release to the gold substrate depend on the potential at the nanoscale tip and the oxidation state of POV6.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Hongde Yu, Jianwei Sun, Thomas Heine
Summary: This study establishes a benchmark dataset of 25 magnetic systems, including triangulene monomer, dimer, and their analogues, to evaluate the performance of 22 commonly used density functional theory (DFT) methods in material science. The results show that achieving quantitative accuracy with small relative errors is currently not feasible. PBE0, M06-2X, and MN15 functionals are able to predict the correct electronic ground state for all systems and have the lowest mean absolute error for predicting Delta E (spin) and J. Therefore, they can serve as starting points for higher-level methods such as GW or the random phase approximation. Other functionals that fail to predict the ground state are not recommended for metal-free magnetic systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
Lars Grunenberg, Goekcen Savasci, Sebastian T. Emmerling, Fabian Heck, Sebastian Bette, Afonso Cima Bergesch, Christian Ochsenfeld, Bettina V. Lotsch
Summary: We present a facile method for synthesizing nitrone-linked covalent organic frameworks (COFs) from imine- and amine-linked COFs. The resulting nitrone-linked COFs exhibit high crystallinity, large surface areas, and improved water adsorption properties compared to their imine- or amine-linked precursors.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Charlotte Koschnick, Maxwell W. Terban, Ruggero Frison, Martin Etter, Felix A. Boehm, Davide M. Proserpio, Simon Krause, Robert E. Dinnebier, Stefano Canossa, Bettina V. Lotsch
Summary: This study reports the synthesis of three topologically different MOFs based on the same M6O4(OH)4 clusters (M = Zr or Hf) and methane-tetrakis(p-biphenyl-carboxylate) (MTBC) linkers. The variable coordination geometry of Zr-oxo clusters and the conformational flexibility of the linker contribute to the outstanding diversity of Zr-based MOFs. The structural disorder of the MOFs expands the range of achievable topologies.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Sebastian T. Emmerling, Johannes Maschita, Bettina V. Lotsch
Summary: Covalent organic frameworks (COFs) are versatile platforms for gas separation and storage. In this study, nitric oxide (NO) is used as a reagent for the scalable gas-phase transformation of COFs. The study reveals the interaction and clean deamination of COFs by NO, providing a unique surface passivation strategy. Furthermore, NONOate-COFs show promise as tunable NO delivery platforms for bioregulatory NO release in biomedical applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Kejun Liu, Julien Rehault, Baokun Liang, Mike Hambsch, Yingying Zhang, Sezer Seckin, Yunxia Zhou, Rishi Shivhare, Peng Zhang, Miroslav Polozij, Tobias A. F. Koenig, Haoyuan Qi, Shengqiang Zhou, Andreas Fery, Stefan C. B. Mannsfeld, Ute Kaiser, Thomas Heine, Natalie Banerji, Renhao Dong, Xinliang Feng
Summary: A novel crystalline q2D polypyrrole (q2DPPy) film was synthesized at the air/H2SO4 (95%) interface, which exhibited a layered assembly of protonated quinoidal chains with a fully extended conformation. The temperature-dependent charge-transport properties of q2DPPy were investigated using the van der Pauw method and terahertz time-domain spectroscopy, revealing a semiconducting behavior with a thermally activated hopping mechanism in long-range transport between the electrodes and a record short-range high THz mobility.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Maximilian A. A. Plass, Maxwell W. W. Terban, Tanja Scholz, Igor Moudrakovski, Viola Duppel, Robert E. E. Dinnebier, Bettina V. V. Lotsch
Summary: The structure of the first lithium-containing bismuthortho (o)-thiophosphate was determined using a combination of powder X-ray, neutron, and electron diffraction. The disordered distribution of lithium ions within the host structure was investigated, and the lithium ion dynamics and diffusion pathways were studied. The total lithium ion conductivities and activation energies were measured, showing a range of values depending on the bismuth content.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Tatiana E. Gorelik, Peer Lukat, Christian Kleeberg, Wulf Blankenfeldt, Rolf Mueller
Summary: This study evaluated the performance of molecular replacement (MR) procedures for structure analysis of small-molecule crystal structures from 3D electron diffraction (ED) data. By using different data types and search models, MR was successfully conducted at a resolution of 2 angstrom for the crystal structure of Bi-3812.
ACTA CRYSTALLOGRAPHICA A-FOUNDATION AND ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Xing Huang, Shuai Fu, Cong Lin, Yang Lu, Mingchao Wang, Peng Zhang, Chuanhui Huang, Zichao Li, Zhongquan Liao, Ye Zou, Jian Li, Shengqiang Zhou, Manfred Helm, Petko St Petkov, Thomas Heine, Mischa Bonn, Hai I. Wang, Xinliang Feng, Renhao Dong
Summary: This study demonstrates a strategy for synthesizing high-mobility semiconducting coordination polymers (c-CPs) using novel conjugated ligands with reduced symmetry. The synthesized c-CPs exhibit a small band gap, dispersive energy bands, and high charge carrier mobilities, outperforming previously reported conductive coordination polymers. This molecular design strategy lays the foundation for achieving high-performance c-CP-based (opto-)electronics.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Chuanhui Huang, Weiming Sun, Yingxue Jin, Quanquan Guo, David Muecke, Xingyuan Chu, Zhongquan Liao, Naisa Chandrasekhar, Xing Huang, Yang Lu, Guangbo Chen, Mingchao Wang, Jinxin Liu, Geping Zhang, Minghao Yu, Haoyuan Qi, Ute Kaiser, Gang Xu, Xinliang Feng, Renhao Dong
Summary: Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) are a subclass of layer-stacked crystalline coordination polymers that possess both porous and conductive properties, making them suitable for energy and electronic device applications. Controlled synthesis of hierarchically nanostructured 2D c-MOFs with customized morphologies and dimensions is essential to fully utilize their electronic properties and structural features. A template strategy has been developed to achieve this via insulating MOFs-to-c-MOFs transformations, resulting in higher surface areas and improved access to active sites. The hierarchically nanostructured 2D c-MOFs show superior performance in electrical properties related applications, such as supercapacitors and gas sensors, with significant improvements in specific capacity and response intensity compared to bulk-type c-MOFs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Anupam Prasoon, Hyejung Yang, Mike Hambsch, Nguyen Ngan Nguyen, Sein Chung, Alina Mueller, Zhiyong Wang, Tianshu Lan, Philippe Fontaine, Thomas D. Kuehne, Kilwon Cho, Ali Shaygan Nia, Stefan C. B. Mannsfeld, Renhao Dong, Xinliang Feng
Summary: This study demonstrates an efficient on-water surface synthesis of crystalline monolayer 2D polyimide (2DPI) with excellent stability and coverage. By combining with exfoliated MoS2, innovative organic-inorganic hybrid van der Waals heterostructures (vdWHs) are fabricated, facilitating remarkable charge transfer and improved electron mobility.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Physical
Preetam Dacha, Mike Hambsch, Darius Pohl, Katherina Haase, Markus Loeffler, Tianshu Lan, Xinliang Feng, Bernd Rellinghaus, Stefan C. B. Mannsfeld
Summary: A solution shearing procedure is reported for fabricating micro/nano wires from a diketopyrrolopyrrole (DPP)-based polymer. The as-fabricated wires exhibit a high degree of molecular orientation and enhanced electrical performance in single wire Organic Field Effect Transistors (OFETs).
Article
Chemistry, Multidisciplinary
Xipeng Shu, Liang Hu, Thomas Heine, Yu Jing
Summary: By introducing pyridinic N in the skeletons of carbonyl aromatic compounds, the electrochemical performance can be significantly improved, making them promising organic cathode materials for lithium-ion batteries.
Article
Chemistry, Multidisciplinary
Kejun Liu, Julien Rehault, Baokun Liang, Mike Hambsch, Yingying Zhang, Sezer Seckin, Yunxia Zhou, Rishi Shivhare, Peng Zhang, Miroslav Polozij, Tobias A. F. Koenig, Haoyuan Qi, Shengqiang Zhou, Andreas Fery, Stefan C. B. Mannsfeld, Ute Kaiser, Thomas Heine, Natalie Banerji, Renhao Dong, Xinliang Feng
Summary: This study reports the synthesis of a novel crystalline q2D polypyrrole film at the air/H2SO4 interface. The film exhibits a unique molecular structure and charge transport properties.
ADVANCED MATERIALS
(2023)