Article
Chemistry, Multidisciplinary
Brent Lawson, Percy Zahl, Mark S. Hybertsen, Maria Kamenetska
Summary: Single-molecule circuits with group 8 metallocenes are formed without additional linker groups in scanning tunneling microscope-based break junction measurements. The nature of the gold-pi binding motif and its effect on molecular conductance and persistence characteristics during junction evolution are investigated. The interaction between the cyclopentadienyl rings of the metallocenes and the gold electrodes allows for extended conductance plateaus.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Kai Qu, Ping Duan, Jin-Yun Wang, Bochao Zhang, Qian-Chong Zhang, Wenjing Hong, Zhong-Ning Chen
Summary: This study successfully identified the internal rotation of three crank-shaped molecules using scanning tunneling microscope break junction technique and theoretical simulation. Theoretical computational study demonstrated that the orbital energy changes with the conformational flipping, affecting the single-molecule conductance.
Article
Multidisciplinary Sciences
Takanori Harashima, Shintaro Fujii, Yuki Jono, Tsuyoshi Terakawa, Noriyuki Kurita, Satoshi Kaneko, Manabu Kiguchi, Tomoaki Nishino
Summary: The electrical properties of DNA in the field of molecular electronics have been extensively studied, with a focus on the higher-order structures and design changes associated with single-molecule electronic devices. Researchers have developed a DNA zipper configuration to form a single-molecule junction, which exhibits high conductivity and an attractive self-restoring capability. This strategy provides a basis for novel designs of single-molecule junctions.
NATURE COMMUNICATIONS
(2021)
Article
Materials Science, Multidisciplinary
Huanyan Fu, Cong Zhao, Jie Cheng, Shuyao Zhou, Peizhen Peng, Jie Hao, Zhirong Liu, Xike Gao, Chuancheng Jia, Xuefeng Guo
Summary: This study designs an azulene-based single-molecule FET with ambipolar characteristics and improved gate controllability using ionic liquid gating. Experimental and theoretical research show that the inherent dipole moment of azulene is crucial for achieving high-efficiency gate control.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Yaping Zang, E-Dean Fung, Tianren Fu, Suman Ray, Marc H. Garner, Anders Borges, Michael L. Steigerwald, Satish Patil, Gemma Solomon, Latha Venkataraman
Summary: The structural changes in a DPP molecule induced by charge transport at a high bias increase the average nonresonant conductance of Au-DPP-Au junctions and lead to planarization of the molecular backbone. This conformational planarization is assisted by thermally activated junction reorganization and only occurs under specific electronic conditions.
Article
Chemistry, Multidisciplinary
Chun Tang, Longfeng Huang, Sara Sangtarash, Mohammed Noori, Hatef Sadeghi, Haiping Xia, Wenjing Hong
Summary: This study introduces an atomically precise gating strategy to manipulate the quantum interference patterns at the single-molecule scale, achieving a complete switching from destructive to constructive QI modes and significant conductance modulation at room temperature. The chemical gating effect exerted locally on the pyridine nitrogen through selective interaction with cationic reagents demonstrates unique capabilities in modulating QI and offers potential for developing novel electronic devices.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Saisai Yuan, Xiaohui Xu, Abdalghani Daaoub, Chao Fang, Wenqiang Cao, Hang Chen, Sara Sangtarash, Jiangwei Zhang, Hatef Sadeghi, Wenjing Hong
Summary: Single-atom control allows for modulation of electrical conductance and thermopower in polyoxometalate clusters, leading to manipulation of charge transport at the single-atom level. This work provides fundamental insight into the tuning of charge transport in POM single-cluster junctions through atomic precision.
Article
Chemistry, Multidisciplinary
Haipeng B. Li, Yan-Feng Xi, Ze-Wen Hong, Jingxian Yu, Xiao-Xia Li, Wen-Xia Liu, Lucas Domulevicz, Shan Jin, Xiao-Shun Zhou, Joshua Hihath
Summary: By studying a series of rigid, planar furan oligomers, we found that tunneling transport can change with temperature. Analyzing the correlation between molecular orbital energy offset and the Fermi level, we conclude that thermally assisted tunneling is the main cause for the temperature-dependent conductance in these systems.
Article
Chemistry, Multidisciplinary
Hannah E. Skipper, Brent Lawson, Xiaoyun Pan, Vera Degtiareva, Maria Kamenetska
Summary: Understanding and manipulating quantum interference effects in single molecule junction conductance can lead to the design of molecular-scale devices. In this study, quantum interference between σ and π molecular orbitals in a pyrazine molecule bridging source and drain electrodes was demonstrated. The researchers utilized measurements, analysis, and calculations to show that this phenomenon leads to distinct patterns of electron transport in nanoscale junctions, which can be controlled by manipulating the environmental pH. This work provides a conceptual framework for engineering quantum interference features in short molecular systems.
Review
Nanoscience & Nanotechnology
Hongliang Chen, Chuancheng Jia, Xin Zhu, Chen Yang, Xuefeng Guo, J. Fraser Stoddart
Summary: Developing new materials is a long-standing goal in various fields, and understanding single-molecule reactions can deepen our understanding of chemical reactions and provide new frameworks in materials science. This review focuses on state-of-the-art chemical reactions in single-molecule junctions and highlights the advantages of real-time testbeds for studying reaction dynamics, intermediates, transition states, and solvent effects. The behavior of single-molecule reactions is compared with reactions in ensemble states, and the potential of leveraging single-molecule catalysis for large-scale materials production is explored.
NATURE REVIEWS MATERIALS
(2023)
Article
Electrochemistry
Richard J. Nichols
Summary: EC-STM is a vital tool in modern interfacial electrochemistry, allowing for quantitative studies of electron transfer (ET) mechanisms; monitoring charge flow through single molecules can analyze ET mechanisms, covering a range from superexchange to 2-step hopping mechanisms like the Kuznetsov Ulstrup (KU) mechanism.
ELECTROCHIMICA ACTA
(2021)
Article
Chemistry, Multidisciplinary
Bohuai Xiao, Suhang He, Mingjun Sun, Jianghao Zhou, Zhiye Wang, Yunchuan Li, Simin Liu, Werner M. Nau, Shuai Chang
Summary: This study introduces a versatile recognition tunneling technique using doubly cucurbit[7]uril-functionalized electrodes to form supramolecular junctions that capture analytes dynamically by host-guest complexation, resulting in characteristic changes in their single-molecule conductance. For structurally related drug molecules and mixtures, distinct current switching signals related to their intrinsic conductance properties and pH-dependent effects are observed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Letter
Chemistry, Multidisciplinary
Yahia Chelli, Serena Sandhu, Abdalghani H. S. Daaoub, Sara Sangtarash, Hatef Sadeghi
Summary: It has been found that quantum interference in single molecules can be controlled by changing the spin state of stable open-shell organic radicals, resulting in a significant change in their electrical conductance. This discovery opens up new possibilities for spin interference-based molecular switches for energy storage and conversion applications.
Article
Nanoscience & Nanotechnology
Julia E. Greenwald, Joseph Cameron, Neil J. Findlay, Tianren Fu, Suman Gunasekaran, Peter J. Skabara, Latha Venkataraman
Summary: Researchers have successfully created a molecular system where the constructive quantum interference between certain molecular orbitals is suppressed, while the destructive interference between other molecular orbitals is enhanced, leading to highly nonlinear single-molecule circuits. They demonstrated the effectiveness of this strategy using fluorene oligomers containing a central benzothiadiazole unit, achieving a reproducible modulation of the conductance of a 6-nm molecule by more than 10,000 at room temperature.
NATURE NANOTECHNOLOGY
(2021)
Review
Biochemistry & Molecular Biology
Mong-Wen Gu, Chun-hsien Chen
Summary: The contact between molecules and electrodes is crucial for electron transport in molecule-based devices. The electrode-molecule-electrode configuration is used as a testbed to quantitatively study the underlying physical chemistry. This review focuses on examples of electrode materials and introduces basic concepts and experimental techniques.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Review
Chemistry, Multidisciplinary
Zhibin Zhao, Saurabh Soni, Takhee Lee, Christian A. Nijhuis, Dong Xiang
Summary: Eutectic gallium-indium (EGaIn) is a liquid metal that has attracted significant attention due to its excellent properties. It can be adjusted and mixed with other materials to obtain composite materials with extended properties. This review provides an introduction to the unique properties of EGaIn, illustrates the working principles of EGaIn-based devices, and summarizes the developments in EGaIn-related techniques. Additionally, it reviews the applications of EGaIn in various fields and discusses the challenges and potential applications for the development of EGaIn-based techniques.
ADVANCED MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Giorgio Cortelli, Leroy Grob, Luca Patruno, Tobias Cramer, Dirk Mayer, Beatrice Fraboni, Bernhard Wolfrum, Stefano de Miranda
Summary: Nowadays, many applications in various fields are utilizing micropillars, such as optics, tribology, biology, and biomedical engineering. One of the most attractive applications is the use of three-dimensional microelectrode arrays for in vivo and in vitro studies. The accurate mechanical characterization of the micropillar is crucial in the fabrication and optimization of such devices, as it determines their reliability.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Xueyan Zhao, Xubin Zhang, Kaikai Yin, Surong Zhang, Zhikai Zhao, Min Tan, Xiaona Xu, Zhibin Zhao, Maoning Wang, Bingqian Xu, Takhee Lee, Elke Scheer, Dong Xiang
Summary: The ability to regulate nanogap size is essential for molecular junctions and control of optical signals. This study proposes two approaches for in situ adjustable metal gaps with high resolution, which can be used in wafer-compatible nanogaps and in-plane molecular break junctions. These adjustable nanogaps allow for repeated opening and closing, providing insights into the conductance of single molecules and molecular dimers. The wafer-compatible nanogaps and in-plane break-junctions offer potential for compact devices and dynamical studies of single molecules.
Article
Chemistry, Analytical
Angelica Dominguez-Aragon, Erasto Armando Zaragoza-Contreras, Gabriela Figueroa-Miranda, Andreas Offenhausser, Dirk Mayer
Summary: A novel sandwich-type electrochemical immunosensor was developed for the quantitative detection of carcinoembryonic antigen, a significant tumor marker. The immobilization of antibodies was achieved through Au-S bonds using a novel photochemical technique, allowing control over antibody orientation. The SWCNH/Thi/AuNPs nanocomposite acted as a signal tag for detection and signal amplification. The immunoassay demonstrated a linear detection range from 0.001-200 ng/mL with a low detection limit of 0.1385 pg/mL. Carbon nanohorns hold promise as a conductive and binding matrix for signal amplification in clinical diagnostics.
Article
Physics, Applied
Zhibin Zhao, Zemin Zhang, Jieyi Zhang, Mingwei Wang, Yuelong Li, Dong Xiang
Summary: Metal electrode materials are crucial for the performance of microscale perovskite-based devices. However, it is challenging to investigate the influence of different metal electrode materials on the same microscale perovskite piece. A strategy using liquid metal as top electrode was proposed to fabricate soft-sandwiched perovskite junctions, allowing for replacement of bottom electrode without damage. The shape of photocurrent is mainly controlled by light intensity, while the rectification ratio is determined by electrode materials.
APPLIED PHYSICS LETTERS
(2023)
Editorial Material
Chemistry, Multidisciplinary
Xueyan Zhao, Adila Adijiang, Dong Xiang
CHINESE CHEMICAL LETTERS
(2023)
Review
Chemistry, Analytical
Ziheng Hu, Yaqi Li, Gabriela Figueroa-Miranda, Simon Musall, Hangyu Li, Mateo Alejandro Martinez-Roque, Qinyu Hu, Lingyan Feng, Dirk Mayer, Andreas Offenhaeusser
Summary: Neurotransmitters control signal transmission in chemical synapses by being released from the pre-synaptic neuron and binding to receptors in the postsynaptic neuron. Measurement of neurotransmitter concentrations with high spatiotemporal resolution is essential for understanding brain function and dysfunction in neurological diseases. Aptamer based biosensors are a valuable tool in achieving this goal, offering advantages in tailoring receptors for specific tasks.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Zhibin Zhao, Yuelong Li, Lifa Ni, Jongwoo Nam, Adila Adijiang, Xubin Zhang, Shanshan Li, Mingwei Wang, Takhee Lee, Dong Xiang
Summary: The role of electrode contact geometries in determining the device performance of crystals-based photoelectric devices was investigated by using a liquid metal as an adaptive-deformable electrode. The study found that the carrier transport through perovskite microcrystals can be adjusted by modifying the electrode contacts geometries/positions. Switching, rectifying, and memristor functions were selectively realized by changing the contact geometry, and the underlying mechanism for these observations was elucidated.
ADVANCED MATERIALS INTERFACES
(2023)
Editorial Material
Multidisciplinary Sciences
Xubin Zhang, Adila Adijiang, Dong Xiang
NATIONAL SCIENCE REVIEW
(2023)
Article
Chemistry, Multidisciplinary
Ruifeng Zhu, Gabriela Figueroa-Miranda, Lei Zhou, Ziheng Hu, Bohdan Lenyk, Sven Ingebrandt, Andreas Offenhaeusser, Dirk Mayer
Summary: A dual-signal protocol was developed, combining electrochemical and optical detection methods using gold nanopit arrays, to improve aptamer-based biosensors. The non-fully penetrating AuNpA showed better plasmonic properties and enlarged the electrochemical active surface area compared to fully penetrating structures. The simultaneous use of electrochemical and optical transducers led to different detection limits, dynamic ranges, and sensitivities, providing new opportunities for disease diagnosis and point-of-care testing.
Article
Chemistry, Analytical
Ziheng Hu, Ruifeng Zhu, Gabriela Figueroa-Miranda, Lei Zhou, Lingyan Feng, Andreas Offenhaeusser, Dirk Mayer
Summary: This study presents an electrochemical aptasensor for highly sensitive and selective serotonin (ST) detection, based on truncated DNA aptamers and a polyethylene glycol (PEG) molecule-functionalized sensing interface. The aptasensor shows improved sensitivity and enhanced antifouling ability due to the small size and stable structure of the truncated aptamers, as well as the blocking effect of PEG molecules. The sensor exhibits a wide detection range and low limit of detection, and also demonstrates high selectivity and stability in detecting ST in human serum and artificial cerebrospinal fluid (aCSF).
Article
Materials Science, Biomaterials
Lina Koschinski, Bohdan Lenyk, Marie Jung, Irene Lenzi, Bjoern Kampa, Dirk Mayer, Andreas Offenhaeusser, Simon Musall, Viviana Rincon Montes
Summary: The combination of electrophysiology and neuroimaging methods allows simultaneous measurement of electrical activity signals with calcium dynamics in vivo. Transparent neural implants have been proposed to overcome limitations of traditional techniques, but their effectiveness remains unclear. This study compared two types of transparent surface micro-electrocorticography (mu ECoG) implants and found that the combination of solid gold interconnects and PEDOT:PSS-based electrodes offered the best overall properties for long-term chronic multimodal recordings. These implants showed functional stability for four months and allowed simultaneous mapping of electrical and calcium neural signals during imaging.
JOURNAL OF MATERIALS CHEMISTRY B
(2023)
Article
Biophysics
Yuanying Liang, Gabriela Figueroa-Miranda, Julian Alexander Tanner, Fei Huang, Andreas Offenhaeusser, Dirk Mayer
Summary: In this research, integrated organic electrochemical transistors (iOECTs) with different channel geometries were designed for point-of-care diagnosis of malaria using aptamer as receptor. The experiment showed that iOECTs with thin channels exhibited superior sensitivity for malaria detection, with a detection limit as low as 3.2 aM.
BIOSENSORS & BIOELECTRONICS
(2023)