Review
Chemistry, Multidisciplinary
Weijie Chi, Davin Tan, Qinglong Qiao, Zhaochao Xu, Xiaogang Liu
Summary: Single-molecule localization microscopy (SMLM) has been widely used in biology and chemistry. Fluorophores, as an essential component of SMLM, play a crucial role in obtaining super-resolution fluorescence images. Recent research on spontaneously blinking fluorophores simplifies experimental setups and extends the imaging duration of SMLM. This review provides an overview of the development of spontaneously blinking rhodamines from 2014 to 2023 and the key mechanistic aspects of intramolecular spirocyclization reactions, aiming to accelerate the advancement of super-resolution imaging technologies.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Optics
Angel Cifuentes, Johanna Tragardh
Summary: Multimode optical fiber endoscopes have gained attention as a new tool for imaging deep tissue using light microscopy. This study presents a method for particle tracking through multimode optical fibers, overcoming the limitation of a fast wide-field fluorescence imaging modality for this type of endoscope. The results demonstrate high tracking accuracy and speed.
Article
Chemistry, Multidisciplinary
Wei-Hong Yeo, Yang Zhang, Amy E. Neely, Xiaomin Bao, Cheng Sun, Hao F. Zhang
Summary: Single-molecule localization microscopy (SMLM) allows visualization of cellular nanostructures in vitro with sub-20 nm resolution. However, understanding the structural information from SMLM images has been challenging. To address this, a Monte Carlo (MC) simulation based on experimental imaging parameters was developed to generate synthetic SMLM images. This MC model was used to optimize a clustering algorithm for the separation of fluorescently labeled nuclear pore complex (NPC) proteins and to generate cellular substructures with different angles of labeling.
Article
Instruments & Instrumentation
S. Aravinth, Prakash Joshi, Partha Pratim Mondal
Summary: Molecules capable of emitting a large number of photons, known as fortunate molecules, are important for achieving high-resolution imaging. A new technique called long-exposure single molecule localization microscopy (leSMLM) is proposed to detect and analyze fortunate molecules, leading to improved spatial resolution and better visualization of molecular clusters. This technique sacrifices some temporal resolution but offers significant improvements in spatial resolution.
REVIEW OF SCIENTIFIC INSTRUMENTS
(2022)
Article
Chemistry, Physical
Ariel Rogers, Isabelle I. Niyonshuti, Alice Cai, Feng Wang, Mourad Benamara, Jingyi Chen, Yong Wang
Summary: The study focuses on the kinetics of laser-induced nanowelding of silver nanoparticles (AgNPs), with an observation that laser illumination leads to the formation of higher-order structures of AgNPs. An analytical model based on simple polymerization was developed to predict and understand the dynamics, and experimental verification was conducted by varying laser power and AgNP concentration. The merging of assemblies and diffusion-limited kinetics of laser-induced assembling were taken into account for improved modeling, and the asynchronous blinking behaviors of different regions within formed structures were observed.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Optics
Nicholas A. Vickers, Fatemeh Sharifi, Sean B. Andersson
Summary: Real-time feedback-driven single particle tracking (RT-FD-SPT) is a microscopy technique that uses feedback control loop to track single particles with high resolution. A mathematical framework based on optimization of the Fisher information is presented to select the optimal parameters for particle localization. The framework is applied to three existing fluorescence-based RT-FD-SPT techniques.
Article
Chemistry, Physical
Lucas Herdly, Peter W. Tinning, Angeline Geiser, Holly Taylor, Gwyn W. Gould, Sebastian van de Linde
Summary: Carbocyanines are excellent dyes for single-molecule localization microscopy, but their performance depends on optimized photoswitching buffers. This study examines the role of thiols in cyanine photoswitching and analyzes key metrics such as photon budget, lifetimes, and impact on image resolution. The research provides a general strategy for achieving optimal resolution in single-molecule localization microscopy and has significance for the development of novel buffers and dyes.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Optics
Oumeng Zhang, Zijian Guo, Yuanyuan He, Tingting Wu, Michael D. Vahey, Matthew D. Lew
Summary: Single-molecule orientation-localization microscopy is a powerful tool for studying biochemical processes, but the limited photon budget poses challenges for high-dimensional imaging. A raMVR microscope has been developed with isotropic 3D spatial resolution and precision in measuring molecular orientations, enabling detailed imaging of molecular dynamics within biological and chemical systems.
Article
Instruments & Instrumentation
Naoki Kamiya, Kazuki Kuramoto, Kento Takishima, Tatsuya Yumoto, Haruka Oda, Takeshi Shimi, Hiroshi Kimura, Michio Matsushita, Satoru Fujiyoshi
Summary: This article describes a superfluid helium insert developed for cryogenic microscopy of millimeter-sized specimens, which achieved three-dimensional positioning and stabilization of the sample, and obtained high-quality fluorescence images without sample exchange.
REVIEW OF SCIENTIFIC INSTRUMENTS
(2022)
Article
Cell Biology
Takahiro K. Fujiwara, Taka A. Tsunoyama, Shinji Takeuchi, Ziya Kalay, Yosuke Nagai, Thomas Kalkbrenner, Yuri L. Nemoto, Limin H. H. Chen, Akihiro C. E. Shibata, Kokoro Iwasawa, Ken P. Ritchie, Kenichi G. N. Suzuki, Akihiro Kusumi
Summary: The ultrafast camera developed by Fujiwara et al. has significantly improved the time resolution of single-molecule localization microscopy, revealing the dynamic nano-architecture of focal adhesions and leading to the model of compartmentalized focal adhesion protein islands.
JOURNAL OF CELL BIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Kai Gu, Shuzhen Liu, Chunming Liu
Summary: The development of single-molecule techniques allows for the investigation of individual molecules' properties and heterogeneities, which are difficult to obtain through ensemble measurements. This study aimed to optimize the surface preparation procedures for single-molecule fluorescence imaging in organic solvents. The researchers developed a method to control the surface density of chemically immobilized dye molecules and reduce nonspecific adsorbed impurities. The impacts of solvent polarity and surface functionality were also studied, with higher polarities leading to better control and reduced adsorption. The researchers further performed single-molecule fluorescence imaging and studied the photophysical properties of dyes and impurities in DMF, which could be used to filter out false counts in measurements.
Article
Multidisciplinary Sciences
Simao Coelho, Jongho Baek, James Walsh, J. Justin Gooding, Katharina Gaus
Summary: Two-photon direct laser writing enables nanometer-accuracy fabrication of three-dimensional structures, providing high-resolution imaging possibilities for optical microscopy.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Yang Zhang, Yu Zhang, Ki-Hee Song, Wei Lin, Cheng Sun, George C. Schatz, Hao F. Zhang
Summary: The study investigated the causes of single-molecule fluorescence spectral heterogeneities and found that they were influenced by structural rigidity and environmental changes. Factors such as system noise uncertainty and environmental polarity were ruled out. The rotational flexibility of N,N-dialkylated groups was found to contribute to the heterogeneities.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Bertus van Heerden, Tjaart P. J. Kruger
Summary: Real-time feedback-driven single-particle tracking is a technique that allows for single-molecule spectroscopy of freely diffusing particles. This study compared the performance of different methods using statistical calculations and dynamical simulations. The results showed a trade-off between precision and speed, with iSCAT providing better tracking for most samples. The study highlights the importance of selecting the appropriate method and can be extended to other techniques.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Analytical
Jie Yang, Chaoqing Dong, Aidi Zhang, Jicun Ren
Summary: This study presents a novel approach for detecting intracellular mRNA using nonblinking quantum dot dimers as probes, induced by mRNA. The detection strategy relies on the formation of nonblinking bright spots through the hybridization of target DNA (or mRNA) with a probe. Experimental results confirmed the feasibility and simplicity of this single-molecule detection method.
ANALYTICAL CHEMISTRY
(2022)
Article
Materials Science, Multidisciplinary
Jakub Sitek, Iwona Pasternak, Karolina Czerniak-Losiewicz, Michal Swiniarski, Pawel P. Michalowski, Clifford McAleese, Xiaochen Wang, Ben R. Conran, Konrad Wilczynski, Michal Macha, Aleksandra Radenovic, Mariusz Zdrojek, Wlodek Strupinski
Summary: Van der Waals heterostructures provide a unique platform for studying the fundamental physics and practical applications of two-dimensional materials. In this study, we successfully prepared a monolayered MoS2/WS2/graphene vertical heterostructure using chemical vapor deposition without the need for transfer. By employing various characterization techniques, we confirmed the vertical stacking of the three different materials. Our findings highlight the importance of the chemical potential of crystal formation and the substrate-layer adhesion energy in the synthesis of 2D materials.
Article
Nanoscience & Nanotechnology
Agata Piacentini, Damiano Marian, Daniel S. Schneider, Enrique Gonzalez Marin, Zhenyu Wang, Martin Otto, Barbara Canto, Aleksandra Radenovic, Andras Kis, Gianluca Fiori, Max C. Lemme, Daniel Neumaier
Summary: This study reports a scalable encapsulation approach for MoS2 FETs, where h-BN monolayers are employed as a barrier layer to significantly reduce charge transfer and exhibit very low hysteresis even under ambient operating conditions.
ADVANCED ELECTRONIC MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Zhenyu Wang, Mukesh Tripathi, Zahra Golsanamlou, Poonam Kumari, Giuseppe Lovarelli, Fabrizio Mazziotti, Demetrio Logoteta, Gianluca Fiori, Luca Sementa, Guilherme Migliato Marega, Hyun Goo Ji, Yanfei Zhao, Aleksandra Radenovic, Giuseppe Iannaccone, Alessandro Fortunelli, Andras Kis
Summary: In this study, high-quality NbS2-MoS2 lateral heterostructures were synthesized by one-step metal-organic chemical vapor deposition (MOCVD) with Nb substitutionally doped monolayer MoS2, showing p-type doped behavior. The heterojunction exhibited p-type transfer characteristic with a high on/off current ratio of approximately 10^4, surpassing previous reports. The band structure of the NbS2-MoS2 heterojunction was investigated using density functional theory (DFT) and quantum transport simulations. This research provides a scalable approach to synthesize doped TMDC materials and offers insight into the interface between 2D metals and semiconductors in lateral heterostructures, which is crucial for the development of next-generation nanoelectronics and highly integrated devices.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Andrey Chernev, Yunfei Teng, Mukeshchand Thakur, Victor Boureau, Lucie Navratilova, Nianduo Cai, Tzu-Heng Chen, Liping Wen, Vasily Artemov, Aleksandra Radenovic
Summary: Nature provides a wide range of self-assembled structures, and this study presents a fast, nature-inspired method for growing stalactite nanopores using heterogeneous atomic deposition. The stalactite nanostructures combine the advantages of reduced sensing region typically for 2D material nanopores with the asymmetric geometry of capillaries, resulting in ionic selectivity, stability, and scalability. The proposed growing method provides an adaptable nanopore platform for basic and applied nanofluidic research.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Vasily Artemov, Laura Frank, Roman Doronin, Philipp Staerk, Alexander Schlaich, Anton Andreev, Thomas Leisner, Aleksandra Radenovic, Alexei Kiselev
Summary: The surface charge of an open water surface is determined by electrostatic effects in the contact line vicinity of three phases. The contact potential difference between two aqueous interfaces created by charge redistribution is shown to be pH-dependent. This discovery provides insights into solvation phenomena and interfacial processes in aqueous systems and has implications for various experimental environments.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Nanoscience & Nanotechnology
S. M. Leitao, V. Navikas, H. Miljkovic, B. Drake, S. Marion, G. Pistoletti Blanchet, K. Chen, S. F. Mayer, U. F. Keyser, A. Kuhn, G. E. Fantner, A. Radenovic
Summary: In current nanopore-based label-free single-molecule sensing technologies, stochastic processes make it challenging to control the selection, rate, and velocity of single-molecule translocations. This study proposes a method that uses a glass nanopore mounted on a three-dimensional nanopositioner to spatially select and deterministically translocate molecules tethered on a glass surface. By controlling the distance between the nanopore and glass surface, the region of interest on the molecule can be actively selected and scanned at a controlled number of times and velocity. The method demonstrates versatility in assessing DNA-protein complexes, DNA rulers, and DNA gaps, enabling single-nucleotide gap detection.
NATURE NANOTECHNOLOGY
(2023)
Article
Multidisciplinary Sciences
Alexey M. Romshin, Vadim Zeeb, Evgenii Glushkov, Aleksandra Radenovic, Andrey G. Sinogeikin, Igor I. Vlasov
Summary: We present a novel approach to manipulate the temperature of individual living cells and their compartments using a polycrystalline diamond particle containing silicon-vacancy color centers. This particle acts as both a heater and a thermometer, allowing for precise control and measurement of local temperature changes. By heating the vicinity of HeLa cells and isolated mouse hippocampal neurons, we observe alterations in the intracellular distribution of free calcium ions, indicating the importance of temperature in cellular processes.
SCIENTIFIC REPORTS
(2023)
Article
Nanoscience & Nanotechnology
Mukeshchand Thakur, Nianduo Cai, Miao Zhang, Yunfei Teng, Andrey Chernev, Mukesh Tripathi, Yanfei Zhao, Michal Macha, Farida Elharouni, Martina Lihter, Liping Wen, Andras Kis, Aleksandra Radenovic
Summary: Nanopores in 2D membranes, especially in single-layer MoS2, have great potential in various applications. However, the stability of these nanopores remains a challenge. This study identifies chemical oxidation and delamination of monolayers as the main reasons for instability and proposes surface modification and reducing oxygen to improve nanopore stability. Understanding nanopore growth and stability can lead to controlled pore size and shape and enable durable nanopore devices with high signal-to-noise ratio.
NPJ 2D MATERIALS AND APPLICATIONS
(2023)
Article
Biology
Arielle Louise Planchette, Cedric Schmidt, Olivier Burri, Mercedes Gomez de Agueero, Aleksandra Radenovic, Alessio Mylonas, Jerome Extermann
Summary: Optical projection tomography (OPT) enables the observation and understanding of tissue-wide networks in three dimensions. A multi-modal workflow for characterizing the mouse small intestine is presented, demonstrating its applicability for imaging the intestinal immune compartment and mucosal structures.
COMMUNICATIONS BIOLOGY
(2023)
Article
Nanoscience & Nanotechnology
Jakub Sitek, Karolina Czerniak-Losiewicz, Arkadiusz P. Gertych, Malgorzata Giza, Pawel Dabrowski, Maciej Rogala, Konrad Wilczynski, Anna Kaleta, Slawomir Kret, Ben R. Conran, Xiaochen Wang, Clifford McAleese, Michal Macha, Aleksandra Radenovic, Mariusz Zdrojek, Iwona Pasternak, Wlodek Strupinski
Summary: Researchers have achieved the selective fabrication of van der Waals heterostructures (vdWHSs) using chemical vapor deposition by electron-beam irradiation. They have identified two growth modes, positive (P) mode on graphene and tungsten disulfide (WS2) substrates, and negative (N) mode on the graphene substrate. The growth mode can be controlled by limiting the air exposure and the time between irradiation and growth. The selective growth mechanism is explained by the competition of three effects: EB-induced defects, adsorption of carbon species, and electrostatic interaction. This study is a critical step towards industry-scale fabrication of 2D-materials-based devices.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Svetlana Melnik, Alexander Ryzhov, Alexei Kiselev, Aleksandra Radenovic, Tanja Weil, Keith J. Stevenson, Vasily G. Artemov
Summary: The electrodynamics properties of nanoconfined water have been significantly changed compared to bulk water, providing opportunities for safe electrochemical systems. We present a nanofluidic water-only battery that exploits the unusually high electrolytic properties of pure water under strict confinement. The device, composed of carbon-based nanomaterials, creates interconnected nanochannels filled with water between the separator and electrodes. The efficiency of the battery shows a maximum energy density at 3 nm, challenging the current metal-ion batteries. Our findings establish the electrodynamic fundamentals of nanoconfined water and pave the way for low-cost and inherently safe energy storage solutions needed in the renewable energy sector.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Guilherme Migliato Marega, Zhenyu Wang, Yanfei Zhao, Hyun Goo Ji, Asmund Ottesen, Mukesh Tripathi, Aleksandra Radenovic, Andras Kis
Summary: Memory devices have gained attention again due to the increasing interest in using in-memory computing architectures. Flash memories based on monolayer MoS2 show promise as the ideal elements for this technology, but achieving large-area ultra-fast operation remains a challenge.
IEEE NANOTECHNOLOGY MAGAZINE
(2023)
Meeting Abstract
Biophysics
Jenny Sulzle, Wayne Yang, Yuta Shimoda, Eveline S. Mayner, Michal Macha, Nathan Ronceray, Aleksandra Radenovic, Suliana Manley
BIOPHYSICAL JOURNAL
(2023)
Meeting Abstract
Biophysics
Wayne Yang, Jenny Sulzle, Yuta Shimoda, Eveline Mayner, Michal Macha, Nathan Ronceray, Suliana Manley, Aleksandra Radenovic
BIOPHYSICAL JOURNAL
(2023)
Article
Engineering, Electrical & Electronic
Guilherme Migliato Marega, Hyun Goo Ji, Zhenyu Wang, Gabriele Pasquale, Mukesh Tripathi, Aleksandra Radenovic, Andras Kis
Summary: Data-driven algorithms are needed to process the massive amounts of data being produced, but the traditional von Neumann architecture limits processing capabilities, leading to the development of in-memory computing. This research presents an integrated 32x32 vector-matrix multiplier using floating-gate field-effect transistors with monolayer molybdenum disulfide as the channel material. Wafer-scale fabrication achieves high yield and low variability, and statistical analysis reveals the potential for multilevel and analogue storage. Reliable parallel signal processing is also demonstrated. In-memory computing chips for vector-matrix multiplication and signal processing can be fabricated using these transistors.
NATURE ELECTRONICS
(2023)