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| Open AccessSpatially resolved multi-omics highlights cell-specific metabolic remodeling and interactions in gastric cancer
The spatial signature of metabolic remodeling in tumours remains to be explored. Here, the integration of mass spectrometry imaging-based spatial metabolomics and lipidomics with microarray-based spatial transcriptomics allows the visualisation of metabolic heterogeneity in gastric cancer.
- Chenglong Sun
- , Anqiang Wang
- & Jiuming He
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Article
| Open AccessHigh-resolution discrimination of homologous and isomeric proteinogenic amino acids in nanopore sensors with ultrashort single-walled carbon nanotubes
Ultrashort single-walled carbon nanotubes inserted in lipid bilayers can be used as nanopore sensors. Here, the authors demonstrate the high-resolution discrimination of homologous and isomeric proteinogenic amino acids with such carbon-based nanopores.
- Weichao Peng
- , Shuaihu Yan
- & Yuliang Zhao
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Article
| Open AccessDesigning reliable and accurate isotope-tracer experiments for CO2 photoreduction
Current verification of CO2 photoreduction products using isotope-tracer methods is insufficient and can provide false-positive results. Here, rigorous protocols and case studies are presented to avoid pitfalls in isotope-tracer experiments.
- Shengyao Wang
- , Bo Jiang
- & Jinhua Ye
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Article
| Open AccessSolvent-derived defects suppress adsorption in MOF-74
Defects in metal-organic frameworks impact their structure and properties. Here authors uncover formate defects in MOF-74 that originate from decomposed DMF solvent. NMR shows that the defects partially eliminate open metal sites and lead to a decrease of gas adsorption; the adsorption mechanism of CO2 in defective MOF is also elucidated.
- Yao Fu
- , Yifeng Yao
- & Xueqian Kong
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Article
| Open AccessSwitchable biomimetic nanochannels for on-demand SO2 detection by light-controlled photochromism
Conventional nanochannel sensors are passively responsive and may be slowly damaged by analytes present in the environment before detection. Here, authors developed a light-controlled inert/active-switchable biomimetic nanochannel sensor to achieve SO2 on-demand detection and long-term preservation.
- Dan Zhang
- , Yongjie Sun
- & Xuanjun Zhang
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Article
| Open AccessUnequivocal identification of two-bond heteronuclear correlations in natural products at nanomole scale by i-HMBC
The inability to distinguish two-bond from long-range HMBC correlation has historically impeded NMR structure elucidation. Here the authors developed a practical iHMBC methodology utilizing accurate isotope shift measurement to overcome this limitation.
- Yunyi Wang
- , Aili Fan
- & Xiao Wang
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Article
| Open AccessIn situ orderly self-assembly strategy affording NIR-II-J-aggregates for in vivo imaging and surgical navigation
J-aggregation, is an effective strategy to extend the wavelength of organic NIR-II fluorescence dyes but weak intermolecular interactions often lead to decomposition of the aggregates in biological environment. Here, the authors demonstrate a series of activatable quinazoline derivatives which can self-assemble in vivo into highly stable NIR-IIJ-aggregates.
- Zhe Li
- , Ping-Zhao Liang
- & Xiao-Bing Zhang
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Article
| Open AccessIdentification of tagged glycans with a protein nanopore
The structural complexity of glycans seriously challenges the currently available analytical methods. Here, the authors report the identification of glycan isomers, glycans with varying chain lengths, and distinct branched glycans, via a glycan derivatization strategy and nanopore sensing.
- Minmin Li
- , Yuting Xiong
- & Guangyan Qing
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Article
| Open AccessHigh-resolution separation of bioisomers using ion cloud profiling
Ion mobility is used in mass spectrometers for structure analysis of biomolecules. Here, the authors show that ion mobility analysis in an ion trap under ultra-high fields enables isomer separation at resolutions over 10,000, wich they demonstrate for isomers of disaccharides, phospholipids, and peptides.
- Xiaoyu Zhou
- , Zhuofan Wang
- & Zheng Ouyang
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Article
| Open AccessTwo-photon fluorescence imaging and specifically biosensing of norepinephrine on a 100-ms timescale
Norepinephrine (NE) is a key neurotransmitter in the central nervous system of organisms however specifically tracking the transient NE dynamics with high spatiotemporal resolution in living systems remains a great challenge. Herein, the authors developed a small molecular fluorescent probe that can precisely anchor on neuronal cytomembranes and specifically respond to NE on a 100-ms timescale.
- Leiwen Mao
- , Yujie Han
- & Yang Tian
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Article
| Open Access1,2,4,5-Tetrazine-tethered probes for fluorogenically imaging superoxide in live cells with ultrahigh specificity
Specific detection of cellular superoxide is challenging. Here, the authors designed 1,2,4,5-tetrazine based fluorogenic probes for specific and sensitive imaging of superoxide, and applied them in high throughput screening of modulators of oxidative stress.
- Xuefeng Jiang
- , Min Li
- & Xin Li
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Article
| Open AccessWell-TEMP-seq as a microwell-based strategy for massively parallel profiling of single-cell temporal RNA dynamics
Gene expression of cells is a heterogeneous and dynamic program involved in various biological processes. Here, authors develop Well-TEMPseq, a high-throughput, cost-effective, and accurate method for massively parallel profiling of the temporal dynamics of single-cell gene expression.
- Shichao Lin
- , Kun Yin
- & Chaoyong Yang
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Article
| Open AccessVisible light-exposed lignin facilitates cellulose solubilization by lytic polysaccharide monooxygenases
Degradation of plant biomass, comprised of cellulose and polyaromatic lignin, is promoted by light. Here, the authors show that light promotes lignin-catalyzed generation of hydrogen peroxide, which is used by redox enzymes to degrade cellulose.
- Eirik G. Kommedal
- , Camilla F. Angeltveit
- & Vincent G. H. Eijsink
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Article
| Open AccessInvestigating microstructure evolution of lithium metal during plating and stripping via operando X-ray tomographic microscopy
Understanding the plating and stripping behaviours of lithium metal is crucial for high-energy battery development. Here, authors track these electrochemical processes in real time by an operando synchrotron X-ray tomographic microscopy, revealing the formation of inactive lithium microstructures.
- Matthew Sadd
- , Shizhao Xiong
- & Aleksandar Matic
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Article
| Open AccessA supramolecular cucurbit[8]uril-based rotaxane chemosensor for the optical tryptophan detection in human serum and urine
Sensing small biomolecules in biofluids using host-guest chemosensors remains challenging, in part due to the impact of interfering components. Here, the authors develop a dual-macrocyclic rotaxane for tryptophan detection which can function in biofluids such as human serum and urine.
- Joana Krämer
- , Laura M. Grimm
- & Frank Biedermann
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Article
| Open AccessUnderstanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy
All-solid-state lithium batteries performance is affected by the solid electrolyte interphase (SEI) and electrically disconnected (“dead”) Li metal. Here, via operando NMR measurements, the authors quantify the Li metal in the SEI and “dead” regions using various inorganic solid-state electrolytes.
- Ziteng Liang
- , Yuxuan Xiang
- & Yong Yang
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Article
| Open AccessGas induced formation of inactive Li in rechargeable lithium metal batteries
The formation of electrochemically inactive, or “dead”, lithium limits the reversibility of lithium metal batteries. Here the authors elucidate the (electro)chemical roles of ethylene gas produced from electrolyte decomposition on the formation of inactive lithium.
- Yuxuan Xiang
- , Mingming Tao
- & Yong Yang
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Article
| Open AccessPlasmonic imaging of the layer-dependent electrocatalytic activity of two-dimensional catalysts
Probing the localized electrocatalytic activity of heterogeneous electrocatalysts is crucial. Here, the authors propose a method of imaging the surface charge density and electrocatalytic activity of single two-dimensional electrocatalyst nanosheets.
- Xiaona Zhao
- , Xiao-Li Zhou
- & Xian-Wei Liu
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Article
| Open AccessArginine-modified black phosphorus quantum dots with dual excited states for enhanced electrochemiluminescence in bioanalysis
Electrochemiluminescence is emitted via the radiative transition of a singlet or triplet excited state. Here, the authors propose an arginine modification of black phosphorus quantum dots that exhibits enhanced emission based on dual excited states.
- Siqi Yu
- , Yu Du
- & Huangxian Ju
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Article
| Open AccessA medium-entropy transition metal oxide cathode for high-capacity lithium metal batteries
Structural instability is a major drawback of high-capacity lithium-based battery cathodes. Here, the authors report a cathode active material with a medium-entropy state created by partial cation disordering capable of restraining the structural evolution in the high-capacity operated spinel phase.
- Yi Pei
- , Qing Chen
- & Cheng-Yan Xu
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Article
| Open AccessContinuous biomarker monitoring with single molecule resolution by measuring free particle motion
Various applications would benefit from the ability to continuously measure biomolecules. Here the authors describe a biosensing technology based on the free diffusion of biofunctionalized particles hovering over a sensor surface, which enables monitoring of analytes (pM-µM) over long timespans.
- Alissa D. Buskermolen
- , Yu-Ting Lin
- & Menno W. J. Prins
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Article
| Open AccessVisualizing inflammation with an M1 macrophage selective probe via GLUT1 as the gating target
Studying the specific roles of macrophage subsets has been hampered by a lack of subset-specific probes. Here the authors report an M1 selective fluorescent probe named CDr17, and demonstrate the suitability of this probe for tracking M1 macrophages in vivo.
- Heewon Cho
- , Haw-Young Kwon
- & Young-Tae Chang
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Article
| Open AccessDifferential nuclear import sets the timing of protein access to the embryonic genome
Here the authors address how embryos control the timing of specific gene activation in early frog development. They find transcription factors for early gene activation are maternally loaded and remain at constant levels, and rather that order of activation is based on their sequential entry into the nucleus based largely on their respective affinity to importins.
- Thao Nguyen
- , Eli J. Costa
- & Martin Wühr
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Article
| Open AccessOrthogonally-tunable and ER-targeting fluorophores detect avian influenza virus early infection
Methods to detect and distinguish the early stage of viral infection often involve complicated and time-consuming protocols. Here, the authors disclose a class of fluorescent molecules that enable fast detection of avian influenza virus infection by selectively localizing at the endoplasmic reticulum in the cell.
- Taewon Kang
- , Md Mamunul Haque
- & Dongwhan Lee
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Article
| Open AccessChiral molecular imprinting-based SERS detection strategy for absolute enantiomeric discrimination
Absolute chiral discrimination in chiral imprinted systems is complicated by the nonspecific binding of enantiomers. Here, the authors report a SERS “inspector” recognition mechanism to distinguish between specifically and nonspecifically bound enantiomers, even in seawater and urine.
- Maryam Arabi
- , Abbas Ostovan
- & Lingxin Chen
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Article
| Open AccessReaction-based fluorogenic probes for detecting protein cysteine oxidation in living cells
Fluorogenic detection of H2O2 in cells is established, but equivalent tools to monitor its cellular targets remain in their infancy. Here authors develop fluorogenic probes for detecting cysteine sulfenic acid, a redox modification inextricably linked to H2O2 signalling and oxidative stress.
- Renan B. Ferreira
- , Ling Fu
- & Kate S. Carroll
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Matters Arising
| Open AccessPitfalls in the location of guest molecules in metal-organic frameworks
- Tomasz Poręba
- , Piero Macchi
- & Michelle Ernst
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Article
| Open AccessNeolithic culinary traditions revealed by cereal, milk and meat lipids in pottery from Scottish crannogs
Despite archaeobotanical evidence for domesticated cereals, organic residue evidence is scarce. Here, the authors identify cereal-specific markers in pottery from Scottish ‘crannogs’, revealing the presence of cereals in Neolithic pottery which might have been mixed with dairy products as a milk-based gruel.
- Simon Hammann
- , Rosie R. Bishop
- & Lucy J. E. Cramp
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Article
| Open AccessControllable synthesis of conjugated microporous polymer films for ultrasensitive detection of chemical warfare agents
The high toxicity of nerve agents makes the development of fluorescence sensors with suitable limit of detection challenging. Here, the authors propose a sensor design based on a conjugated microporous polymer film for the detection of diethyl chlorophosphate, a substitute of Sarin, with low detection limit of 2.5 ppt.
- Wanqi Mo
- , Zihao Zhu
- & Bin Li
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Article
| Open AccessComprehensive structural assignment of glycosaminoglycan oligo- and polysaccharides by protein nanopore
Glycosaminoglycans (GAGs) are highly anionic functional polysaccharides with subtle structural variations that are very difficult to differentiate. Here the authors demonstrate proof-of-concept single-molecule detection by nanopore, taking a first step towards the ultimate goal of GAG sequencing.
- Parisa Bayat
- , Charlotte Rambaud
- & Régis Daniel
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Article
| Open AccessMolecular identification and quantification of defect sites in metal-organic frameworks with NMR probe molecules
Defects in porous materials can alter the pore structure and chemical properties. Here authors demonstrate an approach for studying defects in metal-organic frameworks using 31P NMR and probe molecules.
- Jinglin Yin
- , Zhengzhong Kang
- & Xueqian Kong
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Article
| Open AccessOxidative decomposition mechanisms of lithium carbonate on carbon substrates in lithium battery chemistries
Lithium carbonate is ubiquitous in lithium battery chemistries and leads to overpotentials, however its oxidative decomposition is unclear. Here, the authors study its decomposition in ether electrolyte, clarify the role of the carbon substrate, and propose a route to limit released singlet oxygen.
- Deqing Cao
- , Chuan Tan
- & Yuhui Chen
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Article
| Open AccessUnderstanding the lithium–sulfur battery redox reactions via operando confocal Raman microscopy
The complex redox processes in lithium–sulfur batteries are not yet fully understood at the fundamental level. Here, the authors report operando confocal Raman microscopy measurements to provide mechanistic insights into polysulfide evolution and sulfur deposition during battery cycling.
- Shuangyan Lang
- , Seung-Ho Yu
- & Héctor D. Abruña
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Article
| Open AccessA mid-infrared lab-on-a-chip for dynamic reaction monitoring
Rapid investigation of chemical reactions is a challenge in bio-medical analysis. Here, the authors demonstrate sensitive in-situ real-time reaction-monitoring of conformational changes in protein solution, based on a fingertip-sized mid-IR lab-on-a-chip.
- Borislav Hinkov
- , Florian Pilat
- & Gottfried Strasser
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Article
| Open AccessA facile way to construct sensor array library via supramolecular chemistry for discriminating complex systems
The development of sensor unit libraries that require minimal synthetic effort is challenging. Here, the authors report the preparation of sensor array libraries based on a supramolecular approach that relies on the recognition and assembly of macrocyclic amphiphiles.
- Jia-Hong Tian
- , Xin-Yue Hu
- & Dong-Sheng Guo
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Article
| Open AccessAcceptor engineering for NIR-II dyes with high photochemical and biomedical performance
Small molecule NIR-II fluorophores are of interest for a range of applications but can suffer from chemical and photostability issues. Here, the authors report on the development of an acceptor molecule with improved stability in alkaline conditions expanding the range of possible applications.
- Aiyan Ji
- , Hongyue Lou
- & Zhen Cheng
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Article
| Open AccessBioorthogonally activatable cyanine dye with torsion-induced disaggregation for in vivo tumor imaging
Expanding the responsive dyes repertoire is currently a developing field in biorthogonal chemistry. In this article, the authors develop fluorophores that turn on their near-infrared fluorescence upon biorthogonal reaction based on a “torsion-induced disaggregation” approach, allowing for sensitive in vivo imaging of tumors.
- Xianghan Zhang
- , Jingkai Gao
- & Zhongliang Wang
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Article
| Open AccessDual-resolving of positional and geometric isomers of C=C bonds via bifunctional photocycloaddition-photoisomerization reaction system
The simultaneous identification of position and configuration of double bonds in unsaturated lipids is challenging. Here, the authors develop a workflow for deep structural lipidomics to address this issue using a bifunctional reaction system combined with liquid chromatography-mass spectrometry, revealing double bond patterns in bacteria and in mouse brain ischemia.
- Guifang Feng
- , Ming Gao
- & Suming Chen
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Article
| Open AccessNext-generation biomonitoring of the early-life chemical exposome in neonatal and infant development
Exposure to synthetic and natural toxicants is a major risk factor in the etiology of disease. Here, authors describe the development of a method to quantify >80 xenobiotics and apply it to assess early-life exposure in vulnerable infants.
- Thomas Jamnik
- , Mira Flasch
- & Benedikt Warth
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Article
| Open AccessWater coordinated on Cu(I)-based catalysts is the oxygen source in CO2 reduction to CO
Understanding the underlying mechanisms for catalytic reduction of CO2 over Cu based catalysts remains challenging. Here, the authors develop an effective method to reveal the vital roles of H2O in promoting metal catalysts to CO2 reduction via a modified triple stage quadrupole mass spectrometer.
- Yajun Zheng
- , Hedan Yao
- & Zhiping Zhang
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Article
| Open AccessA synergistic strategy to develop photostable and bright dyes with long Stokes shift for nanoscopy
Super-resolution microscopy is a powerful tool for cellular studies but requires bright and stable fluorescent probes. Here, the authors report on a strategy to introduce quinoxaline motifs to conventional probes to make them brighter, more photostable, larger Stokes shift, and demonstrate the probes for biosensing applications.
- Gangwei Jiang
- , Tian-Bing Ren
- & Lin Yuan
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Article
| Open AccessThree-dimensional structure determination of protein complexes using matrix-landing mass spectrometry
Mass spectrometry (MS) is a powerful tool for the structural characterization of protein complexes. Here the authors offer a path for direct integration of MS and electron microscopy with a MS approach that enables grid deposition and structural preservation of gaseous protein complex ions.
- Michael S. Westphall
- , Kenneth W. Lee
- & Joshua J. Coon
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Article
| Open AccessHost-guest liquid gating mechanism with specific recognition interface behavior for universal quantitative chemical detection
In field, visual, chemical detection is of use for a wide range of possible applications. Here, the authors report on the creation of a host-guest liquid gating mechanism where detection of the target host triggers gate opening allowing for gas through the liquid gate, which can be used for visual detection.
- Huimeng Wang
- , Yi Fan
- & Xu Hou
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Article
| Open AccessTemporal and spatial characterisation of protein liquid-liquid phase separation using NMR spectroscopy
Protein liquid-liquid phase separation is an important phenomenon in biology. Here, the authors demonstrate an approach to characterize the evolution of protein phases in both time and space using a fluorinated probe molecule in NMR spectroscopy.
- Jack E. Bramham
- & Alexander P. Golovanov
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Article
| Open AccessHyper-CEST NMR of metal organic polyhedral cages reveals hidden diastereomers with diverse guest exchange kinetics
Self-assembling nanostructures that trap guest molecules find applications in materials research and the life sciences. Here, authors describe how ultra-sensitive NMR reveals sub-types with broken symmetry that significantly impacts guest exchange.
- Jabadurai Jayapaul
- , Sanna Komulainen
- & Leif Schröder
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Article
| Open AccessProgrammable design of isothermal nucleic acid diagnostic assays through abstraction-based models
Detecting nucleic acids often requires choosing between different amplification mechanisms. Here the authors present a generalisable and programmable isothermal methodology, demonstrated in clinical applications, including for multiplexed detection of short miRNAs.
- Gaolian Xu
- , Julien Reboud
- & Jonathan M. Cooper
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Article
| Open AccessAtomic resolution dynamics of cohesive interactions in phase-separated Nup98 FG domains
The permeability barrier of nuclear pores is formed by disordered and yet self-interacting FG repeat domains, whose sequence heterogeneity is a challenge for mechanistic insights. Here the authors overcome this challenge and characterize the protein’s dynamics by applying NMR techniques to an FG phase system that has been simplified to its essentials.
- Eszter E. Najbauer
- , Sheung Chun Ng
- & Loren B. Andreas
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Article
| Open AccessExtra kinetic dimensions for label discrimination
Label discrimination is challenging in fluorescence microscopy due to broad spectra and narrow lifetime distribution. Here, the authors introduce extra kinetic dimensions by illuminating reversibly photoswitchable fluorophores with different intensities, and discriminate 20 spectrally similar fluorophores.
- Raja Chouket
- , Agnès Pellissier-Tanon
- & Ludovic Jullien
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Article
| Open AccessIdentification of plasmon-driven nanoparticle-coalescence-dominated growth of gold nanoplates through nanopore sensing
This study shows the light-driven morphology conversion from gold nanospheres to gold nanoplates through an aggregation-coalescence-dominated growth pathway, demonstrated by the nanopore sensing technique.
- Bintong Huang
- , Longfei Miao
- & Yueming Zhai