Featured
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| Open AccessNanopore blockade sensors for ultrasensitive detection of proteins in complex biological samples
Nanopore sensors have long analysis times when analytes are at low concentration and non-specific signals in complex media. Here the authors use antibody-modified magnetic nanoparticles to detect prostate-specific antigen at sub-femtomolar concentrations in blood.
- Kyloon Chuah
- , Yanfang Wu
- & J. Justin Gooding
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Article
| Open AccessA generic approach towards afterglow luminescent nanoparticles for ultrasensitive in vivo imaging
Afterglow luminescence is used to reduce background noise and increase sensitivity; however, biocompatible afterglow materials are limited. Here, the authors report on an approach to turn standard optical agents into afterglow nanoparticles and demonstrate the application in tumour imagining in vivo.
- Yuyan Jiang
- , Jiaguo Huang
- & Kanyi Pu
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Article
| Open AccessSmall molecule electro-optical binding assay using nanopores
Nanopore detection of small molecules can be improved using molecular carriers, but separating a small analyte from the carrier signal can be challenging. Here the authors address this challenge using simultaneous electrical and optical readout in nanopore sensing to detect small molecules and quantify binding affinities.
- Shenglin Cai
- , Jasmine Y. Y. Sze
- & Joshua B. Edel
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Article
| Open AccessMicrofluidic multipoles theory and applications
Microfluidic multipoles use arrays of sources and sinks to confine fluids and reagents without the use of physical channels. Here the authors use conformal mappings to predict both convective and diffusive transport in these flows and 3D print multipoles to automate surface-based immunoassays.
- Pierre-Alexandre Goyette
- , Étienne Boulais
- & Thomas Gervais
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Article
| Open AccessScalable dissolution-dynamic nuclear polarization with rapid transfer of a polarized solid
Dissolution-dynamic nuclear polarization is able to enhance nuclear magnetic resonance signals, but requires complex procedures to generate hyperpolarized nuclear spins. Here the authors establish a fast and facile method to transfer hyperpolarized samples into the liquid solution where the measurement is performed.
- Karel Kouřil
- , Hana Kouřilová
- & Benno Meier
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Matters Arising
| Open Access1H NMR is not a proof of hydrogen bonds in transition metal complexes
- J. Vícha
- , C. Foroutan-Nejad
- & M. Straka
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Article
| Open AccessIn-situ electron microscopy mapping of an order-disorder transition in a superionic conductor
Solid-solid phase transitions are processes ripe for the discovery of correlated atomic motion in crystals. Here, the authors monitor an order-disorder transition in real-time in a single nanoparticle of the super-ionic solid, cuprous selenide, using in-situ high-resolution transmission electron microscopy.
- Jaeyoung Heo
- , Daniel Dumett Torres
- & Prashant K. Jain
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Review Article
| Open AccessLigand design strategies to increase stability of gadolinium-based magnetic resonance imaging contrast agents
Gadolinium(III) complexes are strong enhancers of magnetic resonance imaging (MRI) signals, thus are widely used as contrast agents despite their potential toxicity. Here, the authors review ligand design approaches aimed at improving the stability of Gd(III)-based MRI contrast agents.
- Thomas J. Clough
- , Lijun Jiang
- & Nicholas J. Long
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Article
| Open AccessControl of capillary behavior through target-responsive hydrogel permeability alteration for sensitive visual quantitative detection
DNA hydrogels have received considerable attention in analytical science but limitations still exist in the applications of intelligent hydrogels. Here, the authors describe a DNA hydrogel sensor for quantitative detection of cocaine based on the permeability change in a DNA hydrogel film.
- Yansheng Li
- , Yanli Ma
- & Yongqiang Wen
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Article
| Open AccessTime-space-resolved origami hierarchical electronics for ultrasensitive detection of physical and chemical stimuli
Developing portable, disposable and cost-effective electronics for multifunctional sensing is desirable. Here, the authors present origami-based hierarchical electronics with time-space-resolved high-discriminative pattern recognition (TSR-HDPR) features for multifunctional detection of complex physical and chemical stimuli.
- Min Zhang
- , Jiaxing Jeccy Sun
- & Hossam Haick
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Article
| Open AccessAnti-quenching NIR-II molecular fluorophores for in vivo high-contrast imaging and pH sensing
Fluorophores operating in the second near-infrared window suffer from solvatochromism-caused fluorescence quenching in biological aqueous solution. Here, the authors synthesized a series of pH-responsive pentamethine cyanine fluorophores that afford stable absorption/emission beyond 1000 nm.
- Shangfeng Wang
- , Yong Fan
- & Fan Zhang
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Article
| Open AccessRapid one-step 18F-radiolabeling of biomolecules in aqueous media by organophosphine fluoride acceptors
The synthesis of 18F-labeled positron emission tomography (PET) tracers is difficult and typically requires anhydrous conditions. Here, the authors developed organophosphine precursors that allow for quick, high-yield synthesis of 18F-labeled probes in either organic solvents or aqueous media.
- Huawei Hong
- , Lei Zhang
- & Zijing Li
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Article
| Open AccessIon mobility conformational lipid atlas for high confidence lipidomics
The biological functions of lipids critically depend on their highly diverse molecular structures. Here, the authors determine the mass-resolved collision cross sections of 456 sphingolipid and glycerophospholipid species, providing a reference for future structural lipidomics studies.
- Katrina L. Leaptrot
- , Jody C. May
- & John A. McLean
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Article
| Open AccessDesign strategy for serine hydroxymethyltransferase probes based on retro-aldol-type reaction
The enzyme serine hydroxymethyltransferase (SHMT) has been implicated in several diseases, however is hard to investigate. Here, the authors used a design strategy based on the retro-aldol-type reaction catalyzed by SHMT to develop SHMT-responsive fluorescence and 19F NMR molecular probes.
- Hiroshi Nonaka
- , Yuki Nakanishi
- & Shinsuke Sando
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Article
| Open AccessAmine-responsive cellulose-based ratiometric fluorescent materials for real-time and visual detection of shrimp and crab freshness
Simple, fast, and accurate detection of food freshness has great significance to food safety and business. Here, the authors develop cellulose-based ratiometric fluorescent materials with superior amine-response, which can be used for visual monitoring the freshness of shrimp and crab.
- Ruonan Jia
- , Weiguo Tian
- & Jun Zhang
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Article
| Open AccessElectrochromic semiconductors as colorimetric SERS substrates with high reproducibility and renewability
Electrochromic technology has diverse cutting-edge applications, but it has never been used to overcome the critical problems in the field of surface-enhanced Raman scattering (SERS). Here, the authors demonstrate a generic electrochromic strategy for ensuring the reproducibility and renewability of SERS substrates.
- Shan Cong
- , Zhen Wang
- & Zhigang Zhao
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Article
| Open AccessBisnorgammacerane traces predatory pressure and the persistent rise of algal ecosystems after Snowball Earth
It remains unclear when and why the world’s oceans, once largely occupied by bacteria, became dominated by photosynthetic algae. Here, using fossil lipids in million year old rocks, the authors show that predation after the Snowball Earth glaciations created the opportunity for a global shift to algal ecosystems.
- Lennart M. van Maldegem
- , Pierre Sansjofre
- & Christian Hallmann
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Article
| Open AccessUnveiling coherently driven hyperpolarization dynamics in signal amplification by reversible exchange
There is increasing effort to improve the signal sensitivity and explore the hyperpolarization dynamics. Here the authors demonstrate the parahydrogen spin transfer dynamics in compounds containing 15N using SABRE hyperpolarization technique with different strengths of the magnetic field.
- Jacob R. Lindale
- , Shannon L. Eriksson
- & Warren S. Warren
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Article
| Open AccessShifts in the selectivity filter dynamics cause modal gating in K+ channels
Spontaneous activity shifts at constant experimental conditions are widespread among ion channels but the molecular origins are poorly understood. Here, using solid-state NMR and MD simulations, the authors reveal that modal gating shifts in K + channels are caused by large shifts in the channel dynamics which perturb the selectivity filter.
- Shehrazade Jekhmane
- , João Medeiros-Silva
- & Markus Weingarth
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Article
| Open AccessUltrasensitive detection of miRNA with an antimonene-based surface plasmon resonance sensor
Label-free molecular-level quantification of MicroRNA (miRNA) remains challenging. Here, the authors develop a new surface plasmon resonance sensor based on two-dimensional nanomaterial of antimonene for the specific label-free detection of clinically relevant biomarkers such as miRNA-21 and miRNA-155.
- Tianyu Xue
- , Weiyuan Liang
- & Qiaoliang Bao
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Article
| Open AccessDeoxyribose and deoxysugar derivatives from photoprocessed astrophysical ice analogues and comparison to meteorites
Sugars are known to form from the UV photoprocessing of ices under astrophysical conditions. Here, the authors report the detection of deoxyribose, the sugar of DNA, and other deoxysugars from the UV photoprocessing of H2O:CH3OH ice mixtures, which are compared with materials from carbonaceous meteorites.
- Michel Nuevo
- , George Cooper
- & Scott A. Sandford
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Article
| Open AccessClick chemistry enables quantitative chiroptical sensing of chiral compounds in protic media and complex mixtures
Chiroptical sensing in complex mixtures remains a challenging task. Here, the authors report an efficient coumarin probe for chiroptical click chirality sensing of absolute configuration, concentration and enantiomeric excess of several compound classes. The method can be directly applied to crude asymmetric reaction mixtures.
- F. Yushra Thanzeel
- , Kaluvu Balaraman
- & Christian Wolf
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Article
| Open AccessMonitoring drug nanocarriers in human blood by near-infrared fluorescence correlation spectroscopy
While nanocarrier-based drug delivery is a promising therapeutic approach, in situ characterization of drug nanocarriers in blood remains difficult. Here, the authors demonstrate how the fluorescence correlation spectroscopy can be used to directly characterize drug nanocarriers in flowing blood.
- Inka Negwer
- , Andreas Best
- & Kaloian Koynov
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Article
| Open AccessReal-time determination of enantiomeric and isomeric content using photoelectron elliptical dichroism
The analysis of chiral chemical mixtures is crucial for many applications. Here, the authors perform real-time analysis of samples by ionizing them with elliptically polarized femtosecond laser pulses and detecting the angular distributions of the photoelectrons.
- A. Comby
- , E. Bloch
- & Y. Mairesse
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Article
| Open AccessDetermining molecular properties with differential mobility spectrometry and machine learning
The fast and accurate determination of molecular properties is particularly crucial in drug discovery. Here, the authors employ supervised machine learning to treat differential mobility spectrometry – mass spectrometry data for ten classes of drug candidates and predict several condensed-phase properties.
- Stephen W. C. Walker
- , Ahdia Anwar
- & W. Scott Hopkins
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Article
| Open AccessThree-dimensional localization spectroscopy of individual nuclear spins with sub-Angstrom resolution
Electron spins in nitrogen vacancy centres are perturbed by nearby nuclear spins, making it possible to infer some of the nuclear spins' properties. Here the authors demonstrate a technique that can determine the location of nuclear spins in three-dimensional space using only one electron spin.
- J. Zopes
- , K. S. Cujia
- & C. L. Degen
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Article
| Open AccessDirect oxygen isotope effect identifies the rate-determining step of electrocatalytic OER at an oxidic surface
Understanding reaction mechanisms is crucial for catalyst design. Here, natural-abundance isotope quantifications of O2 yield mechanistically significant reaction kinetic isotope effects for water oxidation over metal oxide electrodes, the bottleneck step of water electrolysis.
- Sandra Haschke
- , Michael Mader
- & Julien Bachmann
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Article
| Open AccessDistinct functional elements for outer-surface anti-interference and inner-wall ion gating of nanochannels
Nanochannels are often modified with functional elements, but most studies have focused on functionalizing only the inner wall. Here, the authors design nanochannels with distinct chemical modifications on the inner and outer surfaces, providing a route to dual-function channels.
- Pengcheng Gao
- , Qun Ma
- & Fan Xia
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Article
| Open AccessMass spectrometry and Monte Carlo method mapping of nanoparticle ligand shell morphology
Determining the arrangement of ligands on a nanoparticle is challenging, given the limitations of existing characterization tools. Here, the authors describe an accessible method for resolving ligand shell morphology that uses simple MALDI-TOF mass spectrometry measurements in conjunction with an open-access Monte Carlo fitting program.
- Zhi Luo
- , Yanfei Zhao
- & Francesco Stellacci
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Article
| Open AccessFine-tuning the efficiency of para-hydrogen-induced hyperpolarization by rational N-heterocyclic carbene design
Hyperpolarization methods play a crucial role in the in vivo observation of molecular metabolism by MRI techniques. Here, the authors develop NHC-containing iridium complexes which improve the NMR detectability of 1H, 13C and 15N nuclei via transfer of latent magnetism of para-hydrogen into a substrate.
- Peter J. Rayner
- , Philip Norcott
- & Simon B. Duckett
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Article
| Open AccessUnravelling the structure of glycosyl cations via cold-ion infrared spectroscopy
Glycosyl cations are key intermediates in glycosylation reactions, but their structure has remained elusive due to their transient nature. Here, the authors perform an in-depth structural analysis and report that C2-participating protective groups induce acetoxonium cations with distinct ring conformations.
- Eike Mucha
- , Mateusz Marianski
- & Kevin Pagel
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Article
| Open AccessHighly-sensitive optical organic vapor sensor through polymeric swelling induced variation of fluorescent intensity
Traditional optical organic vapor sensors with solvatochromic shift mechanisms have lower sensitivity due to weak intermolecular interactions. Here, the authors report a general strategy to prepare a higher sensitivity optical organic vapor sensor through polymeric swelling-induced variation of fluorescent intensity.
- Xiangyu Jiang
- , Hanfei Gao
- & Lei Jiang
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Article
| Open AccessManipulating and visualizing the dynamic aggregation-induced emission within a confined quartz nanopore
The difficulty in recovering the aggregation-induced emission fluorogens (AIEgens) to the initial dispersed state upon illuminating has limited their applications. Here, the authors employ the confined space in the quartz nanopore to achieve a nanopore-size dependent restriction of AIEgens.
- Yi-Lun Ying
- , Yuan-Jie Li
- & He Tian
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Article
| Open AccessLiquid-state quantitative SERS analyzer on self-ordered metal liquid-like plasmonic arrays
The design and application of a liquid interfacial plasmonic platform promises for practical applications of surface-enhanced Raman scattering (SERS). Here, the authors report a reversible chloroform/water encasing strategy to self-assemble metal liquid-like 3D gold nanorod arrays with attractive SERS capability.
- Li Tian
- , Mengke Su
- & Weihong Tan
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Article
| Open AccessTropical peatland carbon storage linked to global latitudinal trends in peat recalcitrance
Large peatlands exist at high latitudes because flooded conditions and cold temperatures slow decomposition, so the presence of (sub)tropical peat is enigmatic. Here the authors show that low-latitude peat is preserved due to lower carbohydrate and greater aromatic content resulting in chemical recalcitrance.
- Suzanne B. Hodgkins
- , Curtis J. Richardson
- & Jeffrey P. Chanton
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Article
| Open AccessLayer specific observation of slow thermal equilibration in ultrathin metallic nanostructures by femtosecond X-ray diffraction
Heat transport in ultrathin metal layers is important for potential applications in optical‐magnetic switching, but difficult to access experimentally. Here, the authors use ultrafast X‐ray diffraction to directly probe and explain unexpected time‐dependent transport behavior in Au–Ni nanolayers.
- J. Pudell
- , A. A. Maznev
- & M. Bargheer
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Article
| Open AccessSurveying silicon nitride nanopores for glycomics and heparin quality assurance
The complexity of polysaccharides significantly complicates their analysis in comparison to other biopolymers. Here, the authors demonstrate that solid-state silicon nitride nanopore sensors can be used to reliably detect native polysaccharides and to perform a simple quality assurance assay on a polysaccharide therapeutic, heparin.
- Buddini Iroshika Karawdeniya
- , Y. M. Nuwan D. Y. Bandara
- & Jason R. Dwyer
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Article
| Open AccessSingle-particle mass spectrometry with arrays of frequency-addressed nanomechanical resonators
Nano-electro-mechanical system-based mass spectrometry holds promise for detecting supramolecular assemblies at large molecular weights, but its efficiency is too poor to be practical. Sage et al. overcome this problem using a nanomechanical resonator array, which significantly decreases detection time.
- Eric Sage
- , Marc Sansa
- & Sébastien Hentz
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Article
| Open AccessSingle-molecule detection with a millimetre-sized transistor
The sensing capability of nanometric transducers designed for label-free single molecule detection has been limited by the small number of recognition elements. Here, the authors demonstrate a millimetre-sized field effect transistor capable of selective single-molecule Immunoglobulin-G detection.
- Eleonora Macchia
- , Kyriaki Manoli
- & Luisa Torsi
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Article
| Open AccessContinuous biomarker monitoring by particle mobility sensing with single molecule resolution
Biomarkers are natural indicators of some biological conditions, often used in diagnostics. Here, the authors developed a biosensor that continuously measures concentrations of DNA or protein biomarkers, and is based on particles that change mobility by directly interacting with individual molecules.
- Emiel W. A. Visser
- , Junhong Yan
- & Menno W. J. Prins
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Article
| Open AccessSimultaneous and stoichiometric purification of hundreds of oligonucleotides
Chemically synthesized DNA oligonucleotides (oligos) require purification to remove truncated species. Here, the authors developed a high-throughput method for oligo purification that also normalises the concentrations of the oligos in the final samples.
- Alessandro Pinto
- , Sherry X. Chen
- & David Yu Zhang
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Article
| Open AccessTomographic and multimodal scattering-type scanning near-field optical microscopy with peak force tapping mode
Scanning near-field optical microscopy (SNOM) offers nanometer-scale spatial resolution, but generally does not retain tomographic information. Here, Wang et al. develop peak-force SNOM to section scattered fields and improve imaging resolution.
- Haomin Wang
- , Le Wang
- & Xiaoji G. Xu
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Article
| Open AccessLight-induced formation of partially reduced oxygen species limits the lifetime of photosystem 1-based biocathodes
Photobiodevices use photosynthetic proteins such as those of the photosystem 1 (PS1) to enable light-induced charge separation, but they suffer from limited long-term stability. Here authors employ scanning photoelectrochemical microscopy on a PS1 biocathode and find that several pathways generate oxygen radicals.
- Fangyuan Zhao
- , Steffen Hardt
- & Felipe Conzuelo
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Article
| Open AccessA multistage rotational speed changing molecular rotor regulated by pH and metal cations
Molecular rotors with rotational speed modulation have not yet been well established. Here, the authors report a pH and metal cation triggered molecular rotor, which allows for a four stage speed modulation in the slow-to-fast frequency range.
- Yingying Wu
- , Guangxia Wang
- & Ying Wang
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Article
| Open AccessSelf-organizing layers from complex molecular anions
Using ions of one polarity to form functional layers on surfaces is usually challenging because of counter ions which are inevitably present in the condensed phase. Here the authors demonstrate accumulation of mass-selected anions and neutral molecules from the gas phase to form a self-organizing liquid-like layer on a surface.
- Jonas Warneke
- , Martin E. McBriarty
- & Julia Laskin
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Article
| Open AccessRechargeable lithium-ion cell state of charge and defect detection by in-situ inside-out magnetic resonance imaging
The development of noninvasive methodology plays an important role in advancing lithium ion battery technology. Here the authors utilize the measurement of tiny magnetic field changes within a cell to assess the lithiation state of the active material, and detect defects.
- Andrew J. Ilott
- , Mohaddese Mohammadi
- & Alexej Jerschow
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Article
| Open AccessNon-contact identification and differentiation of illicit drugs using fluorescent films
Sensitive and rapid identification of illicit drugs in a non-contact mode remains a challenge. Here, the authors report three film-based fluorescent sensors showing remarkable sensitivity, selectivity and response speed to six widely abused illicit drugs in vapor phase.
- Ke Liu
- , Congdi Shang
- & Yu Fang
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Article
| Open AccessThe influence of the molecular packing on the room temperature phosphorescence of purely organic luminogens
Organic luminogens with persistent room temperature phosphorescence will find wide applications in optoelectronic devices and bioimaging, but they are still scarce. Here, the authors synthesize seven organic luminogens and investigate their different properties and potential imaging applications.
- Jie Yang
- , Xu Zhen
- & Zhen Li
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Article
| Open AccessUltrasensitive reversible chromophore reaction of BODIPY functions as high ratio double turn on probe
BODIPY dyes, though widely explored, have not been pursued as chromophore reaction based chemical probes. Here, the authors synthesize a meso-naked BODIPY core flanked with two electron-withdrawing groups, which undergoes a reversible change in conjugated structure in the presence of base and functions as a dual signal and ultrahigh turn-on ratio chemical probe.
- Dehui Hu
- , Tao Zhang
- & Guoqiang Yang