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| Open AccessA chip-scale atomic beam clock
Compact atomic clocks and atom interferometers are desired for on-chip integration. Here the authors demonstrate a chip-scale atomic beam of 87Rb atoms and its application as an atomic beam clock
- Gabriela D. Martinez
- , Chao Li
- & William R. McGehee
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Article
| Open AccessUncovering the chiral bias of meteoritic isovaline through asymmetric photochemistry
Excess of l-amino acids in meteorites suggests an extraterrestrial origin of biomolecular homochirality, which may stem from chiral light-matter interactions. Here the authors support this hypothesis with asymmetric photolysis experiments on racemic isovaline films, showing that circularly polarized starlight can produce l-enantiomeric excesses that can be amplified during parent bodies’ alteration.
- Jana Bocková
- , Nykola C. Jones
- & Cornelia Meinert
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| Open AccessCoherent Stokes Raman scattering microscopy (CSRS)
Coherent Stokes Raman scattering (CSRS) has never been explored previously for chemical imaging due to a strong fluorescence background. Here, the authors demonstrate the first fluorescence-free CSRS laser scanning microscope and predict CSRS’ unique backscattering properties.
- Sandro Heuke
- & Hervé Rigneault
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| Open AccessGiant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering
Extreme confinement of light in plasmonic nanocavities strongly enhances the optomechanical coupling of light with molecular vibrations. Here, the authors use a giant optical spring effect to reversibly weaken molecular bonds.
- Lukas A. Jakob
- , William M. Deacon
- & Jeremy J. Baumberg
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| Open AccessMeasurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid
Spontaneous Raman scattering is classically understood as an incoherent process. Here, the authors demonstrate that macroscopic quantum coherence among billions of vibrating molecules in a liquid is generated when single photon detection and single spatio-temporal mode excitation are implemented.
- Valeria Vento
- , Santiago Tarrago Velez
- & Christophe Galland
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Article
| Open AccessIn-plane and out-of-plane excitonic coupling in 2D molecular crystals
The mixing between Frenkel and charge-transfer characters in molecular excitons is difficult to analyze. Here, the authors demonstrate the onset and evolution of the mixing using 2D perylene molecular crystals by measuring the reorientation of emission transition dipoles with varying thicknesses.
- Dogyeong Kim
- , Sol Lee
- & Sunmin Ryu
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Article
| Open AccessMany-body screening effects in liquid water
Electron screening is crucial to interpret inelastic X-ray scattering experiments in materials. Here the authors use a combined analysis based on the Bethe-Salpeter equation and time-dependent density functional theory to calculate the dielectric function and obtain the band gap of liquid water.
- Igor Reshetnyak
- , Arnaud Lorin
- & Alfredo Pasquarello
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| Open AccessUltrafast charge transfer in mixed-dimensional WO3-x nanowire/WSe2 heterostructures for attomolar-level molecular sensing
2D materials are promising substrates for surface-enhanced Raman scattering (SERS)-based molecular sensing, but their performance is usually inferior to their plasmonic counterparts. Here, the authors report the synthesis of 1D/2D WO3-x/WSe2 heterostructures, showing high molecular sensitivity associated to ultrafast charge transfer timescales of ~1 ps.
- Qian Lv
- , Junyang Tan
- & Ruitao Lv
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Article
| Open AccessSingle-pulse terahertz spectroscopy monitoring sub-millisecond time dynamics at a rate of 50 kHz
Single-pulse THz spectroscopy at 50 kHz is performed with a table-top system to extract rapid changes of a material’s complex dielectric function. This technique is demonstrated by monitoring carrier accumulation and relaxation dynamics in silicon.
- Nicolas Couture
- , Wei Cui
- & Jean-Michel Ménard
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Article
| Open AccessTriboelectric-induced ion mobility for artificial intelligence-enhanced mid-infrared gas spectroscopy
Isopropyl alcohol can play a significant role in anti-virus diagnosis but generally yields limited response in conventional detection. Here, authors propose a methodology of AI-enhanced ion mobility and mid-infrared spectroscopy for accurate gas identification despite presence different carbon-based gases.
- Jianxiong Zhu
- , Shanling Ji
- & Chengkuo Lee
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Article
| Open AccessSpectroscopic visualization and phase manipulation of chiral charge density waves in 1T-TaS2
Two-dimensional charge density waves in layered semiconductors may exhibit chirality. Here, the authors utilize thermal annealing to reversibly switch the in-plane chirality of charge density waves in 1T-TaS2 and demonstrate a vertical chirality-locking effect between the van der Waals-stacked layers.
- Yan Zhao
- , Zhengwei Nie
- & Jin Zhang
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Article
| Open AccessAll-optical control of high-purity trions in nanoscale waveguide
The authors induce a nanoscale strain gradient in monolayer MoS2 suspended on a waveguide and take advantage of propagating surface plasmon polaritons to localize hot electrons in the suspended area. They funnel excitons in the waveguide, facilitating all-optical control of exciton-to-trion conversion.
- Hyeongwoo Lee
- , Yeonjeong Koo
- & Kyoung-Duck Park
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Article
| Open AccessDeducing subnanometer cluster size and shape distributions of heterogeneous supported catalysts
IR spectra are great for characterizing single-crystals and large nanoparticles, but not for highly dispersed heterogeneous catalysts made up of single-atoms and ultra-small clusters. To solve this, the authors developed a method to generate synthetic IR spectra using data-based approaches and physics-driven surrogate models.
- Vinson Liao
- , Maximilian Cohen
- & Dionisios G. Vlachos
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Article
| Open AccessTwo-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality
Direct spectroscopic probes of the impact of structure on dynamical processes in liquids remain scarce. Here, the authors use molecular dynamics simulations to show that the correlation between vibrational coupling and the local tetrahedral structure of liquid water can be studied via hybrid terahertz- and infrared-Raman spectroscopy.
- Tomislav Begušić
- & Geoffrey A. Blake
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Article
| Open AccessImaging-based intelligent spectrometer on a plasmonic rainbow chip
The authors develop an imaging-based intelligent spectrometer on a plasmonic “rainbow” chip. It can accurately and precisely determine the spectroscopic and polarimetric information of the illumination spectrum using a single image assisted by suitably trained deep learning algorithms.
- Dylan Tua
- , Ruiying Liu
- & Qiaoqiang Gan
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Article
| Open AccessRapid handheld time-resolved circularly polarised luminescence photography camera for life and material sciences
Despite their high brightness and long-lived emission, lanthanide based circularly polarised luminophores have not been fully exploited for real-life application. Here, the authors present an all solid-state circularly polarised luminescence camera to facilitate ad hoc time-resolved enantioselective differential chiral contrast-based one-shot photography that can be applied in life and material sciences.
- Davide F. De Rosa
- , Patrycja Stachelek
- & Robert Pal
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Article
| Open AccessObservation of Chiral-selective room-temperature phosphorescence enhancement via chirality-dependent energy transfer
Despite increasing interest in organic room temperature phosphorescence, it can still be challenging to determine mechanism and develop practical applications. Here, the authors report room temperature phosphorescent systems from chiral components, with strong phosphorescence observed only when both host and guest had the same chirality.
- Biao Chen
- , Wenhuan Huang
- & Guoqing Zhang
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Article
| Open AccessReal-time single-molecule 3D tracking in E. coli based on cross-entropy minimization
Single-molecule 3D tracking is critical to understand macromolecular dynamics but achieving this at a sub-millisecond resolution remains challenging. Here the authors present a 3D tracking method based on cross-entropy minimization and the true excitation point spread function.
- Elias Amselem
- , Bo Broadwater
- & Johan Elf
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Article
| Open AccessVibrational signature of hydrated protons confined in MXene interlayers
Intercalation of protons in 2D materials plays a major role for several applications in energy storage and conversion. Here, the authors show that protons intercalated in Ti3C2Tx MXene interlayer during electrochemical cycling have a different hydration structure than protons in bulk water.
- Mailis Lounasvuori
- , Yangyunli Sun
- & Tristan Petit
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| Open AccessTheoretical and experimental analysis of circularly polarized luminescence spectrophotometers for artifact-free measurements using a single CCD camera
The authors present an artifact-free circularly polarized luminescence spectrophotometer using a single camera and two polarization encoding paths. The spectra are measured in a few seconds without the need of calibration by inverting the role of the paths.
- Bruno Baguenard
- , Amina Bensalah-Ledoux
- & Stéphan Guy
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| Open AccessMid-infrared cross-comb spectroscopy
The authors introduce and demonstrate cross-comb spectroscopy in the mid-infrared as a variant of dual-comb spectroscopy. It provides enhanced performance and allows mid-infrared spectral information to be obtained by near-infrared detection.
- Mingchen Liu
- , Robert M. Gray
- & Alireza Marandi
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Article
| Open AccessPhonon-driven intra-exciton Rabi oscillations in CsPbBr3 halide perovskites
Coupling electromagnetic radiation with matter is promising to tailor optoelectronics properties of functional materials. Here, the authors demonstrate that internal fields induced by coherent lattice motions can be used to control transient excitonic optical response in halide perovskite crystals.
- Xuan Trung Nguyen
- , Katrin Winte
- & Antonietta De Sio
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| Open AccessDual-comb optical activity spectroscopy for the analysis of vibrational optical activity induced by external magnetic field
Dual-comb spectroscopy was first applied to the measurement of magnetic optical activity spectroscopy, realizing Doppler-limited gas-phase molecular analysis, and was further extended to the rapid measurement of liquid-phase chiroptical activity.
- Daowang Peng
- , Chenglin Gu
- & Wenxue Li
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Article
| Open AccessIn vivo detection of bile duct pre-cancer with endoscopic light scattering spectroscopy
Diagnosis of bile duct cancer often occur in advanced stages, leading to poor survival. Here, the authors combine light scattering and diffuse reflectance spectroscopies in a minimally invasive endoscopic technique for directly assessing the malignant potential of the bile duct lining, and demonstrate 97% detection accuracy.
- Douglas K. Pleskow
- , Mandeep S. Sawhney
- & Lev T. Perelman
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Article
| Open AccessQuantum interference between dark-excitons and zone-edged acoustic phonons in few-layer WS2
Here, the authors investigate the Raman spectra of few-layered WS2 when the excitation energy is in resonance with the dark exciton, and observe a Fano resonance between dark excitonsand zone-edge acoustic phonons.
- Qing-Hai Tan
- , Yun-Mei Li
- & Jun Zhang
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Article
| Open AccessRapid, label-free histopathological diagnosis of liver cancer based on Raman spectroscopy and deep learning
Biopsy is recommended for definitive diagnosis of liver carcinoma, however, this process requires staining and expert pathologists to confirm diagnosis. Here, the authors employ a portable Raman spectroscopy system combined with deep learning to detect carcinoma from normal tissue in real time.
- Liping Huang
- , Hongwei Sun
- & Yi Wang
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Article
| Open AccessMolecular polariton electroabsorption
The authors investigate whether strong light-matter coupling can alter the nonlinear optical response of molecules inside a microcavity. Focusing on electroabsorption as a model third order nonlinearity, they find that apparent discrepancies between experiment and classical transfer matrix modeling arise from dark states in the system and are not a sign of new physics in the strong coupling regime.
- Chiao-Yu Cheng
- , Nina Krainova
- & Noel C. Giebink
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Article
| Open AccessLossless enrichment of trace analytes in levitating droplets for multiphase and multiplex detection
Efficient enrichment of molecules from liquids, solid objects, or the gas phase is critical for their detection at trace concentrations. Here, the authors report on the lossless enrichment of analytes in droplets using acoustic levitation for multiphase and multiplex SERS detection.
- Xueyan Chen
- , Qianqian Ding
- & Shikuan Yang
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Article
| Open AccessBond-selective intensity diffraction tomography
The authors introduce Bond-selective Intensity Diffraction Tomography, a computational mid-infrared photothermal microscopy technique based on a standard bright-field microscope and an add-on pulsed light source. It recovers both mid-infrared spectra and bond-selective 3D refractive index maps based on intensity-only measurements.
- Jian Zhao
- , Alex Matlock
- & Ji-Xin Cheng
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| Open AccessAbsolute excited state molecular geometries revealed by resonance Raman signals
Physical or chemical reactions driven by light absorption are ruled by excited-state multidimensional energy surfaces displaced with respect to the ground state. Here the authors introduce a nonlinear Raman experiment to access an elusive aspect of the excited-state displacements: their sensed directions relative to the ground-state.
- Giovanni Batignani
- , Emanuele Mai
- & Tullio Scopigno
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| Open AccessRemote near-field spectroscopy of vibrational strong coupling between organic molecules and phononic nanoresonators
Vibrational strong coupling (VSC) promises ultrasensitive IR spectroscopy and modification of material properties. Here, nanoscale mapping of VSC between organic molecules and individual IR nanoresonators is achieved by remote near-field spectroscopy.
- Irene Dolado
- , Carlos Maciel-Escudero
- & Rainer Hillenbrand
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Article
| Open AccessNanoscale heterogeneity of ultrafast many-body carrier dynamics in triple cation perovskites
The optoelectronic performance of lead halide perovskite in highfluence applications are hindered by heterogeneous multi-polaron interactions in the nanoscale. Here, Nishda et al. spatially resolve sub-ns relaxation dynamics on the nanometer scale by ultrafast infrared pumpprobe nanoimaging.
- Jun Nishida
- , Peter T. S. Chang
- & Markus B. Raschke
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Article
| Open AccessProbing the ultrafast dynamics of excitons in single semiconducting carbon nanotubes
Excitonic states govern the optical response of low-dimensional nanomaterials and are key for a wide range of applications. Here, the authors investigate the exciton decay dynamics in single carbon nanotubes with few-exciton detection sensitivity.
- Konrad Birkmeier
- , Tobias Hertel
- & Achim Hartschuh
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Article
| Open AccessThe coupling of the hydrated proton to its first solvation shell
The Zundel [H(H2O)2]+ and Eigen [H(H2O)4]+ cations exhibit radicallly different infrared spectra and are the limiting dynamical structures involved in proton mobility in liquid water. Here, the authors find through quantum dynamics simulations that two polarized water molecules and a proton suffice to explain the key spectroscopic features connected to proton mobility for both species.
- Markus Schröder
- , Fabien Gatti
- & Oriol Vendrell
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| Open AccessDirect observation of ultrafast singlet exciton fission in three dimensions
Here, the authors use quantitative ultrafast interferometric pump-probe microscopy to track photoexcitations with sub-10 nm spatial precision in three dimensions and 15 fs temporal resolution to study the spatiotemporal dynamics of singlet exciton fission in polycrystalline pentacene films.
- Arjun Ashoka
- , Nicolas Gauriot
- & Akshay Rao
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Article
| Open AccessSub-optical-cycle light-matter energy transfer in molecular vibrational spectroscopy
Energy transfer between the electromagnetic field and atoms or molecules is fundamentally interesting. Here the authors demonstrate stepwise energy transfer between broadband mid-infrared optical pulses and vibrating methylsulfonylmethane molecules in aqueous solution.
- Martin T. Peschel
- , Maximilian Högner
- & Ioachim Pupeza
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| Open AccessInsight into the transient inactivation effect on Au/TiO2 catalyst by in-situ DRIFT and UV–vis spectroscopy
A molecular-level understanding of the Au-catalyzed CO oxidation on a fast time-resolved scale is still lacking. Here the authors monitor the rapid dynamic changes during CO oxidation over Au/TiO2 using in situ DRIFTS and UV-Vis spectroscopy, and reveal that the catalyst undergoes a surprising structural change at the beginning of the reaction.
- Xianwei Wang
- , Arnulf Rosspeintner
- & Thomas Bürgi
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Article
| Open AccessA blind benchmark of analysis tools to infer kinetic rate constants from single-molecule FRET trajectories
The ability to infer quantitative kinetic information from single-molecule FRET (smFRET) data can be challenging. Here the authors perform a blind benchmark study assessing different analysis tools used to infer kinetic rate constants from smFRET trajectories, testing on simulated and experimental data.
- Markus Götz
- , Anders Barth
- & Sonja Schmid
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Article
| Open AccessElectron-phonon coupling and vibrational properties of size-selected linear carbon chains by resonance Raman scattering
H-capped polyynes are the simplest system to observe finite-length effects in carbyne. Here, the authors exploit synchrotron-based UV resonance Raman spectroscopy to explain a peculiar intensity behavior of multiple phonons scattering and show a size-dependent electron-phonon coupling.
- P. Marabotti
- , M. Tommasini
- & C. S. Casari
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Article
| Open AccessSub-10-fs observation of bound exciton formation in organic optoelectronic devices
Ultrafast action spectroscopies of organic optoelectronic devices reveal that the formation of bound exciton state occurs as fast as 10 fs. Excitons having excess energy can dissociate spontaneously within 50-fs before acquiring bound character.
- Marios Maimaris
- , Allan J. Pettipher
- & Artem A. Bakulin
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Article
| Open AccessCoherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3
CrI3 is a van der Waals material which exhibits magnetic ordering down to the monolayer limit. Here, using ultrafast optical spectroscopy, Padmanabhan and Buessen et al. investigate the coupling between the magnetically ordered spins and lattice distortions, finding a coherent spin-coupled phonon mode.
- P. Padmanabhan
- , F. L. Buessen
- & R. P. Prasankumar
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Article
| Open AccessSingle-droplet surface-enhanced Raman scattering decodes the molecular determinants of liquid-liquid phase separation
The authors introduce a unique single-droplet surface-enhanced Raman scattering (SERS) methodology that illuminates a wealth of molecular information within the mesoscopic liquid condensed phase of Fused in Sarcoma in the absence and presence of RNA.
- Anamika Avni
- , Ashish Joshi
- & Samrat Mukhopadhyay
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Article
| Open AccessSpectral signatures of excess-proton waiting and transfer-path dynamics in aqueous hydrochloric acid solutions
The spectroscopic signatures of excess protons in HCl solutions are studied by ab initio simulations and THz experiments. Two contributions beyond the normal-mode scenario are identified that reflect proton-waiting and proton-transfer processes.
- Florian N. Brünig
- , Manuel Rammler
- & Roland R. Netz
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Article
| Open AccessConformational heterogeneity of molecules physisorbed on a gold surface at room temperature
Tip-enhanced vibrational spectroscopy at room temperature is complicated by molecular conformational dynamics, photobleaching, contaminations, and chemical reactions in air. This study demonstrates that a sub-nm protective layer of Al2O3 provides robust conditions for probing single-molecule conformations.
- Mingu Kang
- , Hyunwoo Kim
- & Kyoung-Duck Park
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Article
| Open AccessWavelength-multiplexed hook nanoantennas for machine learning enabled mid-infrared spectroscopy
Infrared spectroscopy with plasmonic nanoantennas is limited by small overlap between molecules and hot spots, and sharp resonance peaks. The authors demonstrate spectral multiplexing of hook nanoantennas with gradient dimensions as ultrasensitive vibrational probes in a continuous ultra-broadband region and utilize machine learning for enhanced sensing performance.
- Zhihao Ren
- , Zixuan Zhang
- & Chengkuo Lee
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Article
| Open AccessFree charge photogeneration in a single component high photovoltaic efficiency organic semiconductor
When light hits organic semiconductors, bound charge pairs, called excitons, are usually produced. Here, the authors show that in the best performing organic solar material to date, free charges, rather than excitons, are directly created by light.
- Michael B. Price
- , Paul A. Hume
- & Justin M. Hodgkiss
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Article
| Open AccessDual-comb thin-disk oscillator
Achieving high output powers in dual-comb sources is important for possible applications like deep UV high resolution spectroscopy. Here the authors demonstrate a fully passive scheme of generating a set of high-power dual-combs from a thin-disc gain medium.
- Kilian Fritsch
- , Tobias Hofer
- & Oleg Pronin
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Article
| Open AccessMagnons and magnetic fluctuations in atomically thin MnBi2Te4
MnBi2Te4, referred to as MBT, is a van der Waals material combining topological electron bands with magnetic order. Here, Lujan et al study collective spin excitations in MBT, and show that magnetic fluctuations increase as samples reduce in thickness, implying less robust magnetic order.
- David Lujan
- , Jeongheon Choe
- & Xiaoqin Li
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Article
| Open AccessRatiometric afterglow luminescent nanoplatform enables reliable quantification and molecular imaging
Afterglow luminescence is promising for non-background molecular imaging in vivo. Here the authors report a ratiometric afterglow luminescent nanoplatform to generate activatable afterglow probes for quantification of specific analytes including NO.
- Yongchao Liu
- , Lili Teng
- & Weihong Tan