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| Open AccessOvertone photothermal microscopy for high-resolution and high-sensitivity vibrational imaging
The authors develop overtone photothermal microscopy that leverages a pump-probe detection of second overtone vibrations within the shortwave-infrared (SWIR) window. This technique complements existing large-scale SWIR imaging approaches, offering enhanced resolution and sensitivity for bioimaging applications.
- Le Wang
- , Haonan Lin
- & Ji-Xin Cheng
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Article
| Open AccessProbing the structure of water in individual living cells
Here the authors report a Raman scattering technique to measure vibrational spectrum of water inside living cells. A consistent population (~3%) of non-bulk-like water is seen, exhibiting a more disordered structure with a weakened hydrogen-bonded network.
- Xiaoqi Lang
- , Lixue Shi
- & Wei Min
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Article
| Open AccessBulk-suppressed and surface-sensitive Raman scattering by transferable plasmonic membranes with irregular slot-shaped nanopores
Characterizing surfaces by Raman spectroscopy is limited by the competition of surface and bulk Raman responses. Here the authors use nanoporous plasmonic membranes to enhance surface Raman signals while suppressing bulk contributions.
- Roman M. Wyss
- , Günter Kewes
- & Sebastian Heeg
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Article
| Open AccessBirefringence-induced phase delay enables Brillouin mechanical imaging in turbid media
Non-contact Brillouin microscopy holds potential to disrupt mechanobiology, yet this method faces challenges in presence of strong Rayleigh scattering. Here, the authors introduce a common-path birefringent filter exhibiting ultra-high extinction ratio to investigate turbid biological samples.
- Giuseppe Antonacci
- , Renzo Vanna
- & Giulio Cerullo
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Article
| Open AccessSub-100-fs energy transfer in coenzyme NADH is a coherent process assisted by a charge-transfer state
Excitation energy transfer is important for many photoinduced biological processes in systems with multiple chromophores. Here, the authors elucidate this process for the coenzyme NADH using ultrafast spectroscopy and quantum dynamics.
- Vishal Kumar Jaiswal
- , Daniel Aranda Ruiz
- & Artur Nenov
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Article
| Open AccessCollective chiroptical activity through the interplay of excitonic and charge-transfer effects in localized plasmonic fields
Chiral interaction of molecular ensembles with confined light fields is elusive. Here, the authors report collective chiroptical effects through coupling of exciton and charge-transfer mixed molecular assemblies with plasmonic nanoparticles.
- Huacheng Li
- , Xin Xu
- & Xiang Lan
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Article
| Open AccessIn-situ observation of silk nanofibril assembly via graphene plasmonic infrared sensor
Here, the authors develop a graphene plasmonic infrared sensor to probe the secondary structure of nanoscale assembly intermediates and the morphological evolution of silk nanofibrils, the fundamental building blocks of silk fibres.
- Chenchen Wu
- , Yu Duan
- & Qing Dai
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Article
| Open AccessOrganic and inorganic sublattice coupling in two-dimensional lead halide perovskites
By resonant pumping the organic cation in 2D perovskite, Fu et al. report the electronic and mechanical couplings between the organic and inorganic sublattices, evidenced by the reduced bandgap and modified lattice degree of freedom within the inorganic sublattice, and slow heat transfer process.
- Jianhui Fu
- , Tieyuan Bian
- & Tze Chien Sum
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Article
| Open AccessTime-resolved THz Stark spectroscopy of molecules in solution
Stark spectroscopy of molecules in liquid solutions was once challenging due to orientation effects, solved by freezing but limiting ambient studies. Now, THz Stark spectroscopy with intense terahertz pulses enables dynamic analysis of molecules in both non-polar and polar solvents at any temperature, advancing conventional methods.
- Bong Joo Kang
- , Egmont J. Rohwer
- & Thomas Feurer
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Article
| Open AccessGiant magneto-photoluminescence at ultralow field in organic microcrystal arrays for on-chip optical magnetometer
The optical detection of magnetic fields is difficult for low field strengths. Here, the authors show how strong magneto-photoluminescence can be achieved in rubrene microcrystals and demonstrate its application in a magnetometer.
- Hong Wang
- , Baipeng Yin
- & Chuang Zhang
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Article
| Open AccessCorrelating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging
Physicochemical heterogeneity poses a significant constraint in photocatalyst advancement. Here the authors introduce a multimodal optical microscopy platform to assess activity and defects concurrently in photoelectrocatalysts, revealing that disorder can unexpectedly enhance local photoelectrocatalytic performance in certain instances.
- Camilo A. Mesa
- , Michael Sachs
- & Raj Pandya
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Article
| Open AccessMiniature computational spectrometer with a plasmonic nanoparticles-in-cavity microfilter array
Conventional spectrometers can be bulky and efforts are being made to develop miniaturised versions. Here, the authors present a miniature computational spectrometer based on silver nanoparticles in Fabry-Pérot microcavities for measuring visible spectra.
- Yangxi Zhang
- , Sheng Zhang
- & A. Ping Zhang
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Matters Arising
| Open AccessOn the statistical foundation of a recent single molecule FRET benchmark
- Ayush Saurabh
- , Lance W. Q. Xu
- & Steve Pressé
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Matters Arising
| Open AccessReply to: On the statistical foundation of a recent single molecule FRET benchmark
- Markus Götz
- , Anders Barth
- & Sonja Schmid
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Article
| Open AccessRapid room-temperature phosphorescence chiral recognition of natural amino acids
Chiral recognition of amino acids with luminescence, despite its advantages, is usually slow and lacks generality. Here, the authors demonstrate that L-phenylalanine derived benzamide can manifest the structural difference between the natural, left-handed amino acid and its right-handed counterpart via the difference in room-temperature phosphorescence, irrespective of the specific chemical structure.
- Xiaoyu Chen
- , Renlong Zhu
- & Guoqing Zhang
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Article
| Open AccessSpiral packing and chiral selectivity in model membranes probed by phase-resolved sum-frequency generation microscopy
The properties of lipid membranes are intimately controlled by their complex heterogeneous structure. Here, the authors use phase-resolved sum-frequency generation microscopy to fully determine the hierarchical lipid packing from the molecular to the mesoscopic scale.
- Alexander P. Fellows
- , Ben John
- & Martin Thämer
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Article
| Open AccessA 2D chiral microcavity based on apparent circular dichroism
Here the authors induce asymmetric transmission in planar Fabry–Pérot microcavities by embedding organic thin films exhibiting apparent circular dichroism (ACD), an optical phenomenon based on 2D chirality.
- Tzu-Ling Chen
- , Andrew Salij
- & Randall H. Goldsmith
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Article
| Open AccessOptics miniaturization strategy for demanding Raman spectroscopy applications
Authors present a centimeter-scale miniaturized Raman spectrometer using cheap nonstabilized laser diodes, densely packed optics, and non-cooled small sensors while the performance is comparable with expensive bulky research-grade Raman systems.
- Oleksii Ilchenko
- , Yurii Pilhun
- & Anja Boisen
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Article
| Open AccessLarge exchange-driven intrinsic circular dichroism of a chiral 2D hybrid perovskite
Li et al. report large circular dichroism in 2D chiral perovskite single crystals, arises from the inorganic sublattice, instead of chiral ligands, driven by electron-hole exchange interactions. This is evidenced by both reflective circular dichroism spectroscopy and ab initio theory.
- Shunran Li
- , Xian Xu
- & Peijun Guo
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Article
| Open AccessPhotoswitchable polyynes for multiplexed stimulated Raman scattering microscopy with reversible light control
Bioimaging with photocontrol and multiplexing capability is vital for studying cellular interactions and dynamics, but multiplexed stimulated Raman scattering (SRS) imaging with reversible photocontrol is elusive. Here, the authors report SRS microscopy with Carbow-switch enabling multiplexed SRS imaging and tracking in live cells with reversible photocontrol and high spatiotemporal selectivity.
- Yueli Yang
- , Xueyang Bai
- & Fanghao Hu
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Article
| Open AccessAssessing intra- and inter-molecular charge transfer excitations in non-fullerene acceptors using electroabsorption spectroscopy
The performance of Y6-containing donor-acceptor active layers in organic solar cells is highly related to the charge-transfer nature in Y6 aggregates. Here, authors study charge-transfer characteristics of excitations of isolated and aggregated Y6 molecules through electroabsorption spectroscopy.
- Sudhi Mahadevan
- , Taili Liu
- & Sai-Wing Tsang
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Article
| Open AccessMonolithic thin-film lithium niobate broadband spectrometer with one nanometre resolution
A framework to break the inherent trade-off barrier between spectral resolution and operational bandwidth of integrated optical spectrometers is developed and demonstrated on thin-film lithium niobate without sacrificing the compact footprint.
- Giovanni Finco
- , Gaoyuan Li
- & Rachel Grange
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Article
| Open AccessTime-of-flight detection of terahertz phonon-polariton
Polaritons, light-matter hybridized quasiparticles, are the fundamental excitation of strong coupling systems and are widely applicable in information technologies. Here the authors applied the concept of time-of-flight measurement in terahertz induced second harmonic generation experiments in various systems to comprehensively study the dispersion relation of phonon-polaritons and reveal potential spin-lattice couplings.
- Tianchuang Luo
- , Batyr Ilyas
- & Nuh Gedik
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Article
| Open AccessMolecular near-infrared triplet-triplet annihilation upconversion with eigen oxygen immunity
Molecular triplet-triplet upconversion is useful in a wide range of applications, but is limited by significant oxygen quenching. Here the authors report the combination of sensitiser and annihilator that is stable in aerated environments, and suitable for in vivo sensing.
- Xinyu Wang
- , Fangwei Ding
- & Guanying Chen
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Article
| Open AccessIn situ electrochemical regeneration of nanogap hotspots for continuously reusable ultrathin SERS sensors
SERS is a powerful analytical technique, but achieving reproducibility for continuous analysis a challenge. Here, the authors report a SERS substrate recycling method that enables direct analysis of complex samples without substrate contamination.
- Sarah May Sibug-Torres
- , David-Benjamin Grys
- & Jeremy J. Baumberg
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Article
| Open AccessExtensive photochemical restructuring of molecule-metal surfaces under room light
The nature of the molecule-metal interface is crucial for many technological applications. Here, the authors show that the photostability of the material can be sensitive to room light when coated with a single molecular layer, with implications for devices and processes.
- Chenyang Guo
- , Philip Benzie
- & Jeremy J. Baumberg
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Article
| Open AccessProbing molecules in gas cells of subwavelength thickness with high frequency resolution
Using gas cells for spectroscopic studies opens possibility for miniaturized platforms that can be integrated with other optical components. Here the authors demonstrate molecular rovibrational spectroscopy by confining molecules in a cell of subwavelength thickness.
- Guadalupe Garcia Arellano
- , Joao Carlos de Aquino Carvalho
- & Athanasios Laliotis
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Article
| Open AccessSingle-pixel p-graded-n junction spectrometers
The miniaturization of spectrometers to a submillimeter-scale footprint opens opportunities for applications in hyperspectral imaging and lab-on-a-chip systems. Here, the authors report a high-performance single-pixel photodetector spectrometer based on the III-V semiconductor p-graded-n junction, featuring a voltage-tunable optical response.
- Jingyi Wang
- , Beibei Pan
- & Baile Chen
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Article
| Open AccessMeasuring sub-nanometer undulations at microsecond temporal resolution with metal- and graphene-induced energy transfer spectroscopy
Studying the fluctuations of biological membranes with high resolution is challenging. Here, the authors combine metal- and graphene-induced energy transfer (MIET/GIET) with fluorescence correlation spectroscopy (FCS) to monitor such fluctuations with nanometer and microsecond resolution.
- Tao Chen
- , Narain Karedla
- & Jörg Enderlein
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Article
| Open AccessTransient chemical and structural changes in graphene oxide during ripening
Graphene oxide is in demand for various applications - however, this is complicated by changing physicochemical properties over time. Here, the authors show the intrinsic, metastable, and transient states of graphene oxide colloids upon ripening.
- Hayato Otsuka
- , Koki Urita
- & Katsumi Kaneko
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Article
| Open AccessA compressive hyperspectral video imaging system using a single-pixel detector
The authors showcase a video-rate hyperspectral imager based on a single-pixel photodetector that can achieve high-throughput hyperspectral video recording at a low bandwidth. Specifically, they propose a joint spatial-spectral encoding scheme which can encode the scene into highly compressed single-pixel measurements and obtain temporal correlation at the same time.
- Yibo Xu
- , Liyang Lu
- & Kevin F. Kelly
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Article
| Open AccessIntrinsic dichroism in amorphous and crystalline solids with helical light
Differential absorption of polarized light, called dichroism, does not exist in amorphous solids due to the disordered arrangements of atoms. Here, the authors demonstrate that dichroism is intrinsic to all solids and can be controlled using helical light beams carrying orbital angular momentum.
- Ashish Jain
- , Jean-Luc Bégin
- & Ravi Bhardwaj
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Article
| Open AccessUnified picture of vibrational relaxation of OH stretch at the air/water interface
Using femtosecond time-resolved heterodyne-detected vibrational sum-frequency generation spectroscopy the authors determine the vibrational relaxation (T1) time of the O-H stretch at the air/water interface by observing the decay of excited-state OH signals, providing a comprehensive picture of the interfacial vibrational relaxation process of water.
- Woongmo Sung
- , Ken-ichi Inoue
- & Tahei Tahara
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Article
| Open AccessVisualization-enhanced under-oil open microfluidic system for in situ characterization of multi-phase chemical reactions
Under-oil open microfluidic systems have potential for studying multi-phase chemical reactions but have so far demonstrated largely only for biological applications. Here, the authors report the development of a system for in situ characterization of gas-liquid reactions by Raman spectroscopy.
- Qiyuan Chen
- , Hang Zhai
- & Bu Wang
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Article
| Open AccessRatiometric fluorescent sensing of pyrophosphate with sp³-functionalized single-walled carbon nanotubes
Inorganic pyrophosphate is a key molecule in many biological processes. Here, the authors develop an optical sensor that enables its ratiometric detection in the near infrared with functionalized single-walled carbon nanotubes.
- Simon Settele
- , C. Alexander Schrage
- & Jana Zaumseil
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Article
| Open AccessFolding pathway of a discontinuous two-domain protein
Here, using single molecule FRET, the unfolding and folding of a discontinuous two-domain protein was studied. The authors find that a dynamic, intermediate population entropically limits the rate of folding while the order of domain folding is kept in a slow-folding mutant.
- Ganesh Agam
- , Anders Barth
- & Don C. Lamb
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Article
| Open AccessCochaperones convey the energy of ATP hydrolysis for directional action of Hsp90
The precise role of cochaperones and ATP hydrolysis in driving Hsp90’s chaperone cycle is largely unclear. Here, the authors use single-molecule FRET to show that several cochaperones are necessary to establish directionality in Hsp90’s conformational cycle.
- Leonie Vollmar
- , Julia Schimpf
- & Thorsten Hugel
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Article
| Open AccessScalable integrated two-dimensional Fourier-transform spectrometry
The authors propose and demonstrate a novel integrated spectrometer that measures any arbitrary spectrum with two-dimensional Fourier transform, breaking the scalability limit in chip-scale spectrometry.
- Hongnan Xu
- , Yue Qin
- & Hon Ki Tsang
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Article
| Open AccessTheory predicts 2D chiral polaritons based on achiral Fabry–Pérot cavities using apparent circular dichroism
2D chiral polaritons are light-matter states with select angular momentum holding technological promise. Here, the authors present the theory of such states, and propose their realisation based on a phenomenon called “apparent circular dichroism”.
- Andrew H. Salij
- , Randall H. Goldsmith
- & Roel Tempelaar
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Article
| Open AccessDual-wavelength metalens enables Epi-fluorescence detection from single molecules
The requirement for sophisticated objective lenses hinders the miniaturisation of single molecule fluorescence spectroscopy for portable sensing applications. Here, the authors demonstrate a dual-wavelength metalens for real-time monitoring of individual fluorescent nanoparticles.
- Aleksandr Barulin
- , Yeseul Kim
- & Inki Kim
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Article
| Open AccessSub-Doppler optical-optical double-resonance spectroscopy using a cavity-enhanced frequency comb probe
Probing molecules in excited vibrational states requires precise methods to extract the spectroscopic parameters. Here the authors demonstrate optical-optical double-resonance spectroscopy of excited-bands of methane using single pass high power continuous wave pump and cavity-enhanced frequency comb probe.
- Vinicius Silva de Oliveira
- , Isak Silander
- & Aleksandra Foltynowicz
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Comment
| Open AccessExcitonic Complexes in Two-Dimensional Transition Metal Dichalcogenides
The enhanced Coulomb interaction in two dimensions leads to not only tightly bound excitons but also many-particle excitonic complexes: excitons interacting with other quasiparticles, which results in improved and even new exciton properties with better controls. Here, we summarize studies of excitonic complexes in monolayer transition metal dichalcogenides and their moiré heterojunctions, envisioning how to utilize them for exploring quantum many-body physics.
- Xiaotong Chen
- , Zhen Lian
- & Su-Fei Shi
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Article
| Open AccessHot luminescence from single-molecule chromophores electrically and mechanically self-decoupled by tripodal scaffolds
A fundamental challenge for molecular electronics is the change in photophysical properties of molecules upon direct electrical contact. Here, the authors observe hot luminescence emitted by single-molecule chromophores that are electrically and mechanically self-decoupled by a tripodal scaffold.
- Vibhuti Rai
- , Nico Balzer
- & Michal Valášek
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Article
| Open AccessMid-infrared supermirrors with finesse exceeding 400 000
The researchers showcase all-crystalline and hybrid mid-infrared supermirrors with the lowest optical losses ever demonstrated in this wavelength range, representing an unprecedented improvement over any existing mirrors made with any production technology.
- Gar-Wing Truong
- , Lukas W. Perner
- & Garrett D. Cole
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Article
| Open AccessOperando dynamics of trapped carriers in perovskite solar cells observed via infrared optical activation spectroscopy
Conventional spectroscopic techniques are not sufficiently selective to follow the dynamics of trapped carriers in working perovskite solar cells. Here, authors use infrared optical activation spectroscopy to observe real time evolution of trapped carriers and compare the behaviour of trapped holes.
- Jiaxin Pan
- , Ziming Chen
- & Artem A. Bakulin
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Article
| Open AccessSharp zero-phonon lines of single organic molecules on a hexagonal boron-nitride surface
Low-temperature spectroscopy of single fluorescent molecules can be of use to study dynamics in the nano-environment around them. Here, Smit et al. show that the fluorescence wavelength of molecules on the surface of hexagonal boron-nitride is particularly sensitive to how clean this surface is.
- Robert Smit
- , Arash Tebyani
- & Michel Orrit
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Article
| Open AccessDynamic construction of refractive index-dependent vibrations using surface plasmon-phonon polaritons
Molecular vibrations serve as valuable signatures for the constituent elements and bonding in compounds. Here, using Surface-Enhanced Infrared Absorption spectroscopy, the authors study refractive index dependent vibrations of surface phonon polaritons and surface plasmon platform, targeting dynamic biomonitoring.
- Hong Zhou
- , Zhihao Ren
- & Chengkuo Lee
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Article
| Open AccessTime-domain observation of interlayer exciton formation and thermalization in a MoSe2/WSe2 heterostructure
Here, the authors use ultrafast transient absorption spectroscopy with a broadband white-light probe to simultaneously resolve interlayer charge transfer and interlayer exciton formation dynamics in a MoSe2/WSe2 heterostructure.
- Veronica R. Policht
- , Henry Mittenzwey
- & Stefano Dal Conte
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Article
| Open AccessAccessible hotspots for single-protein SERS in DNA-origami assembled gold nanorod dimers with tip-to-tip alignment
The identification of individual proteins is highly desirable in diagnostics. Here, the authors report on DNA-origami assembled dimers of gold nanorod with accessible hotspots to capture and identify single proteins from solution by SERS.
- Francis Schuknecht
- , Karol Kołątaj
- & Theobald Lohmueller