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| 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
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Article
| Open AccessDual-comb photothermal spectroscopy
'Recent developments in spectroscopy have witnessed the establishment of dual-comb techniques. In this work the authors demonstrate dual-comb photothermal spectroscopy providing gas sensing with superfine resolution and high sensitivity
- Qiang Wang
- , Zhen Wang
- & Wei Ren
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Article
| Open AccessRed edge effect and chromoselective photocatalysis with amorphous covalent triazine-based frameworks
Chromoselective catalysis offers an intriguing opportunity to enable a specific reaction pathway in photocatalysis. Here, the authors look into the ability of covalent triazine frameworks to enable the synthesis of different organic compounds by using safer red light instead of harsh UV light.
- Yajun Zou
- , Sara Abednatanzi
- & Aleksandr Savateev
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Article
| Open AccessIntracavity Raman scattering couples soliton molecules with terahertz phonons
Here, the authors demonstrate intra-cavity excitation and time-domain sampling of coherent optical phonons inside an active laser oscillator. They discover that Terahertz crystal vibrations link successive ultrashort solitons which offers an approach to highspeed Raman spectroscopy inside laser cavities.
- Alexandra Völkel
- , Luca Nimmesgern
- & Georg Herink
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Article
| Open AccessThe stability of covalent dative bond significantly increases with increasing solvent polarity
Non covalent complexes are often considerably destabilized in the solvent. Here the authors combine vibrational Raman and NMR spectroscopy with a coupled-cluster computational investigation to show that the solvent polarity enhance the complex stability of a Me3NBH3 complex.
- Rabindranath Lo
- , Debashree Manna
- & Pavel Hobza
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Article
| Open AccessUltraviolet optical horn antennas for label-free detection of single proteins
The authors introduce optical horn antennas, a nanophotonic platform combining plasmonic enhancement, efficient collection and background screening, for detection of UV autofluorescence from single proteins. They demonstrate label-free monitoring of protein unfolding and dissociation upon denaturation.
- Aleksandr Barulin
- , Prithu Roy
- & Jérôme Wenger
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Article
| Open AccessChemically identifying single adatoms with single-bond sensitivity during oxidation reactions of borophene
Here, the authors report the use of ultrahigh vacuum tip-enhanced Raman spectroscopy to characterize the oxidation processes of monolayer borophene with atomic-scale resolution and single-bond sensitivity, demonstrating the potential of the technique for probing the local chemistry of surface adsorbates on low-dimensional materials.
- Linfei Li
- , Jeremy F. Schultz
- & Nan Jiang
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Article
| Open AccessHollow-core optical fibre sensors for operando Raman spectroscopy investigation of Li-ion battery liquid electrolytes
New analytical tools are needed to identify chemical degradation and failure mechanisms in Li-ion batteries. Here, the authors report an operando Raman spectroscopy method, based on hollow-core optical fibres, that enables monitoring the chemistry of liquid electrolytes during battery cycling.
- Ermanno Miele
- , Wesley M. Dose
- & Tijmen G. Euser
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Article
| Open AccessRapid age-grading and species identification of natural mosquitoes for malaria surveillance
Knowing the age of malaria-transmitting mosquitoes is important to understand transmission risk as only old mosquitoes can transmit the disease. Here, the authors develop a method based on mid-infrared spectra of mosquito cuticle that can rapidly identify the species and age class of main malaria vectors.
- Doreen J. Siria
- , Roger Sanou
- & Francesco Baldini
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Article
| Open AccessTransient quantum beatings of trions in hybrid organic tri-iodine perovskite single crystal
Understanding photo-physics giving rise to quantum beating oscillations in hybrid organic-inorganic perovskites aids their applications in spintronics and quantum information science. Here, authors demonstrate that quantum beatings observed in single crystal perovskite at cryogenic temperatures are originating from positive and negative trions.
- Uyen N. Huynh
- , Ye Liu
- & Z. Valy Vardeny
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Article
| Open AccessExtracting quantitative dielectric properties from pump-probe spectroscopy
Photoinduced changes in transmission, reflection and scattering prevent conventional pump-probe spectroscopy to unambiguously assign the origin of spectral signatures. Ashoka et al. have developed an optical modelling technique to extract quantitative and unambiguous changes in the dielectric function from standard pump-probe measurements.
- Arjun Ashoka
- , Ronnie R. Tamming
- & Akshay Rao
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Article
| Open AccessMeasuring mechanical anisotropy of the cornea with Brillouin microscopy
Here, Brillouin optical microscopy noninvasively visualizes microscale anisotropy of the porcine cornea owing to its lamellar fiber structure and quantifies the longitudinal moduli of the bulk tissue. Anisotropy is also detected in angle-resolved measurement of the human cornea in vivo.
- Amira M. Eltony
- , Peng Shao
- & Seok-Hyun Yun
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Article
| Open AccessQuantum interference directed chiral raman scattering in two-dimensional enantiomers
Quantum interference among elementary Raman processes has only been observed in few materials under specific excitation configurations. Here, the authors show that quantum interference can lead to significant chiral Raman response in a monolayer material of transitional metal dichalcogenide with triclinic symmetry.
- Shishu Zhang
- , Jianqi Huang
- & Jin Zhang
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Article
| Open AccessUltrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
Ultrafast infrared nano-imaging has enabled the study of nanoscale dynamics, but has been limited to probing short-lived carrier lifetimes. Here, the authors present pump-probe nano-spectroscopy with enhanced sensitivity to image both carrier and vibrational dynamics associated with long-lived excitations.
- Jun Nishida
- , Samuel C. Johnson
- & Markus B. Raschke
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Article
| Open AccessMulti-parameter photon-by-photon hidden Markov modeling
In this work, the authors demonstrate the application of multi-parameter photon-by-photon hidden Markov modeling (mpH2MM) on alternating laser excitation (ALEX)-based smFRET measurements. The utility of mpH2MM in identifying and quantifying dynamic biomolecular sub-populations is demonstrated in three different systems.
- Paul David Harris
- , Alessandra Narducci
- & Eitan Lerner
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Article
| Open AccessSuperresolution concentration measurement realized by sub-shot-noise absorption spectroscopy
Here, the authors use entangled photon pairs as the light source for absorption spectroscopy and demonstrate sub-shot-noise spectra in the entire visible wavelength region. They quantify chemical species in highly diluted solutions with precision beyond the limit of conventional spectroscopy.
- Korenobu Matsuzaki
- & Tahei Tahara
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Article
| Open AccessOptical-domain spectral super-resolution via a quantum-memory-based time-frequency processor
Spectral super-resolution methods generally apply only to laser spectroscopy. Here, thanks to a Gradient Echo Memory with time-frequency processing capabilities, the authors are able to resolve frequency differences with precision below the Fourier limit for narrowband and ultra-low input-light level.
- Mateusz Mazelanik
- , Adam Leszczyński
- & Michał Parniak
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Article
| Open AccessCircularly polarised luminescence laser scanning confocal microscopy to study live cell chiral molecular interactions
Here, the authors introduce a live-cell imaging system using chiroptical contrast, enabling the study of chiral interactions. They demonstrate simultaneous imaging of enantiomeric pairs of molecular probes emitting circularly polarised light, using both single and two-photon excitation.
- Patrycja Stachelek
- , Lewis MacKenzie
- & Robert Pal
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Article
| Open AccessNano-spectroscopy of excitons in atomically thin transition metal dichalcogenides
Excitons play an important role in the optical properties of 2D semiconductors, but their spatial characterization is usually constrained by the diffraction limit. Here, the authors report near-field optical spectroscopy of 2D transition metal dichalcogenides with 20 nm resolution, revealing their spatially dependent excitonic spectra and complex dielectric function.
- Shuai Zhang
- , Baichang Li
- & D. N. Basov
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Article
| Open AccessAmino acid gas phase circular dichroism and implications for the origin of biomolecular asymmetry
Chiroptical properties of amino acids are challenging to investigate in the gas phase due to the low vapor pressure of these molecules. Here the authors succeed in measuring circular dichroism active transitions and anisotropies in the ultraviolet range for several gas-phase amino acids, shedding light on the interactions between molecules and circularly polarized light that lead to chiral symmetry breaking.
- Cornelia Meinert
- , Adrien D. Garcia
- & Uwe J. Meierhenrich
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Article
| Open AccessComparing ultrastable lasers at 7 × 10−17 fractional frequency instability through a 2220 km optical fibre network
Precision measurement plays an important role in frequency metrology and optical communications. Here the authors compare two geographically separate ultrastable lasers at 7 × 10−17 fractional frequency instability over a 2220 km optical fibre link and these measurements can be useful for dissemination of ultrastable light to distant optical clocks.
- M. Schioppo
- , J. Kronjäger
- & G. Grosche
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Article
| Open AccessMapping the broadband circular dichroism of copolymer films with supramolecular chirality in time and space
Time-resolved circular dichroism spectra can reveal changes in chirality on ultrashort time scales, but achieving sub-picosecond time resolution is still a challenge. Here the authors demonstrate 100-femtosecond time-resolved CD mapping of polyfluorene copolymer thin films, revealing a supramolecular origin of their chiroptical response.
- Marius Morgenroth
- , Mirko Scholz
- & Thomas Lenzer
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Article
| Open AccessTracking excited state decay mechanisms of pyrimidine nucleosides in real time
The photophysical mechanism by which nucleosides dissipate energy after UV light irradiation is still under debate. Here the authors, using ultrafast time resolved optical spectroscopies and quantum chemical computations, resolve the early steps of such mechanism in uridine and 5-methyluridine in aqueous solution.
- Rocío Borrego-Varillas
- , Artur Nenov
- & Giulio Cerullo
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Article
| Open AccessNanosecond-resolution photothermal dynamic imaging via MHZ digitization and match filtering
Photothermal microscopy is limited for imaging of thermal dynamics. Here, the authors introduce a lock-in free, mid-infrared photothermal dynamic imaging system, which significantly increases SNR and imaging speed, and demonstrate metabolism analysis at single-cell level and background removal.
- Jiaze Yin
- , Lu Lan
- & Ji-Xin Cheng
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Article
| Open AccessEngineering of a fluorescent chemogenetic reporter with tunable color for advanced live-cell imaging
Fluorescent reporters spanning the visible spectrum are needed for imaging live cells and organisms. Here the authors report a collection of fluorogenic chromophores that cover the visible spectrum from blue to red using a single engineered and optimised protein tag.
- Hela Benaissa
- , Karim Ounoughi
- & Arnaud Gautier
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Article
| Open AccessTwo-colour single-molecule photoinduced electron transfer fluorescence imaging microscopy of chaperone dynamics
Revealing mechanisms of complex protein machines requires simultaneous exploration of multiple structural coordinates. Here the authors report two-colour fluorescence microscopy combined with photoinduced electron transfer probes to simultaneously detect two structural coordinates in single protein molecules.
- Jonathan Schubert
- , Andrea Schulze
- & Hannes Neuweiler
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Article
| Open AccessUltra-rapid and highly efficient enrichment of organic pollutants via magnetic mesoporous nanosponge for ultrasensitive nanosensors
The authors demonstrate a sensing approach for effectively monitoring organic micropollutants in water. They first use mesoporous nanosponge and magnetic nanoparticles for fast enrichment of micropollutants, and demonstrate SERS-based sensing with 2-3 orders of magnitude improvement in detection limits.
- Lingling Zhang
- , Yu Guo
- & Jixiang Fang
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Article
| Open Access6 nm super-resolution optical transmission and scattering spectroscopic imaging of carbon nanotubes using a nanometer-scale white light source
The authors present a super-resolution hyperspectral imaging technique using a nanoscale white light source generated by superfocusing light from a tungsten-halogen lamp. They achieve 6 nm resolution, measuring longitudinal and transverse optical electronic transitions in single-walled carbon nanotubes.
- Xuezhi Ma
- , Qiushi Liu
- & Ming Liu
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Article
| Open AccessResolving sub-angstrom ambient motion through reconstruction from vibrational spectra
Tracking single molecule movements is a challenging task, but highly desired for applications and fundamental studies. Here the authors reconstruct the sub-angstrom relative movements of a molecule interacting with a metal adatom, by measuring its vibrational spectrum in a self-assembled monolayer, continuously modified by the adatom in a nanoparticle-on-mirror construct.
- Jack Griffiths
- , Tamás Földes
- & Jeremy J. Baumberg
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Article
| Open AccessStructures of prokaryotic ubiquitin-like protein Pup in complex with depupylase Dop reveal the mechanism of catalytic phosphate formation
Pupylation is a bacterial post-translational protein modification, where the small ubiquitin-like protein Pup is covalently attached to lysine side chains of target proteins, which is a reversible process and depupylation is catalysed by the depupylase enzyme, Dop. Here, the authors present crystal structures of Dop in different functional states, which together with biochemical experiments provide insights into the catalytic mechanism of this enzyme.
- Hengjun Cui
- , Andreas U. Müller
- & Eilika Weber-Ban
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Article
| Open AccessOptical deciphering of multinary chiral compound mixtures through organic reaction based chemometric chirality sensing
The stereoselective analysis of mixtures of chiral compounds typically requires time-consuming chromatography. Here, the authors combine reaction based chiroptical sensing and chemometric tools to directly determine the absolute configuration, enantiomeric composition and concentration of convoluted samples without physical separation.
- Diandra S. Hassan
- & Christian Wolf
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Article
| Open AccessTracking Brownian motion in three dimensions and characterization of individual nanoparticles using a fiber-based high-finesse microcavity
Tracking of nanoparticle dynamics in solution often require labelling. Here, the authors use a high-finesse microcavity and simultaneously measure dispersive frequency shifts of three transverse modes, demonstrating 3D tracking of unlabelled single nanospheres, and quantitatively determine their physical properties.
- Larissa Kohler
- , Matthias Mader
- & David Hunger
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Article
| Open AccessBiomimetic CO oxidation below −100 °C by a nitrate-containing metal-free microporous system
CO oxidation is of importance both for inorganic and living systems. Here the authors demonstrate that CO can be oxidized by nitrate in small-pore SSZ-13 zeolite at a temperature below −100 °C using spectroscopy and density functional theory calculations.
- Konstantin Khivantsev
- , Nicholas R. Jaegers
- & Janos Szanyi
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Article
| Open AccessIntrinsically disordered protein biosensor tracks the physical-chemical effects of osmotic stress on cells
Methods to monitor osmolarity-dependent changes in cell are currently lacking. Here the authors use the Arabidopsis intrinsically disordered AtLEA4-5 protein, which is expressed in plants under water deficit, to develop a FRET biosensor (SED1) to monitor osmotic stress.
- Cesar L. Cuevas-Velazquez
- , Tamara Vellosillo
- & José R. Dinneny
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Article
| Open AccessVacancy control in acene blends links exothermic singlet fission to coherence
A complete understanding of singlet fission (SF) in molecular materials will enable the design of optimised optoelectronic devices. Here, the authors use vacancy control in acene-based blends to link coherent and incoherent SF pathways to energetics.
- Clemens Zeiser
- , Chad Cruz
- & Katharina Broch
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Article
| Open AccessIntegration of FRET and sequencing to engineer kinase biosensors from mammalian cell libraries
Existing Förster Resonance Energy Transfer (FRET) biosensors are often limited in their sensitivity. Here the authors report FRET-seq which they use to identify Fyn and ZAP70 kinase biosensors with enhanced performance, and use them to image T-cell activation and screen drugs.
- Longwei Liu
- , Praopim Limsakul
- & Yingxiao Wang
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Article
| Open AccessNon-invasive hydrodynamic imaging in plant roots at cellular resolution
Existing methods for non-invasively monitoring water flow in plants have limited spatial/temporal resolution. Here, the authors report that Raman microspectroscopy, complemented by hydrodynamic modelling, can monitor hydrodynamics within living root tissues at cell- and sub-second-scale resolutions.
- Flavius C. Pascut
- , Valentin Couvreur
- & Kevin F. Webb
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Article
| Open AccessIn-situ nanospectroscopic imaging of plasmon-induced two-dimensional [4+4]-cycloaddition polymerization on Au(111)
Here, the authors use tip-enhanced Raman spectroscopy for in-situ investigation of plasmon-induced [4+4]-cycloaddition polymerization on Au(111). They find that this occurs by a hot electron tunneling mechanism, while crosslinks form via a self-stimulating growth mechanism.
- Feng Shao
- , Wei Wang
- & Renato Zenobi
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Article
| Open Access9-Cyanopyronin probe palette for super-multiplexed vibrational imaging
The authors develop a method to build Manhattan Raman Scattering (MARS) probes based on different core atoms, conjugation ring numbers, and stable isotope substitutions. A quantitative model predicts vibrational frequencies of MARS dyes from structures, which are used in supermultiplexed vibrational imaging.
- Yupeng Miao
- , Naixin Qian
- & Wei Min
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Article
| Open AccessAn on-demand, drop-on-drop method for studying enzyme catalysis by serial crystallography
Currently many of the time resolved serial femtosecond (SFX) crystallography experiments are done with light driven protein systems, whereas the reaction initiation for non-light triggered enzymes remains a major bottle neck. Here, the authors present an expanded Drop-on-Tape system, where picoliter-sized droplets of a substrate or inhibitor are turbulently mixed with nanoliter sized droplets of microcrystal slurries, and they use it for time-resolved SFX measurements of inhibitor binding to lysozyme and secondly, binding of a β-lactam antibiotic to a bacterial serine β-lactamase.
- Agata Butryn
- , Philipp S. Simon
- & Allen M. Orville
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Article
| Open AccessFrequency comb ptychoscopy
Frequency-comb-based multiheterodyne spectroscopy requires that total bandwidth of the measured spectrum covers less than half the comb spacing, which is usually not the case for incoherent spectra. Here, the authors propose a technique that lifts this requirement, and demonstrate it in the microwave regime.
- David J. Benirschke
- , Ningren Han
- & David Burghoff
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Article
| Open AccessLiquid flow reversibly creates a macroscopic surface charge gradient
Reactions at the interface between mineral surfaces and flowing liquids are ubiquitous in nature. Here the authors explore, using surface-specific sum frequency generation spectroscopy and numeric calculations, how the liquid flow affects the charging and dissolution rates leading to flow-dependent charge gradients along the surface.
- Patrick Ober
- , Willem Q. Boon
- & Mischa Bonn
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Article
| Open AccessManipulation of hot carrier cooling dynamics in two-dimensional Dion–Jacobson hybrid perovskites via Rashba band splitting
Hybrid perovskite is a promising class of material for optoelectronic applications due to the slow hot-carrier cooling, yet the process is not well-understood in material with Rashba band splitting. Here, the authors reveal spin-flipping and spin-dependent scattering of hot electrons are responsible for accelerating the cooling at longer delays.
- Jun Yin
- , Rounak Naphade
- & Omar F. Mohammed
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Matters Arising
| Open AccessReply to ‘Comment on “Coherent control in the extreme ultraviolet and attosecond regime by synchrotron radiation”’
- Y. Hikosaka
- , T. Kaneyasu
- & M. Katoh
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Matters Arising
| Open AccessOn “Coherent control in the extreme ultraviolet and attosecond regime by synchrotron radiation” by Hikosaka et al, Nat. Comm. 10, 4988 (2019)
- Kevin C. Prince
- & Bruno Diviacco