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| Open AccessProbing femtosecond lattice displacement upon photo-carrier generation in lead halide perovskite
The electron–phonon coupling is the key to understand optoelectronic properties in lead halide perovskites but it is difficult to probe. Here Batignani et al. observe two new phonon modes with impulsive vibrational spectroscopy providing the evidence of the polaronic nature of the photo-excitation.
- Giovanni Batignani
- , Giuseppe Fumero
- & Tullio Scopigno
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Article
| Open AccessSilicon-chip-based mid-infrared dual-comb spectroscopy
Dual-comb spectroscopy is a powerful tool for realizing rapid spectroscopic measurements with high sensitivity and selectivity. Here, Yu et al. demonstrate silicon microresonator-based dual comb spectroscopy in the mid-infrared region, where strong vibrational resonances of many liquids exist.
- Mengjie Yu
- , Yoshitomo Okawachi
- & Alexander L. Gaeta
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Article
| Open AccessDetermination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
The determination of thermal and non-thermal carrier populations in plasmonic systems generally requires assumptions on the types of distributions present. Here, Heilpern et al. directly determine such populations in thin film pump-probe measurements using a double inversion procedure.
- Tal Heilpern
- , Manoj Manjare
- & Hayk Harutyunyan
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Article
| Open AccessHigh spatial resolution nanoslit SERS for single-molecule nucleobase sensing
Direct and real-time identification of nucleobases in DNA strands is still limited by the sensitivity and spatial resolution of the established solid-state nanopore devices. Here, the authors use CMOS compatible, plasmonic nanoslits to locally enable SERS for identifying nucleobases, both individual and incorporated in DNA strands.
- Chang Chen
- , Yi Li
- & Pol Van Dorpe
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Article
| Open AccessEffect of interstitial palladium on plasmon-driven charge transfer in nanoparticle dimers
Plasmon coupling between nanoparticles may depend not only on interparticle gap distance, but also on gap conductance. Here, the authors modify the gap conductance—and thus the plasmon response—between gold nanoparticle dimers by growing varying amounts of palladium nanoparticles in the gap.
- Sarah Lerch
- & Björn M. Reinhard
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Article
| Open AccessGeneration and characterization of ultrathin free-flowing liquid sheets
X-ray spectroscopy is a tool used for the investigation of aqueous solutions but the strong absorption of water means that very thin liquid sheets are needed for accurate analysis. Here the authors produce free-flowing liquid sheets 2 orders of magnitude thinner than sheets obtained with existing techniques.
- Jake D. Koralek
- , Jongjin B. Kim
- & Daniel P. DePonte
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Article
| Open AccessExperimentally quantifying anion polarizability at the air/water interface
Understanding anion-specific interactions with hydrophobic interfaces is challenging due to an absence of local structural probes. Here, the authors experimentally quantify the anisotropy of perchlorate’s polarizability at the air/water interface, a window into anion and solvation shell structure.
- Yujin Tong
- , Igor Ying Zhang
- & R. Kramer Campen
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Article
| Open AccessDual-comb spectroscopy of laser-induced plasmas
Dual-comb spectroscopy has become a valuable tool for broadband high-resolution measurements. Here Bergevin et al. apply this technique to a laser-induced plasma detecting different species in a solid sample with a spectral resolution sufficient to resolve hyperfine splitting of the Rb D2 line.
- Jenna Bergevin
- , Tsung-Han Wu
- & R. Jason Jones
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Article
| Open AccessOxygen radical character in group 11 oxygen fluorides
While transition metal complexes bearing terminal oxido ligands are common, those of group 11 elements have yet to be experimentally observed. Here, Riedel and colleagues synthesise molecular oxygen fluorides of copper, silver and gold, and show that the oxo ligands possess radical character.
- Lin Li
- , Tony Stüker
- & Sebastian Riedel
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Article
| Open AccessElectron heating and thermal relaxation of gold nanorods revealed by two-dimensional electronic spectroscopy
Electron dynamics in plasmonic nanoparticles are often studied with transient absorption spectroscopy. Here, Lietard et al. apply two-dimensional electronic spectroscopy, a method generally used for molecular spectroscopy, to study ultrafast nonlinear dynamics of electrons in excited gold nanorods.
- Aude Lietard
- , Cho-Shuen Hsieh
- & Minhaeng Cho
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Article
| Open AccessCoupling between intra- and intermolecular motions in liquid water revealed by two-dimensional terahertz-infrared-visible spectroscopy
Liquid water molecules are in constant vibrational motion, but probing how their local behaviour influences collective dynamics remains a challenge. Here, the authors present terahertz-infrared spectroscopy to elucidate coupling of the O-H stretch vibration to collective, delocalized intermolecular modes.
- Maksim Grechko
- , Taisuke Hasegawa
- & Mischa Bonn
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Article
| Open AccessUltrafast quantum control of ionization dynamics in krypton
Photoionization of atoms and molecules is a complex process and requires sensitive probes to explore the ultrafast dynamics. Here the authors combine transient absorption and photo-ion spectroscopy methods to explore and control the attosecond pulse initiated excitation, ionization and Auger decay in Kr atoms.
- Konrad Hütten
- , Michael Mittermair
- & Birgitta Bernhardt
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Article
| Open AccessResonance Raman signature of intertube excitons in compositionally-defined carbon nanotube bundles
Bundles of single-wall carbon nanotubes with enriched chirality can be used as model systems for exploring exciton physics in low-dimensional nanostructures. Here, the authors use resonant Raman spectroscopy to probe intertube interactions in bundles of (6,5)-enriched carbon nanotubes, and observe a Fano resonance arising from coupling between intertube and intratube excitons.
- Jeffrey R. Simpson
- , Oleksiy Roslyak
- & Stephen K. Doorn
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Article
| Open AccessGeneralized Fano lineshapes reveal exceptional points in photonic molecules
Fano lineshapes are found in many photonic systems where discrete and extended spectra interfere. Here, the authors extend this description and introduce generalized Fano lineshapes to describe the results from hyperspectral mapping around an exceptional point in a coupled-cavity system.
- Niccolò Caselli
- , Francesca Intonti
- & Massimo Gurioli
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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
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Article
| Open AccessOrientation of non-spherical protonated water clusters revealed by infrared absorption dichroism
Protein-bound water clusters play a key role for proton transport and storage in molecular biology. Here, the authors show by simulations and experiments that the orientation of non-spherical protonated water clusters in bacteriorhodopsin is unveiled by polarization-resolved infrared spectroscopy.
- Jan O. Daldrop
- , Mattia Saita
- & Roland R. Netz
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Article
| Open AccessEngineering the vibrational coherence of vision into a synthetic molecular device
The ultrafast, vibrationally coherent photoisomerization of rhodopsin is a model of efficient photomechanical energy conversion at the molecular scale. Here, the authors demonstrate a similar photoreaction in synthetic compounds, unraveling the underlying mechanism and discussing its implications.
- Moussa Gueye
- , Madushanka Manathunga
- & Jérémie Léonard
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Article
| Open AccessRaman spectroscopy of graphene under ultrafast laser excitation
Non-equilibrium ultrafast processes in graphene entail relaxation pathways involving electron–electron and electron–phonon scattering events. Here, the authors probe graphene optical phonons at high electronic temperatures by means of Raman spectroscopy under pulsed excitation
- C. Ferrante
- , A. Virga
- & T. Scopigno
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Article
| Open AccessOrder enables efficient electron-hole separation at an organic heterojunction with a small energy loss
Achieving charge separation in low energy loss organic heterojunctions is crucial to the efficiency of donor-acceptor solar cells, whilst the timescale of the process remains largely unknown. Here, Menke et al. observe slow charge separation up to 5 ps in a system with small energy offset of 50 meV.
- S. Matthew Menke
- , Alexandre Cheminal
- & Richard H. Friend
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Article
| Open AccessA biosensor-based framework to measure latent proteostasis capacity
A pool of quality control proteins (QC) maintains the protein-folding homeostasis in the cell, but its quantitative analysis is challenging. Here the authors develop a FRET sensor based on the protein barnase, able to quantify QC holdase activity and its ability to suppress protein aggregation.
- Rebecca J. Wood
- , Angelique R. Ormsby
- & Danny M. Hatters
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Article
| Open AccessSingle-molecule FRET reveals multiscale chromatin dynamics modulated by HP1α
Chromatin fibers undergo continuous structural rearrangements but their dynamic architecture is poorly understood. Here, the authors use single-molecule FRET to determine the structural states and interconversion kinetics of chromatin fibers, monitoring their effector protein-dependent dynamic motions.
- Sinan Kilic
- , Suren Felekyan
- & Beat Fierz
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Article
| Open AccessRaman enhancement on ultra-clean graphene quantum dots produced by quasi-equilibrium plasma-enhanced chemical vapor deposition
Surface-enhanced Raman spectroscopy (SERS) is a promising technology for sensitive optical sensors, generally using rough metal films. Here, Liu et al. synthesize high-quality graphene quantum dot films which offer a large SERS enhancement due to a strong light-matter interaction with Van Hove singularities.
- Donghua Liu
- , Xiaosong Chen
- & Dacheng Wei
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Article
| Open AccessTransient two-dimensional vibrational spectroscopy of an operating molecular machine
A deeper understanding of the mechanics of molecular machines is limited by the fast motions which are in the nanosecond or picosecond timescale. Here the authors present a real-time observation of structural changes in a rotaxane-based molecular shuttle by transient two-dimensional infrared spectroscopy.
- Matthijs R. Panman
- , Chris N. van Dijk
- & Sander Woutersen
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Article
| Open AccessIntracellular localization of nanoparticle dimers by chirality reversal
The ability to spectroscopically pinpoint whether nanoparticles are located inside or outside of cells represents an overarching need in biology and medicine. Here, the authors show that the chirality of DNA-bridged particle dimers reverses when they cross the cell membrane, providing a real-time chiroptical signature of their intra- or extracellular location.
- Maozhong Sun
- , Liguang Xu
- & Chuanlai Xu
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Article
| Open AccessAnti-Stokes photoluminescence probing k-conservation and thermalization of minority carriers in degenerately doped semiconductors
Anti-Stokes luminescence - the emission of photons with higher energy than those absorbed – in nanomaterials is widely used for optoelectronic applications. Here the authors observe it in degenerately doped bulk InP and GaAs, indicating it as a more general property of direct bandgap semiconductors.
- K. Mergenthaler
- , N. Anttu
- & M.-E. Pistol
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Article
| Open AccessSelf-probing spectroscopy of XUV photo-ionization dynamics in atoms subjected to a strong-field environment
Single photon ionization—one of the most fundamental light matter interactions—can be significantly altered in a strong-field environment. Here the authors demonstrate a self-probing spectroscopy technique, resolving the evolution of the interaction in helium atoms with attosecond precision.
- Doron Azoury
- , Michael Krüger
- & Nirit Dudovich
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Article
| Open AccessStrain-shear coupling in bilayer MoS2
Layered materials have strikingly anisotropic mechanical properties. Here, the authors use Raman spectroscopy and first-principles calculations to unveil that MoS2, an archetypal layered material, possesses a coupling between in-plane uniaxial strain and interlayer shear, enabling derivation of an unexplored off-diagonal elastic constant.
- Jae-Ung Lee
- , Sungjong Woo
- & Hyeonsik Cheong
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Article
| Open AccessSecond-order spectral lineshapes from charged interfaces
Charged interfaces are important in chemical systems, but the influence of charge on vibrational sum frequency spectra has only recently been considered. Here the authors show the importance of accounting for the interfacial potential-dependent χ(3) term in interpreting spectral lineshapes from charged interfaces.
- Paul E. Ohno
- , Hong-fei Wang
- & Franz M. Geiger
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Article
| Open AccessMapping the ultrafast flow of harvested solar energy in living photosynthetic cells
During photosynthesis, energy is transferred from photosynthetic antenna to reaction centers via ultrafast energy transfer. Here the authors track energy transfer in photosynthetic bacteria using two-dimensional electronic spectroscopy and show that these transfer dynamics constrain antenna complex organization.
- Peter D. Dahlberg
- , Po-Chieh Ting
- & Gregory S. Engel
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Article
| Open AccessElucidating the origins of multimode vibrational coherences of polyatomic molecules induced by intense laser fields
Nuclear dynamics of polyatomic molecules involves multiple degrees of freedom and is challenging to explore. Here the authors study the internuclear distance-dependent depletion and bond-softening induced vibrational wavepacket dynamics of CH3I molecules using femtosecond XUV transient absorption spectroscopy.
- Zhengrong Wei
- , Jialin Li
- & Zhi-Heng Loh
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Article
| Open AccessDual-comb spectroscopic ellipsometry
Spectroscopic ellipsometry is an established technique to characterize the optical properties of a material. Here, Minamikawa et al. combine the method with dual-comb spectroscopy, which allows them to obtain ellipsometric parameters including the phase difference between s-polarized and p-polarized light.
- Takeo Minamikawa
- , Yi-Da Hsieh
- & Takeshi Yasui
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Article
| Open AccessWhite light emission from a single organic molecule with dual phosphorescence at room temperature
The development of single molecule white light-emitters is extremely challenging for pure phosphorescent metal-free systems at room temperature. Here the authors show a single pure organic room temperature phosphor, 4-chlorobenzoyldibenzothiophene, utilizing the emission from both T1 and T2 states.
- Zikai He
- , Weijun Zhao
- & Ben Zhong Tang
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Article
| Open AccessRaman evidence for pressure-induced formation of diamondene
The synthesis of two-dimensional diamond is the ultimate goal of diamond thin-film technology. Here, the authors perform Raman spectroscopy of bilayer graphene under pressure, and obtain spectroscopic evidence of formation of diamondene, an atomically thin form of diamond.
- Luiz Gustavo Pimenta Martins
- , Matheus J. S. Matos
- & Luiz Gustavo Cançado
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Article
| Open AccessA volumetric three-dimensional digital light photoactivatable dye display
Despite living in a three-dimensional world, almost all information in our society is conveyed in a two-dimensional format. Here, the authors provide a technique for the generation of spatially accurate and high-resolution three-dimensional images using fluorescent photoswitch chemistry.
- Shreya K. Patel
- , Jian Cao
- & Alexander R. Lippert
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Article
| Open AccessNeutral and charged inter-valley biexcitons in monolayer MoSe2
Atomically thin transition metal dichalcogenides host excitons and trions, however higher-order states, although possible, are difficult to identify experimentally. Here, the authors perform polarization-resolved coherent spectroscopy to unveil the signature of neutral and charged inter-valley biexcitons in monolayer MoSe2.
- Kai Hao
- , Judith F. Specht
- & Galan Moody
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Article
| Open AccessObserving electron localization in a dissociating H2+ molecule in real time
Time resolved measurements provide insights to the intriguing process of ultrafast molecular fragmentation. Here the authors use CEP-locked laser pulses in pump–probe scheme to explore the H2+dissociation and find out that the electron localization to one of the nuclei occurs in about 15 fs.
- H. Xu
- , Zhichao Li
- & I. V. Litvinyuk
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Article
| Open AccessIn situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy
Rational design of heterogeneous catalysts requires molecular understanding of catalytic processes. Here, the authors attach PtFe and Pd nanocatalysts to Raman signal-enhancing Au-silica nanoparticles, allowing them to spectroscopically observe the active species and bonds involved in CO oxidation in real time.
- Hua Zhang
- , Chen Wang
- & Zhong-Qun Tian
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Article
| Open AccessUnified model for singlet fission within a non-conjugated covalent pentacene dimer
Singlet fission is an important process occurring in solar cells, however the mechanism is not well understood. Here the authors reveal intermediates during singlet fission of a non-conjugated pentacene dimer, developing a single kinetic model to describe the data over seven temporal orders of magnitude at room and cryogenic temperatures.
- Bettina S. Basel
- , Johannes Zirzlmeier
- & Dirk M. Guldi
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Article
| Open AccessObservation of the universal magnetoelectric effect in a 3D topological insulator
The electrodynamics of topological insulators has been predicted to show a new magnetoelectric term, but this hasn’t been observed. Here, Dziomet al. observe a universal Faraday rotation angle equal to the fine structure constant, evidencing the so-called topological magnetoelectric effect.
- V. Dziom
- , A. Shuvaev
- & L. W. Molenkamp
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Article
| Open AccessRETRACTED ARTICLE: Precise determination of graphene functionalization by in situ Raman spectroscopy
Raman spectroscopy is a versatile tool to gain insight into the functionalization of graphene-based materials, yet unequivocal assignment of the vibrational modes associated with covalent binding has so far remained elusive. Here, the authors succeed in an experimental and theoretical identification of this molecular fingerprint.
- Philipp Vecera
- , Julio C. Chacón-Torres
- & Andreas Hirsch
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Article
| Open AccessVolumetric chemical imaging by stimulated Raman projection microscopy and tomography
Recent advances have enabled high-speed three-dimensional optical imaging through the use of fluorescent markers. Here, Chenet al. integrate stimulated Raman imaging into those methods, enabling the label-free and chemically specific volumetric imaging of complex samples.
- Xueli Chen
- , Chi Zhang
- & Ji-Xin Cheng
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Article
| Open AccessTransient birefringence of liquids induced by terahertz electric-field torque on permanent molecular dipoles
Low-frequency structural dynamics in liquids and their underlying interactions are complex and challenging to resolve. Here, Sajadiet al. use intense terahertz fields to directly interrogate intermolecular modes in polar liquids by coupling the fields to their permanent molecular dipole moments.
- Mohsen Sajadi
- , Martin Wolf
- & Tobias Kampfrath
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Article
| Open AccessEnabling valley selective exciton scattering in monolayer WSe2 through upconversion
Monolayer transition metal dichalcogenides host excitons, bound electron-hole pairs that play a pivotal role in optoelectronic applications relying on strong light-matter interaction. Here, the authors unveil the spectroscopic signature of boson scattering of two-dimensional excitons in monolayer WSe2.
- M. Manca
- , M. M. Glazov
- & B. Urbaszek
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Article
| Open AccessPressure modulates the self-cleavage step of the hairpin ribozyme
Studying the reactivity of ribozymes under extreme pressure could provide insights to optimize biocatalytic RNA design. Here, the authors show that at high pressure the transesterification step of the hairpin ribozyme self-cleavage reaction accelerates, while the overall process is slower.
- Caroline Schuabb
- , Narendra Kumar
- & Roland Winter
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Article
| Open AccessQuantum coherence selective 2D Raman–2D electronic spectroscopy
Electronic and vibrational correlations report on the dynamics and structure of molecular species, yet revealing these correlations experimentally is challenging. Here the authors develop a method called GAMERS that probes correlations between states within the vibrational and electronic manifold with quantum coherence selectivity.
- Austin P. Spencer
- , William O. Hutson
- & Elad Harel
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Article
| Open AccessIntervalley scattering by acoustic phonons in two-dimensional MoS2 revealed by double-resonance Raman spectroscopy
Double-resonance Raman scattering is a sensitive spectroscopic probe of the interplay between electrons and phonons in a crystal. Here, the authors unveil the signature of double-resonance intervalley scattering by acoustic phonons in two-dimensional MoS2, underpinning the physics of valley depolarization.
- Bruno R. Carvalho
- , Yuanxi Wang
- & Marcos A. Pimenta
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Article
| Open AccessUltrafast fluxional exchange dynamics in electrolyte solvation sheath of lithium ion battery
The lithium solvation structure in the electrolyte solution for lithium-ion batteries has not been fully understood. Here, the authors show ultrafast fluxional exchange of carbonate solvent molecules in and out of lithium-ion solvation sheath utilizing coherent two-dimensional infrared spectroscopy.
- Kyung-Koo Lee
- , Kwanghee Park
- & Minhaeng Cho
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Article
| Open AccessTowards high-resolution laser ionization spectroscopy of the heaviest elements in supersonic gas jet expansion
It is challenging to explore properties of heavy elements as they can only be produced artificially. Here, the authors demonstrate a high resolution spectroscopy method, studying the properties of actinium, which can be extended to the study of other elements located at the end of the periodic table.
- R. Ferrer
- , A. Barzakh
- & A. Zadvornaya
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Article
| Open AccessQuantification of re-absorption and re-emission processes to determine photon recycling efficiency in perovskite single crystals
Fanget al. develop a method to determine the photon recycling efficiency for organic-inorganic hybrid single crystal perovskites by differentiating between emitted and re-absorbed photons based on their polarization difference. For these systems efficiencies of less than 0.5% are reported.
- Yanjun Fang
- , Haotong Wei
- & Jinsong Huang