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| Open AccessTwofold rigidity activates ultralong organic high-temperature phosphorescence
Obtaining high-temperature phosphorescence in organic materials can potentially lead to broader applications, but can be challenging to achieve. Here, the authors report the use of rigid molecules as both host and guest to give temperature resistance and therefore high-temperature phosphorescence.
- Kaijun Chen
- , Yongfeng Zhang
- & Xiang Ma
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Article
| Open AccessBioinspired light-driven chloride pump with helical porphyrin channels
Artificial ion channels have potential in a range of applications, but achieving performance comparable to biological channels has been challenging. Here, the authors report an artificial, light-driven chloride pump, inspired by halorhodopsin, with a helical porphyrin channel array.
- Chao Li
- , Yi Zhai
- & Lei Jiang
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Article
| Open AccessAnti-Kasha triplet energy transfer and excitation wavelength dependent persistent luminescence from host-guest doping systems
Anti-Kasha processes have potential in organic luminogens, but design of materials with these characteristics is challenging. Here, the authors report the development of a host-guest system with anti-Kasha behaviour and triplet energy transfer.
- Weiwei Xie
- , Wenbin Huang
- & Ben Zhong Tang
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Article
| Open AccessTheory predicts UV/vis-to-IR photonic down conversion mediated by excited state vibrational polaritons
Vibrational polaritons steer chemical reactions and control quantum states for information processing. Here the authors predict their formation during electronic photo-excitation, enabling a down-conversion of visible to infrared photons.
- Connor K. Terry Weatherly
- , Justin Provazza
- & Roel Tempelaar
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Article
| Open AccessEntangled spin-polarized excitons from singlet fission in a rigid dimer
Singlet fission is recognized as an enabling process for next-generation solar cells. Here the authors design a molecular system where specific spin sub-levels can be initialized to produce a highly entangled state and demonstrate that the coherence between magnetic sub-levels of that state is preserved at higher temperatures than those encountered in conventional superconducting quantum hardware.
- Ryan D. Dill
- , Kori E. Smyser
- & Joel D. Eaves
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Article
| Open AccessEnergy cascades in donor-acceptor exciton-polaritons observed by ultrafast two-dimensional white-light spectroscopy
Exciton-polaritons are hybridized light-matter states that exhibit intriguing phenomena that are unobserved in purely excitonic states. Here, the authors elucidate the photophysical mechanism of polariton-assisted long-range energy transfer in carbon nanotubes using two-dimensional white-light spectroscopy and quantum calculations.
- Minjung Son
- , Zachary T. Armstrong
- & Martin T. Zanni
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Article
| Open AccessTowards the engineering of a photon-only two-stroke rotary molecular motor
Improving the efficiency of light-driven molecular rotary motors is a challenging task. Here, the authors combine theoretical modeling, synthesis and spectroscopy to prepare a prototype molecular motor capable of avoiding inefficient thermally activated motion; thus offering prospects to implement a 2-stroke photon-only molecular motor.
- Michael Filatov(Gulak)
- , Marco Paolino
- & Massimo Olivucci
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Article
| 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 AccessTriple ionization and fragmentation of benzene trimers following ultrafast intermolecular Coulombic decay
Higher-order aromatic clusters are prevalent in biochemical systems, but a full understanding of their structural and dynamical properties is lacking. Here, the authors demonstrate that inner-valence ionization can induce ultrafast relaxation and further fragmentation mechanisms in benzene trimers.
- Jiaqi Zhou
- , Xitao Yu
- & Xueguang Ren
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Article
| Open AccessA reconfigurable and magnetically responsive assembly for dynamic solar steam generation
Despite a promising water harvesting approach solar steam generation low efficiency remains a challenging obstacle. Here, authors present a macro- and microscopically reconfigurable and magnetically responsive assembly towards a dynamic evaporation system with improved performance and salt resistance.
- Yajie Hu
- , Hongyun Ma
- & Liangti Qu
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Article
| Open AccessEnergy-efficient pathway for selectively exciting solute molecules to high vibrational states via solvent vibration-polariton pumping
Hybrid light-matter states formed in the strong light-matter coupling regime can alter the molecular ground-state reactivity. Here, Li et al. computationally demonstrate that pumping a collection of solvent molecules forming hybrid vibrational light-matter states in an optical cavity can excite solute molecules to very high excited states.
- Tao E. Li
- , Abraham Nitzan
- & Joseph E. Subotnik
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Article
| Open AccessA bioinspired sequential energy transfer system constructed via supramolecular copolymerization
Sequential energy transfer is ubiquitous in natural light harvesting systems, but most artificial mimics have unsatisfactory energy transfer efficiency. Here, authors synthesize a sequential energy transfer system with overall efficiency of 87.4% via supramolecular copolymerization mimicking the aggregation mode of bacteriochlorophyll pigments in green photosynthetic bacteria.
- Yifei Han
- , Xiaolong Zhang
- & Feng Wang
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Article
| Open AccessMicrocavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors
Exciton-polaritons are typically formed in organic systems when the molecules are confined between metallic or dielectric mirrors. Here, the authors reveal that interactions between excitons and moderately confined photonic states within the bare organic film can also lead to polariton formation, making them the primary photoexcitation.
- Raj Pandya
- , Richard Y. S. Chen
- & Akshay Rao
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Article
| Open AccessPhoton upconversion through triplet exciton-mediated energy relay
Photon upconversion in lanthanide-doped nanoparticles enables important technological developments. Here the authors demonstrate a mechanism leading to enhanced upconversion emission in core-shell nanoparticles, and long-distance energy transfer between nanoparticles, through triplet state population of an organic surface ligand.
- Sanyang Han
- , Zhigao Yi
- & Xiaogang Liu
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Article
| Open AccessThrough bonds or contacts? Mapping protein vibrational energy transfer using non-canonical amino acids
Vibrational energy transfer (VET) is essential for protein function as it is responsible for efficient energy dissipation in reaction sites and is linked to pathways of allosteric communication. Here authors equipped a tryptophan zipper with a VET injector and a VET sensor for femtosecond pump probe experiments to map the VET.
- Erhan Deniz
- , Luis Valiño-Borau
- & Jens Bredenbeck
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Article
| Open AccessExcitonic structure and charge separation in the heliobacterial reaction center probed by multispectral multidimensional spectroscopy
The primary energy conversion step in photosynthesis, charge separation, takes place in the reaction center. Here the authors investigate the heliobacterial reaction center using multispectral two-dimensional electronic spectroscopy, identifying the primary electron acceptor and revealing the charge separation mechanism.
- Yin Song
- , Riley Sechrist
- & Jennifer P. Ogilvie
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Article
| Open AccessLong- and short-ranged chiral interactions in DNA-assembled plasmonic chains
Here, the authors experimentally demonstrate chiral transfer over large distances up to 100 nm. They realise the coupling with an achiral nanosphere situated between a pair of distant gold nanorods arranged in a chiral fashion using DNA origami, and observe enhanced circular dichroism signals.
- Kevin Martens
- , Felix Binkowski
- & Tim Liedl
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Article
| Open AccessPolariton-assisted excitation energy channeling in organic heterojunctions
Exploiting delocalized organic polaritons for enhanced exciton harvesting has been advantageous for organic optoelectronic with planar heterojunctions. Here, the authors report polariton-assisted excitation energy channeling in organic heterojunctions coupled to the same cavity mode.
- Mao Wang
- , Manuel Hertzog
- & Karl Börjesson
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Article
| Open AccessShallow distance-dependent triplet energy migration mediated by endothermic charge-transfer
Spin-triplet energy transfer in molecular systems underlies important applications for chemistry and devices. Here, the authors investigate the triplet energy transfer in CdSe quantum dots with varying ZnS shell thicknesses to surface-anchored anthracene molecules and identify a stepwise mechanism mediated by endothermic charge-transfer states.
- Runchen Lai
- , Yangyi Liu
- & Kaifeng Wu
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Article
| Open AccessVibrational couplings and energy transfer pathways of water’s bending mode
Vibrational energy transfer in water involves intermolecular coupling of O-H stretching modes, but much less is known about the role of the bending modes. Here the authors, combining static and femtosecond infrared, Raman, and hyper-Raman spectroscopy and ab initio molecular dynamics simulations, provide insight into the energy dynamics of the bend vibrations.
- Chun-Chieh Yu
- , Kuo-Yang Chiang
- & Yuki Nagata
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Article
| Open AccessDesign of highly efficient deep-blue organic afterglow through guest sensitization and matrices rigidification
Though realizing organic materials with deep blue emission is attractive for next-generation display technologies, achieving this emission in afterglow molecules remains a challenge. Here, the authors report blue organic afterglow via a strategy involving guest sensitization and matrix rigidification.
- Shen Xu
- , Wu Wang
- & Wei Huang
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Perspective
| Open AccessDesigning and understanding light-harvesting devices with machine learning
Photon-induced charge separation phenomena are at the heart of light-harvesting applications but challenging to be described by quantum mechanical models. Here the authors illustrate the potential of machine-learning approaches towards understanding the fundamental processes governing electronic excitations.
- Florian Häse
- , Loïc M. Roch
- & Alán Aspuru-Guzik
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Article
| Open AccessA leap in quantum efficiency through light harvesting in photoreceptor UVR8
Photoreceptor UVR8 in plants senses environmental UV levels through 26 structural tryptophan residues, but the role of 18 of them was unknown. The authors show, by experiments and computations, how these form a light-harvesting network that funnels the excitation to the pyramid centers enhancing the light-perception efficiency.
- Xiankun Li
- , Haisheng Ren
- & Dongping Zhong
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Article
| Open AccessHeavy N+ ion transfer in doubly charged N2Ar van der Waals cluster
There are multiple ways by which energy and charge transfer occur in weakly bound systems. Here the authors reveal a heavy ion N+ transfer in a doubly charged Van der Waals cluster produced in collisions of the highly charged Ne8+ ion with N2Ar, leading to fragmentation of N+ and NAr+ via Coulomb explosion.
- XiaoLong Zhu
- , XiaoQing Hu
- & X. Ma
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Article
| Open AccessWater acting as a catalyst for electron-driven molecular break-up of tetrahydrofuran
Reactions induced by low-energy electrons in hydrated systems are central to radiation therapy, but a full understanding of their mechanism is lacking. Here the authors investigate the electron-impact induced ionization and subsequent dissociation of tetrahydrofuran, model for biochemically relevant systems, in a micro-solvated environment.
- Enliang Wang
- , Xueguang Ren
- & Alexander Dorn
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Article
| Open AccessObservation of dissipative chlorophyll-to-carotenoid energy transfer in light-harvesting complex II in membrane nanodiscs
Resolving the kinetics of energy dissipation during photosynthesis is challenging due to complex photophysics and the coexistence of multiple antenna proteins. Here Son et al. overcome this by applying ultrabroadband 2D spectroscopy to LHCII reconstituted in lipid nanodiscs, revealing mechanisms of dissipation enhanced by the membrane.
- Minjung Son
- , Alberta Pinnola
- & Gabriela S. Schlau-Cohen
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Article
| Open AccessMechanisms of triplet energy transfer across the inorganic nanocrystal/organic molecule interface
Though literature reports models describing triplet energy transfer between inorganic semiconductors and organic molecules, a unified mechanism for this process is still lacking. Here, the authors report triplet energy transfer mechanism at lead halide perovskite nanocrystal/polyacene interfaces.
- Xiao Luo
- , Yaoyao Han
- & Kaifeng Wu
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Article
| Open AccessTopology, landscapes, and biomolecular energy transport
Understanding vibrational energy transfer in macromolecules has been challenging to both theory and experiment. Here the authors use non-equilibrium molecular dynamics to reveal the relationship between heat transport in a model peptide, emergent nonlinearity, and the underlying free energy landscape.
- Justin E. Elenewski
- , Kirill A. Velizhanin
- & Michael Zwolak
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Article
| Open AccessInterplay between structural hierarchy and exciton diffusion in artificial light harvesting
Light-harvesting antennas and efficient energy transfer enable photosynthesis in low light conditions in natural systems. Here the authors resolve exciton properties and the role of structural hierarchy in a model light-harvesting complex by excited-state 2D spectroscopy on a microfluidic platform.
- Björn Kriete
- , Julian Lüttig
- & Maxim S. Pshenichnikov
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Article
| Open AccessDual-color fluorescent nanoparticles showing perfect color-specific photoswitching for bioimaging and super-resolution microscopy
Photoswitchable nanoparticles can be used for selective imaging in biological systems but usually have only one color. Here the authors develop a two-color fluorescent emissive system that allows full on-off switching of one component color of the system while the other color is unaffected, which has implications for super-resolution imaging.
- Dojin Kim
- , Keunsoo Jeong
- & Soo Young Park
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Article
| Open AccessLow-energy electrons transform the nimorazole molecule into a radiosensitiser
Radiosensitisers are believed to interfere with cancer cells by dissociating upon interaction with electrons. Here the authors observe instead that the dominant path for nitroimidazolic radiosensitisers involves formation of a non-dissociated radical anion, prerequisite for their accumulation in tumour cells.
- Rebecca Meißner
- , Jaroslav Kočišek
- & Stephan Denifl
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Article
| Open AccessUltrafast energy relaxation dynamics of amide I vibrations coupled with protein-bound water molecules
Vibrational energy relaxation of proteins helps us to understand ultrafast protein dynamics. Here, the authors determine the vibrational energy transfer time of the amide I mode in aqueous environment and find that water provides a “shortcut” through a direct resonant channel to dissipate energy into the solvent.
- Junjun Tan
- , Jiahui Zhang
- & Shuji Ye
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Article
| Open AccessSpatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria
2D electronic spectroscopy enables a spatially-averaged view of the electronic structure of a heterogeneous system. Here, the authors extend it to sub-micron resolution and ~106 times better sensitivity, to resolve spatially varying excitonic structure in a heterogeneous mixture of photosynthetic cells.
- Vivek Tiwari
- , Yassel Acosta Matutes
- & Jennifer P. Ogilvie
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Article
| Open AccessWater printing of ferroelectric polarization
Controlling ferroelectric polarization is conventionally achieved by applying electric fields, mechanical force or similar. Here reversible switching of the bulk polarization of a BiFeO3 thin film is demonstrated by pattering aqueous solution on to the surface enabling large-scale switching.
- Yu Tian
- , Lanying Wei
- & Jinxing Zhang
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Article
| Open AccessNear-infrared-triggered photon upconversion tuning in all-inorganic cesium lead halide perovskite quantum dots
Optimizing luminescence from quantum dots benefits various optoelectronic and photovoltaic applications. Here the authors drive high-efficiency, tunable upconversion luminescence in perovskite quantum dots by energy transfer from lanthanide-doped nanoparticles excited by near-infrared light, to produce full-color emission with low driving power.
- Wei Zheng
- , Ping Huang
- & Xueyuan Chen
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Article
| Open AccessThe influence of retardation and dielectric environments on interatomic Coulombic decay
Interatomic Coulombic Decay is a non-radiative relaxation process between excited systems. Here the authors report a theoretical framework based on macroscopic quantum electrodynamics that shows the role of retardation and an environment in the enhancement or suppression of the ICD rate.
- Joshua Leo Hemmerich
- , Robert Bennett
- & Stefan Yoshi Buhmann
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Article
| Open AccessDirect observation of exciton–exciton interactions
Some photo-physical processes in multichromophore systems might get triggered only if two excitations are present. Here, the authors introduce exciton–exciton-interaction 2D spectroscopy, which is a non-linear optical method that can selectively track the time evolution of such effects.
- Jakub Dostál
- , Franziska Fennel
- & Tobias Brixner
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Article
| Open AccessNear infrared light induced plasmonic hot hole transfer at a nano-heterointerface
Hot hole transfer has applications in plasmonics, photocatalysis, and light harvesting, but is often limited by low quantum yields and short-lived charge separation times. Here, Lian et al. overcome these limitations in heterostructured nanocrystals and proposed a new hot hole transfer mechanism.
- Zichao Lian
- , Masanori Sakamoto
- & Toshiharu Teranishi
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Article
| Open AccessMolecular solar thermal energy storage in photoswitch oligomers increases energy densities and storage times
Molecular solar thermal systems are promising for storing solar energy but achieving high energy storage densities and absorption characteristics matching the solar spectrum is challenging. Here the authors present a design strategy for electronically coupled photoswitches which allow for high energy density storage for solar energy storage applications.
- Mads Mansø
- , Anne Ugleholdt Petersen
- & Kasper Moth-Poulsen
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Article
| Open AccessPhoton antibunching in a cluster of giant CdSe/CdS nanocrystals
Semiconductor nanocrystals have potential applications in optoelectronic devices including single-photon emission sources. Here, Lv et al. demonstrate that nanocrystals within small clusters can electronically couple, thereby increasing their optical cross-section while the optical emission remains antibunched.
- Bihu Lv
- , Huichao Zhang
- & Min Xiao
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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 AccessExperimental demonstration of photon upconversion via cooperative energy pooling
Photon upconversion methods demonstrated thus far involve challenging requirements. Here Weingartenet al. demonstrate a mechanism called cooperative energy pooling, in which multiple photoexcited sensitizers resonantly and simultaneously transfer their energies to a higher-energy state on a single acceptor.
- Daniel H. Weingarten
- , Michael D. LaCount
- & Sean E. Shaheen
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Article
| Open AccessModified relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons
Vibration-cavity polaritons are mixed states produced by strong coupling between a vibrational mode and an optical cavity. Here, the authors show that these polaritons can coherently exchange energy and exhibit drastically altered transient spectra and dynamics compared to uncoupled vibrations.
- A. D. Dunkelberger
- , B. T. Spann
- & J. C. Owrutsky
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Article
| Open AccessDirect evidence of two interatomic relaxation mechanisms in argon dimers ionized by electron impact
Inter-particle reactions in weakly bound systems are often difficult to pinpoint by detecting exclusively the kinetic energy of the produced ions. Here the authors present a full-coincidence experiment, where inter-particle reaction channels are determined by the measurement of all outgoing particles.
- Xueguang Ren
- , Elias Jabbour Al Maalouf
- & Stephan Denifl
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Article
| Open AccessObservation of correlated electronic decay in expanding clusters triggered by near-infrared fields
In clusters, relaxation of excited atoms can lead to ionization of nearby atoms, a process known as interatomic Coulomb decay. Here, the authors report on a so far unobserved correlated electronic decay process following Rydberg atom generation in clusters ionized by intense near-infrared fields.
- B. Schütte
- , M. Arbeiter
- & A. Rouzée
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Article
| Open AccessBorromean three-body FRET in frozen Rydberg gases
Rydberg atoms are promising platform for quantum simulations, due to their strong and controllable dipole–dipole interactions. Here, the authors predict few-body processes in Rydberg atoms which resemble fluorescence resonance energy transfer in biological setting, and observe them in cold caesium atoms.
- R. Faoro
- , B. Pelle
- & P. Pillet
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Article
| Open AccessIonization-induced annealing of pre-existing defects in silicon carbide
Silicon carbide possesses myriad properties which render it an ideal material for implementation in harsh radiation environments. Here, the authors show that damaged SiC can be repaired through ionization-induced healing, which has broader implications for the design of future radiation-tolerant materials.
- Yanwen Zhang
- , Ritesh Sachan
- & William J. Weber
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Article
| Open AccessDirect observation of multistep energy transfer in LHCII with fifth-order 3D electronic spectroscopy
Photosynthesis is a complex process, involving the transfer of sunlight driven excitation energy to a reaction centre. Here, the authors directly observe the multistep excitation energy transitions in a light-harvesting complex using ultrafast fifth-order three-dimensional electronic spectroscopy.
- Zhengyang Zhang
- , Petar H. Lambrev
- & Howe-Siang Tan
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Article
| Open AccessThermodynamic picture of ultrafast charge transport in graphene
A linear energy–momentum relation of graphene results in a high direct-current electron mobility, but this is not necessarily true at terahertz frequencies. Here, the authors show that its ultrafast conductivity is dependent on a highly nonlinear interplay between heating and cooling of the electron gas.
- Zoltán Mics
- , Klaas-Jan Tielrooij
- & Dmitry Turchinovich