Featured
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| Open AccessBioinspired polymeric supramolecular columns as efficient yet controllable artificial light-harvesting platform
The formation of artificial light-harvesting systems with high donor/acceptor ratios for efficient energy transfer remains challenging. Here, the authors describe a polymeric supramolecular column-based light-harvesting system by modular columnar assembly of donor/acceptor chromophores, enabling superior light-harvesting efficiency and dynamic full-color tunable emission.
- Bin Mu
- , Xiangnan Hao
- & Wei Tian
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Article
| Open AccessMulti-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling
Placing an organic material in an optical cavity can enhance exciton transport, but the mechanism is poorly understood. Here, using molecular dynamics simulations, the authors obtained atomistic insights into that mechanism.
- Ilia Sokolovskii
- , Ruth H. Tichauer
- & Gerrit Groenhof
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Article
| Open AccessFerricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy
Reliably identifying transient intermediates is crucial to elucidate chemical reaction mechanisms. Here, the authors use femtosecond Fe Kβ main line and valence-to-core x-ray emission spectroscopy to characterize a short-lived intermediate of the aqueous ferricyanide photo-aquation reaction.
- Marco Reinhard
- , Alessandro Gallo
- & Dimosthenis Sokaras
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Article
| Open AccessUltrafast motion in a third generation photomolecular motor
Controlling molecular motion at nanoscale is important for the design of nanomachines. Here the authors use ultrafast vibrational and electronic spectroscopy to characterize the mechanism of motion of a light driven molecular motor designed to support translational movement.
- Palas Roy
- , Wesley R. Browne
- & Stephen R. Meech
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Article
| Open AccessPhotocatalytic CO2 reduction with aminoanthraquinone organic dyes
A class of inexpensive aminoanthraquinone organic dyes are shown to facilitate visible-light-driven CO2 reduction. Overall reaction efficiencies were found to be optimal when both electron donating and accepting groups were on a single dye molecule.
- Qinqin Lei
- , Huiqing Yuan
- & Zhiji Han
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Article
| Open AccessEnhanced chiroptic properties of nanocomposites of achiral plasmonic nanoparticles decorated with chiral dye-loaded micelles
Circularly polarized luminescent materials with large dissymmetry and efficiency are in demand. Here, the authors investigate chirality-induced spin polarization in achiral gold nanorods decorated with chiral dye-loaded micelles to enhance chiroptic activity.
- Tonghan Zhao
- , Dejing Meng
- & Pengfei Duan
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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 AccessCoemissive luminescent nanoparticles combining aggregation-induced emission and quenching dyes prepared in continuous flow
Developing efficient light harvesting systems at low cost is a challenge. Here, the authors synthesized coemissive dyes in a continuous flow microreactor featuring a controlled cascade FRET process combining aggregation-induced emission and quenching.
- Chong Li
- , Qi Liu
- & Shengyang Tao
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Article
| Open AccessBreaking photoswitch activation depth limit using ionising radiation stimuli adapted to clinical application
Triggered therapeutics are of interest but currently suffer from limited penetration depth of light sources. Here, the authors report on the development of a system, called radioswitch, that uses ionising irradiation to switch an azobenzene modified drug to an active form for deep tissue triggered therapeutic application.
- Alban Guesdon-Vennerie
- , Patrick Couvreur
- & Guillaume Bort
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Article
| Open AccessAn unexpected strategy to alleviate hypoxia limitation of photodynamic therapy by biotinylation of photosensitizers
Type I photodynamic therapy (PDT) sensitizers show good hypoxia tolerance but only few strategies are available for the design of purely organic Type I photosensitizers (PS). Here, the authors use biotinylation as design strategy to obtain PS-Biotin sensitizers with high efficiency for the generation of superoxide anion radicals and singlet oxygen.
- Jing An
- , Shanliang Tang
- & Wen-Heng Zheng
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Article
| Open AccessSynthesis of fluorescent organic nano-dots and their application as efficient color conversion layers
Compared to inorganic nanoparticles, organic nanoparticles aren’t as well understood. Here the authors explore the use of surfactants to prepare organic semiconductor nanoparticles with outstanding photophysical properties.
- Yeasin Khan
- , Soonjae Hwang
- & Jang Hyuk Kwon
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Article
| Open AccessSelective photoinduced charge separation in perylenediimide-pillar[5]arene rotaxanes
The development of complex molecular machinery requires a detailed appreciation of the factors that control energy pathways through the nanoscale scaffold. Here, the authors demonstrate that hetero-rotaxanes can be employed to create assemblies of different redox and photo-active components that enable selective tuning of energy transfer pathways.
- Nicholas Pearce
- , Katherine E. A. Reynolds
- & Neil R. Champness
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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 AccessBoosting photoelectrochemical efficiency by near-infrared-active lattice-matched morphological heterojunctions
The solar conversion efficiencies of photoelectrochemical catalysis are hindered by the light harvesting range. Here, the authors use near-infrared-active photoanodes that feature lattice-matched morphological hetero-nanostructures to realize efficient photoelectrochemical hydrogen production.
- Guo-Qiang Liu
- , Yuan Yang
- & Edward H. Sargent
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Article
| Open AccessProton gradients from light-harvesting E. coli control DNA assemblies for synthetic cells
Controlled actuation is an important aspect of synthetic cellular systems. Here, the authors combine pH responsive DNA origami structures with light triggered proton pump engineered E. coli to trigger a change in pH and control the deformation of giant unilamellar vesicles by simple illumination.
- Kevin Jahnke
- , Noah Ritzmann
- & Kerstin Göpfrich
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Article
| Open AccessBarrier-free reverse-intersystem crossing in organic molecules by strong light-matter coupling
Strong coupling of organic materials with optical cavities allows to manipulate the rate of energy transfer between their internal states. Here, the authors show a hybrid state of singlet character with energy lower than the triplet state, and a flow of energy from the triplet to the hybrid state.
- Yi Yu
- , Suman Mallick
- & Karl Börjesson
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Article
| Open AccessLong wavelength single photon like driven photolysis via triplet triplet annihilation
The use of short wavelength light in photolysis applications in chemistry and biology is limited by photolytic reaction yields, photodamage and photobleaching. Here, the authors report a general long wavelength single photon driven photolysis method using a triplet-triplet annihilation process.
- Ling Huang
- , Le Zeng
- & Gang Han
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Article
| Open AccessSequentially amplified circularly polarized ultraviolet luminescence for enantioselective photopolymerization
Chiral functional materials with circularly polarized luminescence can be used in various applications but rarely reported. Here the authors show, a complex system, which show intense circularly polarized ultraviolet luminescence with large glum value, enabling a chiral UV light triggered enantioselective polymerization.
- Dongxue Han
- , Xuefeng Yang
- & Pengfei Duan
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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 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 AccessVibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering
Photoinduced non-adiabatic intramolecular processes have important applications but their mechanisms are challenging to explore. Here the authors detect and assign vibrational wavepacket dynamics in a Fe carbene complex by ultrafast X-ray emission spectroscopy and X-ray scattering, resolving nuclear and electronic motion.
- Kristjan Kunnus
- , Morgane Vacher
- & Kelly J. Gaffney
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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 AccessCompartmentalization-induced phosphorescent emission enhancement and triplet energy transfer in aqueous medium
Artificial light harvesting systems in aqueous medium are challenging to realize due to quenching effects from water and oxygen. Here the authors demonstrate rod-coil amphiphiles which act as compartmentalization agent to shield platinum(II) phosphors and enable their ordered spatial organization.
- Zijian Li
- , Yifei Han
- & Feng Wang
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Article
| Open AccessSolar energy storage at an atomically defined organic-oxide hybrid interface
Molecular photoswitches provide an extremely simple solution for solar energy conversion and storage. Here, the authors report on the assembly of an operational solar energy-storing organic-oxide hybrid interface, which consists of a tailor-made molecular photoswitch and an atomically-defined semiconducting oxide film.
- Christian Schuschke
- , Chantal Hohner
- & Jörg Libuda
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Article
| Open AccessIminothioindoxyl as a molecular photoswitch with 100 nm band separation in the visible range
The design of photoswitches which operate in the visible light regime, show a large separation of absorption bands and are functional in various solvents is challenging. Here the authors report Iminothioindoxyls as visible-light operated photoswitches with a band separation of 100 nm.
- Mark W. H. Hoorens
- , Miroslav Medved’
- & Wiktor Szymanski
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Article
| Open AccessHighly efficient photothermal nanoagent achieved by harvesting energy via excited-state intramolecular motion within nanoparticles
Molecular motion has attracted a wide range of interest for different applications. Here, the authors develop nanoparticles with internal molecular motion upon near infrared absorption and use the nanoparticles for photoacoustic imaging and demonstrate this application in vivo.
- Zheng Zhao
- , Chao Chen
- & Ben Zhong Tang
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Article
| Open AccessClear and transparent nanocrystals for infrared-responsive carrier transfer
Infrared-light-induced carrier transfer is a key technology for ‘invisible’ optical devices, but making materials with the right properties remains a challenge. Here, the authors fabricate a clear and colourless material which converts infrared light to an electrical signal or energy based on a localized surface plasmon resonance, with implications for the development of invisible optical devices.
- Masanori Sakamoto
- , Tokuhisa Kawawaki
- & Toshiharu Teranishi
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Article
| Open AccessCooperative supramolecular polymers with anthracene‒endoperoxide photo-switching for fluorescent anti-counterfeiting
There is a continual pursuit for different ways to detect counterfeiting in today’s society. Here the authors show photo-responsive supramolecular polymers can be used in fluorescent anti-counterfeit applications, by taking advantage of multicycle anthracene‒endoperoxide switching properties.
- Zhao Gao
- , Yifei Han
- & Feng Wang
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Article
| Open AccessSkin color-specific and spectrally-selective naked-eye dosimetry of UVA, B and C radiations
Current ultraviolet (UV) sensors cannot differentiate between UVA, B and C, each of which has a remarkably different impact on human health. Here the authors show spectrally-selective colorimetric monitoring of ultraviolet radiations by developing a photoelectrochromic ink that consists of a multiredox polyoxometalate and an e– donor.
- Wenyue Zou
- , Ana González
- & Vipul Bansal
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Article
| Open AccessGallium nitride nanowire as a linker of molybdenum sulfides and silicon for photoelectrocatalytic water splitting
Sunlight-harvesting materials require the clean integration of light-absorbing and catalytic components to be efficient. Here, authors link silicon photoelectrodes and molybdenum sulfide catalysts with defect-free gallium nitride nanowire to improve photoelectrochemical hydrogen evolution.
- Baowen Zhou
- , Xianghua Kong
- & Zetian Mi
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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 AccessNanographenes as electron-deficient cores of donor-acceptor systems
Nanographenes in donor-acceptor π-systems generally serve as electron-donating moieties but the reversed structures are hardly reported. Here, the authors present a facile synthetic protocol towards reversed donor-acceptor nanographenes by amination and demonstrate fine property tuning by varying the donating ability of the aniline groups.
- Yu-Min Liu
- , Hao Hou
- & Klaus Müllen
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Economic photoprotection in photosystem II that retains a complete light-harvesting system with slow energy traps
Photosystem II possesses a protection mechanism to prevent damage when exposed to high-intensity light. Here, the authors analyze the functional consequences of structural changes associated with this process, and show that protection does not undermine energy capture by open reaction centres.
- Erica Belgio
- , Ekaterina Kapitonova
- & Alexander V. Ruban
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Maximizing omnidirectional light harvesting in metal oxide hyperbranched array architectures
The development of structured electrode architectures is one of the strategies for improving photovoltaic performance. Here, the authors report hierarchical hyperbranced titania materials, composed of nanowires and nanosheets, linked by nanorods, and assess their solar energy conversion efficiency.
- Wu-Qiang Wu
- , Hao-Lin Feng
- & Cheng-Yong Su
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LTD is a protein required for sorting light-harvesting chlorophyll-binding proteins to the chloroplast SRP pathway
Chloroplast proteins are synthesized in the cytosol and imported into the chloroplast before being delivered to the thylakoids. The authors report that an ankyrin-repeat protein, LTD, is essential for the routing of chlorophyll-binding proteins to the signal recognition particle pathway.
- Min Ouyang
- , Xiaoyi Li
- & Lixin Zhang
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A bacterial proteorhodopsin proton pump in marine eukaryotes
Proteorhodopsin is used by prokaryotes to generate energy from light. In this study, the authors describe a prokaryote-to-eukaryote horizontal gene transfer of a bacterial proteorhodopsin gene to dinoflagellates, suggesting that these eukaryotes can also use proteorhodopsin to obtain light and produce energy.
- Claudio H. Slamovits
- , Noriko Okamoto
- & Patrick J. Keeling