Featured
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Article |
Closed-loop transfer enables artificial intelligence to yield chemical knowledge
Integration of closed-loop experiments with physics-based feature selection and supervised learning, denoted as closed-loop transfer, yields chemical insights in parallel with optimization of objective functions.
- Nicholas H. Angello
- , David M. Friday
- & Nicholas E. Jackson
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Article |
Couple-close construction of polycyclic rings from diradicals
A couple-close approach used to build semisaturated ring systems from dual radical precursors allows sampling of regions of underexplored chemical space, leading to an annulation that can be used for late-stage functionalization of pharmaceutical scaffolds.
- Alice Long
- , Christian J. Oswood
- & David W. C. MacMillan
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Article |
Cryptochrome–Timeless structure reveals circadian clock timing mechanisms
Structural analysis of a protein complex in the circadian clock of Drosophila reveals how a light-sensing cryptochrome recognizes and engages its target.
- Changfan Lin
- , Shi Feng
- & Brian R. Crane
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Article
| Open Access
Orbital-resolved observation of singlet fission
Time- and angle-resolved photoemission spectroscopy is used to observe the primary step of singlet fission with orbital resolution indicating a charge-transfer mediated mechanism with a hybridization of states in the lowest bright singlet exciton.
- Alexander Neef
- , Samuel Beaulieu
- & Ralph Ernstorfer
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Article |
General access to cubanes as benzene bioisosteres
The synthesis of 1,3- and 1,2-disubstituted cubanes is achieved using a cyclobutadiene precursor and a photolytic carboxylation reaction, respectively, and copper-catalysed amination, arylation, alkylation and trifluoromethylation reactions have been developed enabling the use of cubanes as bioisosteres of benzenes in drug design.
- Mario P. Wiesenfeldt
- , James A. Rossi-Ashton
- & David W. C. MacMillan
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Article |
Photosynthesis re-wired on the pico-second timescale
By using in vivo ultrafast TA spectroscopy, extraction of electrons directly from photoexcited PSI and PSII in cyanobacterial cells using exogenous electron mediators is demonstrated.
- Tomi K. Baikie
- , Laura T. Wey
- & Jenny Z. Zhang
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Article
| Open Access
Ultrafast structural changes direct the first molecular events of vision
One picosecond after photoactivation, isomerized retinal pulls away from half of its numerous interactions with its binding pocket, and the excess of the photon energy is released through an anisotropic protein breathing motion in the direction of the extracellular space.
- Thomas Gruhl
- , Tobias Weinert
- & Valerie Panneels
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Article |
Electrophotocatalytic oxygenation of multiple adjacent C–H bonds
Installation of multiple C–O bonds by concurrent oxygenation of contiguous C–H bonds in a selective fashion is highly desirable, and this is achieved by repeated operation of a potent oxidative catalyst via electrophotocatalysis.
- Tao Shen
- , Yi-Lun Li
- & Tristan H. Lambert
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Article |
A designed photoenzyme for enantioselective [2+2] cycloadditions
A genetically encoded triplet photosensitizer is used to develop an efficient photoenzyme that can promote enantioselective intramolecular and bimolecular [2+2] cycloadditions by means of triplet energy transfer.
- Jonathan S. Trimble
- , Rebecca Crawshaw
- & Anthony P. Green
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Article |
Enantioselective [2+2]-cycloadditions with triplet photoenzymes
Triplet photoenzymes developed through genetic encoding and directed evolution result in excited-state photocatalysts that provide a valuable approach to enantioselective photochemical synthesis.
- Ningning Sun
- , Jianjian Huang
- & Yuzhou Wu
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Article |
Photoexcited nitroarenes for the oxidative cleavage of alkenes
Oxidative cleavage of alkenes is achieved using nitroarenes and light irradiation as an alternative to using ozone to break the carbon–carbon bonds, avoiding the explosive intermediates formed with ozone.
- Alessandro Ruffoni
- , Charlotte Hampton
- & Daniele Leonori
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Article |
RETRACTED ARTICLE: Intrinsically unidirectional chemically fuelled rotary molecular motors
A homochiral rotary molecular motor shows autonomous unidirectional rotation around a single bond driven by a chemical fuel.
- Ke Mo
- , Yu Zhang
- & Depeng Zhao
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Article |
Orbital-resolved visualization of single-molecule photocurrent channels
Atomic-level imaging of photocurrents in a single molecule is achieved by combining a tunable laser with scanning tunnelling microscopy, revealing how photons turn into electric current via a photoexcited molecule.
- Miyabi Imai-Imada
- , Hiroshi Imada
- & Yousoo Kim
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Article |
Direct observation of ultrafast hydrogen bond strengthening in liquid water
Liquid ultrafast electron scattering measures structural responses in liquid water with femtosecond temporal and atomic spatial resolution to reveal a transient hydrogen bond contraction then thermalization preceding relaxation of the OH stretch.
- Jie Yang
- , Riccardo Dettori
- & Xijie Wang
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Article |
Xolography for linear volumetric 3D printing
By combining the use of photoswitchable photoinitators and intersecting light beams, objects and complex systems can be produced rapidly with higher definition than is possible using state-of-the art macroscopic volumetric methods.
- Martin Regehly
- , Yves Garmshausen
- & Stefan Hecht
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Article |
Metallaphotoredox aryl and alkyl radiomethylation for PET ligand discovery
A versatile and rapid metallaphotoredox catalytic method of making 3H- and 11C-labelled tracer compounds for use in positron emission tomography (PET) is reported.
- Robert W. Pipal
- , Kenneth T. Stout
- & David W. C. MacMillan
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Article |
Leveraging excited-state coherence for synthetic control of ultrafast dynamics
Information from quantum coherence observations guides synthetic modifications of an iron-based chromophore, increasing the excited-state dynamics lifetime by a factor of 20, with implications for photo-induced electron-transfer applications.
- Bryan C. Paulus
- , Sara L. Adelman
- & James K. McCusker
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Article |
Photocatalytic water splitting with a quantum efficiency of almost unity
Water splitting with an internal quantum efficiency of almost unity is achieved using a modified semiconductor photocatalyst that selectively promotes the hydrogen and oxygen evolution reactions on separate crystal facets.
- Tsuyoshi Takata
- , Junzhe Jiang
- & Kazunari Domen
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Article |
Discovery and characterization of an acridine radical photoreductant
Photoexcited acridine radical catalysts are found to have redox potentials more reducing than lithium, which is attributed to the population of higher-energy doublet excited states via a twisted intramolecular charge-transfer species.
- Ian A. MacKenzie
- , Leifeng Wang
- & David A. Nicewicz
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Letter |
Catalytic deracemization of chiral allenes by sensitized excitation with visible light
Photochemical deracemization through irradiation with visible light in the presence of a chiral sensitizer enables the direct formation of single enantiomers from a racemic mixture of the same compound.
- Alena Hölzl-Hobmeier
- , Andreas Bauer
- & Thorsten Bach
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Letter |
Direct arylation of strong aliphatic C–H bonds
Direct coupling of aliphatic C–H nucleophiles to aryl electrophiles is described, through the combination of light-driven polyoxometalate hydrogen atom transfer and nickel catalysis.
- Ian B. Perry
- , Thomas F. Brewer
- & David W. C. MacMillan
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Letter |
Decarboxylative sp3 C–N coupling via dual copper and photoredox catalysis
The synergistic combination of copper catalysis and photoredox catalysis forms sp3 C–N bonds in a rapid, room-temperature coupling protocol with high efficiencies and regioselectivities and a broad substrate scope.
- Yufan Liang
- , Xiaheng Zhang
- & David W. C. MacMillan
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Letter |
Generating carbyne equivalents with photoredox catalysis
A photocatalytic strategy is described that generates diazomethyl radicals as direct equivalents of carbynes, which are often too reactive to use, enabling the functionalization of a range of medically useful compounds.
- Zhaofeng Wang
- , Ana G. Herraiz
- & Marcos G. Suero
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Review Article |
Enhancing the potential of enantioselective organocatalysis with light
This Review discusses recent developments in the combination of organocatalysis and photochemistry for the activation of molecules, which has enabled previously inaccessible reaction pathways and influenced many fields of chemical research.
- Mattia Silvi
- & Paolo Melchiorre
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Letter |
Visible-light-driven methane formation from CO2 with a molecular iron catalyst
An iron tetraphenylporphyrin complex is shown to catalyse the reduction of carbon dioxide to methane upon visible light irradiation at ambient temperature and pressure.
- Heng Rao
- , Luciana C. Schmidt
- & Marc Robert
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Letter |
Selective sp3 C–H alkylation via polarity-match-based cross-coupling
Using a triple catalytic approach, a selective sp3 C–H alkylation is demonstrated that is applicable in late-stage functionalization of pharmaceutical compounds.
- Chip Le
- , Yufan Liang
- & David W. C. MacMillan
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Letter |
The effect of illumination on the formation of metal halide perovskite films
Films of metal halide perovskite are used as the absorber material in solar cells, and light irradiation during their formation is shown to affect their crystallization, morphology and photovoltaic performance.
- Amita Ummadisingu
- , Ludmilla Steier
- & Michael Grätzel
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Letter |
A low-spin Fe(iii) complex with 100-ps ligand-to-metal charge transfer photoluminescence
An iron complex is described that exhibits photoluminescence at room temperature, opening the way to the use of iron-based materials as low-cost, non-toxic light emitters and photosensitizers.
- Pavel Chábera
- , Yizhu Liu
- & Kenneth Wärnmark
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Letter |
Catalytic alkylation of remote C–H bonds enabled by proton-coupled electron transfer
Catalytic alkylation of C–H bonds is achieved via homolysis of N–H bonds of N-alkyl amides through proton-coupled electron transfer.
- Gilbert J. Choi
- , Qilei Zhu
- & Robert R. Knowles
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Letter |
Real-space investigation of energy transfer in heterogeneous molecular dimers
Scanning tunnelling microscopy is shown to be effective for probing energy transfer in a molecular dimer with submolecular resolution in real space.
- Hiroshi Imada
- , Kuniyuki Miwa
- & Yousoo Kim
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Letter |
Photodissociation of ultracold diatomic strontium molecules with quantum state control
The photodissociation of 88Sr2 molecules is examined at ultracold temperatures with a high degree of control, and a wealth of quantum effects such as barrier tunnelling, matter—wave interference of reaction products and forbidden pathways are observed
- M. McDonald
- , B. H. McGuyer
- & T. Zelevinsky
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Letter |
Asymmetric catalytic formation of quaternary carbons by iminium ion trapping of radicals
A combination of photoredox and asymmetric organic catalysis enables enantioselective radical conjugate additions to β,β-disubstituted cyclic enones to construct quaternary carbon stereocentres with high fidelity.
- John J. Murphy
- , David Bastida
- & Paolo Melchiorre
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Letter |
Visualizing coherent intermolecular dipole–dipole coupling in real space
Luminescence induced by highly localized excitations that are produced by electrons tunnelling from the tip of a scanning tunnelling microscope is used to map the spatial distribution of the excitonic coupling in well-defined arrangements of a few zinc-phthalocyanine molecules and the dependence of this spatial distribution on the relative orientation and phase of the transition dipoles of the individual molecules.
- Yang Zhang
- , Yang Luo
- & J. G. Hou
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Letter |
Sub-particle reaction and photocurrent mapping to optimize catalyst-modified photoanodes
Using single-molecule fluorescence imaging of photoelectrocatalysis, the charge-carrier activities on single TiO2 nanorods and the corresponding water-oxidation photocurrent are mapped at high spatiotemporal resolution, revealing the best catalytic sites and the most effective sites for depositing an oxygen evolution catalyst.
- Justin B. Sambur
- , Tai-Yen Chen
- & Peng Chen
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Letter |
Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)5 in solution
Mapping the frontier-orbital interactions with atom specificity using X-ray laser-based femtosecond-resolution spectroscopy reveals that spin crossover and ligation determine the sub-picosecond excited-state dynamics of a transition-metal complex in solution.
- Ph. Wernet
- , K. Kunnus
- & A. Föhlisch
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Letter |
Efficient planar heterojunction perovskite solar cells by vapour deposition
The use of organometal halide perovskites as the light-absorbing material in nanostructured solar cells has increased efficiency to practical levels; here it is shown that vapour deposition of the perovskite removes the need for complex nanostructures and will hence simplify large-scale manufacture.
- Mingzhen Liu
- , Michael B. Johnston
- & Henry J. Snaith
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Letter |
The role of spin in the kinetic control of recombination in organic photovoltaics
The interplay of spin, energetics and delocalization of the electronic excitations are shown to create a spin blockade of electron–hole recombination in organic photovoltaic cells, resulting in high quantum efficiencies.
- Akshay Rao
- , Philip C. Y. Chow
- & Richard H. Friend
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Research Highlights |
Instant steam from sunlight
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Letter |
All-solid-state dye-sensitized solar cells with high efficiency
A solution-processable inorganic semiconductor is reported that can replace the liquid electrolyte of dye-sensitized solar cells, yielding all-solid-state solar cells with impressive energy conversion efficiencies.
- In Chung
- , Byunghong Lee
- & Mercouri G. Kanatzidis
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Letter |
Structure of full-length Drosophila cryptochrome
- Brian D. Zoltowski
- , Anand T. Vaidya
- & Brian R. Crane
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News |
Nanoparticle solar cells make light work
Cheap, printable photovoltaics might finally live up to their early promise.
- Philip Ball
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Letter |
Temperature-scan cryocrystallography reveals reaction intermediates in bacteriophytochrome
- Xiaojing Yang
- , Zhong Ren
- & Keith Moffat
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News |
Secrets of artificial leaf revealed
Sunlight falling on a catalyst-coated silicon wafer splits water into hydrogen and oxygen.
- Richard Van Noorden
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News Feature |
Physics of life: The dawn of quantum biology
The key to practical quantum computing and high-efficiency solar cells may lie in the messy green world outside the physics lab.
- Philip Ball
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Letter |
Single-molecule fluorescence reveals sequence-specific misfolding in multidomain proteins
- Madeleine B. Borgia
- , Alessandro Borgia
- & Jane Clarke
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News & Views |
Pull-down for single molecules
An innovative marriage of techniques, combining the principles of common protein pull-down assays with single-molecule fluorescence microscopy, opens up new ways of visualizing cellular protein complexes. See Article p.484
- Philip Tinnefeld
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Career Brief |
Boost for solar research
A US federal grant for photovoltaic research will create hundreds of academic and industrial jobs.
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News Feature |
Vision science: Seeing without seeing
There is more to the eye than rods and cones — the discovery of a third photoreceptor is rewriting the visual rulebook.
- Corie Lok
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News & Views |
Feel the light
How is light perceived? The answer that might immediately come to mind is, through the eyes. Fly larvae, however, can 'feel' light using specialized neurons embedded under the cuticle encasing their bodies. See Article p.921
- Paul A. Garrity
