Featured
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Article |
Exciton polaron formation and hot-carrier relaxation in rigid Dion–Jacobson-type two-dimensional perovskites
The detailed interplay between electronic and lattice dynamics in two-dimensional perovskite materials remains elusive. Here the authors establish the room-temperature polaronic nature of the excitons in two-dimensional Dion–Jacobson-type perovskites.
- Somnath Biswas
- , Ruyan Zhao
- & Gregory D. Scholes
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Article
| Open Access
Suppression of Dexter transfer by covalent encapsulation for efficient matrix-free narrowband deep blue hyperfluorescent OLEDs
Suppressed Dexter transfer is needed to achieve efficient and stable hyperfluorescence, but complex matrices must be involved. A molecular design strategy has been proposed where Dexter transfer can be substantially reduced by an encapsulated terminal emitter, leading to ‘matrix-free’ hyperfluorescence.
- Hwan-Hee Cho
- , Daniel G. Congrave
- & Hugo Bronstein
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Research Briefing |
Vibrational optical control via cation motions in perovskite solar cells
Hybrid organic–inorganic perovskite materials have promise as the photovoltaic technology of the future. A method for spectroscopic optical control reveals how the structural dynamics and vibrations of a perovskite’s organic cations affect the electronic performance of working photovoltaic devices.
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Research Briefing |
Mapping the transmission of single-molecule junctions using photoelectron tunnelling spectroscopy
The transmission spectrum of single-molecule junctions provides fingerprint information on the charge-transport properties. A technique called single-molecule photoelectron tunnelling spectroscopy has been developed that enables mapping of the transmission spectrum beyond the highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gap at room temperature and can be used to explore the energy-dependent charge transport through single-molecule junctions.
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Comment |
Revisiting point defects in ionic solids and semiconductors
The study of point defects in non-metallic crystals has become relevant for an increasing number of materials applications. Progress requires a foundation of consistent definitions and terminology. This Comment clarifies the underlying definitions of point defects, encourages the correct use of relative charge for their description and emphasizes their recognition as quasiparticles.
- Roger De Souza
- & George Harrington
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Letter
| Open Access
Probing lithium mobility at a solid electrolyte surface
Understanding lithium dynamics in solid-state electrolytes used for Li-ion batteries can be challenging. Using nonlinear extreme-ultraviolet spectroscopies, a direct spectral signature of surface lithium ions showing a distinct blueshift relative to the bulk absorption spectra is observed in a prototypical solid-state electrolyte.
- Clarisse Woodahl
- , Sasawat Jamnuch
- & Michael Zuerch
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Article |
Operando NMR electrochemical gating studies of ion dynamics in PEDOT:PSS
Understanding charge-compensating interactions and ionic dynamics in organic mixed conductors can be challenging. Operando NMR spectroscopy is now used to quantify cation and water movement during doping/dedoping in mixed conductor films.
- Dongxun Lyu
- , Yanting Jin
- & Clare P. Grey
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Article |
From enhanced diffusion to ultrafast ballistic motion of hybrid light–matter excitations
The authors study ultrafast spatiotemporal dynamics of polaritons formed by mixing surface-bound optical waves with excitons observing a mobility transition from diffusive to ballistic transport flow at two-thirds the speed of light.
- Mukundakumar Balasubrahmaniyam
- , Arie Simkhovich
- & Tal Schwartz
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Article |
Room-temperature logic-in-memory operations in single-metallofullerene devices
Single-molecule electronics provide the potential solution for high-density integration and low-power consumption in massive data-driven applications, but have yet to be explored. Here, the authors report low-power logic-in-memory operations, based on single electric dipole flipping in the two-terminal single-metallofullerene device at room temperature.
- Jing Li
- , Songjun Hou
- & Wenjing Hong
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Letter |
Solid–liquid–gas reaction accelerated by gas molecule tunnelling-like effect
Real-time imaging of accelerated solid–liquid–gas reactions with nanobubbles uncovers the mechanisms of enhanced triple-phase reactions by identifying the critical distance between solid and gas at the nanoscale.
- Wen Wang
- , Tao Xu
- & Litao Sun
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Article |
Organic long-persistent luminescence stimulated by visible light in p-type systems based on organic photoredox catalyst dopants
Organic blends based on cationic photoredox catalyst dopants in neutral donor hosts show p-type charge transport behaviour. This favours reduced reactivity to oxygen in organic long-persistent luminescence materials responsive to visible light.
- Kazuya Jinnai
- , Ryota Kabe
- & Chihaya Adachi
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Article |
Free energy difference to create the M-OH* intermediate of the oxygen evolution reaction by time-resolved optical spectroscopy
Theoretical descriptors differentiate catalytic activity for oxygen evolution reaction by the strength of oxygen binding in the reactive intermediate created upon electron transfer. Picosecond optical spectra of the Ti-OH* population on doped SrTiO3 are now shown to be ordered by surface hydroxylation.
- Ilya Vinogradov
- , Suryansh Singh
- & Tanja Cuk
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Article |
Extending insertion electrochemistry to soluble layered halides with superconcentrated electrolytes
Insertion compounds in layered oxide or sulfide electrodes provide the fundamental basis of current commercialized Li-ion batteries. The feasibility of reversibly intercalating Li+ electrochemically into halide compounds via the use of superconcentrated electrolytes is now demonstrated.
- Nicolas Dubouis
- , Thomas Marchandier
- & Alexis Grimaud
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Article |
Chirality-driven topological electronic structure of DNA-like materials
An orbital polarization effect is proposed to understand chiral-induced spin selectivity.
- Yizhou Liu
- , Jiewen Xiao
- & Binghai Yan
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Article |
Linking in situ charge accumulation to electronic structure in doped SrTiO3 reveals design principles for hydrogen-evolving photocatalysts
Understanding the origin of unprecedented solar-to-hydrogen efficiencies in doped SrTiO3 has proved challenging. Linking in situ charge accumulation to electronic structure in this system now reveals design principles for hydrogen-evolving photocatalysts.
- Benjamin Moss
- , Qian Wang
- & James R. Durrant
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Perspective |
Flow and extraction of energy and charge carriers in hybrid plasmonic nanostructures
Recent developments in the emerging field of hybrid plasmonics focusing on fundamental aspects related to nanoscopic flow of energy and excited charge carriers in these multicomponent materials and their potential applications are now discussed.
- Suljo Linic
- , Steven Chavez
- & Rachel Elias
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Article |
n-type charge transport in heavily p-doped polymers
A broad range of characterization techniques is used to understand the dominant electron conduction in various p-type doped π-conjugated polymers, which show p-type and n-type thermoelectric power factors depending on the dopant concentration.
- Zhiming Liang
- , Hyun Ho Choi
- & Kenneth R. Graham
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News & Views |
Framed by depletion
Colloidal structures and lattices made of patchy particles with chemically distinct lobes are formed by exploring site-specific depletion forces. This approach introduces a simple route to assemble colloidal superlattices.
- Bas G. P. van Ravensteijn
- , Patrick A. Hage
- & Ilja K. Voets
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Perspective |
The topology of electronic band structures
This Perspective provides a broad introduction to topological materials science, with a particular focus on semimetals.
- Prineha Narang
- , Christina A. C. Garcia
- & Claudia Felser
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News & Views |
No free lunch for non-fullerene acceptors
Non-fullerene acceptors have successfully overcome energy losses that were thought to be unavoidable in organic solar cells based on fullerene derivatives. However, it is now shown that they have limits too.
- Justin M. Hodgkiss
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Perspective |
Towards a better understanding of Lewis acidic aluminium in zeolites
Lewis acid aluminium sites in zeolites enable some industrially relevant catalytic reactions, such as biomass valorization. This Perspective explores the origin and interpretation of these species, and discusses characterization techniques that can close knowledge gaps.
- Manoj Ravi
- , Vitaly L. Sushkevich
- & Jeroen A. van Bokhoven
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Article |
Insight into the effects of confined hydrocarbon species on the lifetime of methanol conversion catalysts
The methanol-to-hydrocarbons reaction on zeolites produces olefins from many sources, but catalyst stability is a major challenge. Here, by combining operando measurements and simulations, the formation and identification of deactivating carbonaceous species throughout the reaction are achieved.
- I. Lezcano-Gonzalez
- , E. Campbell
- & A. M. Beale
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News & Views |
Ice goes fully cubic
Two independent studies describe the discovery of structurally pure cubic ice Ic made from either ice XVII or a high-pressure hydrogen hydrate.
- Christoph G. Salzmann
- & Benjamin J. Murray
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Article |
Engineering high-energy-density sodium battery anodes for improved cycling with superconcentrated ionic-liquid electrolytes
Non-uniform metal deposition and dendrite formation reduce the efficiency, safety and life of batteries with metal anodes. The influence of these factors in a sodium electrolyte now shows how a molten-salt-like structure at the electrode surface results in dendrite-free metal cycling at higher rates.
- Dmitrii A. Rakov
- , Fangfang Chen
- & Maria Forsyth
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Article |
Ground-state electron transfer in all-polymer donor–acceptor heterojunctions
Doping through spontaneous electron transfer between donor and acceptor polymers is obtained by selecting organic semiconductors with suitable electron affinity and ionization energy, achieving high conductivity in blends and bilayer configuration.
- Kai Xu
- , Hengda Sun
- & Simone Fabiano
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Article |
Molecular understanding of charge storage and charging dynamics in supercapacitors with MOF electrodes and ionic liquid electrolytes
The electrochemical performance of supercapacitors can be enhanced with porous electrodes. Molecular dynamics simulations can now help to clarify the double-layer structure and capacitive performance of supercapacitors composed of MOF electrodes and ionic liquid electrolytes.
- Sheng Bi
- , Harish Banda
- & Guang Feng
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Article |
Nanoscale percolation in doped BaZrO3 for high proton mobility
Although acceptor-doped barium zirconate is a promising conductor for electrolysers or fuel cells, our understanding of the relationship between proton motion and conductivity is limited. Our simulations now suggest a generic nanoscale percolation mechanism for high mobility in other oxides.
- Fabian M. Draber
- , Christiane Ader
- & Manfred Martin
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Article |
Imaging material functionality through three-dimensional nanoscale tracking of energy flow
A stroboscopic scattering microscopy approach is developed to image the evolution of carrier distributions in three dimensions and with sub-nanosecond resolution while the carriers propagate in organic and inorganic films.
- Milan Delor
- , Hannah L. Weaver
- & Naomi S. Ginsberg
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Article |
Critical role of intermediate electronic states for spin-flip processes in charge-transfer-type organic molecules with multiple donors and acceptors
Triplet excited states related to partial molecular structures are shown to mediate spin-flip between lowest singlet and triplet excited states in multiple donor–acceptor charge-transfer-type organic molecules.
- Hiroki Noda
- , Xian-Kai Chen
- & Chihaya Adachi
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Article |
Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces
Understanding molecular interactions between ionic liquids and interfaces is crucial for electrochemical device applications. Self-assembled amphiphilic nanostructures in surface-active ionic liquids are shown to exhibit enhanced charge storage at electrified surfaces.
- Xianwen Mao
- , Paul Brown
- & T. Alan Hatton
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Article |
A map of the inorganic ternary metal nitrides
High-throughput computation is especially useful for materials screening where synthesis is challenging. Here, it is used to construct a stability map of ternary nitrides, allowing discovery of stable compounds and providing insight into principles that govern nitride stability.
- Wenhao Sun
- , Christopher J. Bartel
- & Gerbrand Ceder
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Article |
Double doping of conjugated polymers with monomer molecular dopants
A monomer molecular dopant with high electron affinity is shown to accept up to two electrons from conjugated polymers with low ionization efficiency and then generate free charge carriers with an efficiency of up to 170%.
- David Kiefer
- , Renee Kroon
- & Christian Müller
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Article |
Addressing the isomer cataloguing problem for nanopores in two-dimensional materials
Nanopores in 2D materials have various possible lattice isomers, making relevant quantitative analysis difficult. An isomer-cataloguing framework is developed to address this problem, demonstrating remarkable agreement between simulated and experimental data.
- Ananth Govind Rajan
- , Kevin S. Silmore
- & Michael S. Strano
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Article |
A multicaloric cooling cycle that exploits thermal hysteresis
Magnetocaloric effects can be used for refrigeration, but application uptake is limited due to large amounts of magnetic material used. Here, a cooling cycle is shown that uses thermal hysteresis, significantly reducing magnetic material quantity.
- Tino Gottschall
- , Adrià Gràcia-Condal
- & Oliver Gutfleisch
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Letter |
Electrifying model catalysts for understanding electrocatalytic reactions in liquid electrolytes
Fundamental understanding of electrocatalysis is key to a transition to renewable energy systems. A strategy to ‘electrify’ complex oxide-based model catalysts is now proposed to explore electrocatalytic reactions in liquid electrolytes.
- Firas Faisal
- , Corinna Stumm
- & Jörg Libuda
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Article |
Continuous-wave infrared optical gain and amplified spontaneous emission at ultralow threshold by colloidal HgTe quantum dots
Stimulated emission under continuous-wave excitation from mercury telluride quantum dots at very low thresholds (compatible with electrical injection) is achieved by exploiting surface traps that render the quantum dots into four-level systems.
- Pieter Geiregat
- , Arjan J. Houtepen
- & Zeger Hens
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Article |
Liquid metal–organic frameworks
The structure and porosity of a zinc imidazolate framework above the melting point was studied with neutron and X-ray scattering, and molecular dynamics. The porosity and local bonding of the framework persist even in the liquid phase.
- Romain Gaillac
- , Pluton Pullumbi
- & François-Xavier Coudert
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Article |
Resolving ultrafast exciton migration in organic solids at the nanoscale
Time-resolved ultrafast spectroscopy is combined with stimulated emission depletion microscopy to observe exciton migration in conjugated polymer films with nanometre and picosecond resolution.
- Samuel B. Penwell
- , Lucas D. S. Ginsberg
- & Naomi S. Ginsberg
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Letter |
Strength of the repulsive part of the interatomic potential determines fragility in metallic liquids
Liquid fragility is a basic characteristic of glasses and there is debate as to what controls it. X-ray scattering of several metallic liquids now suggests that the strength of the repulsive part of the interatomic potential is key.
- Christopher E. Pueblo
- , Minhua Sun
- & K. F. Kelton
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Article |
Controlling the growth of multiple ordered heteromolecular phases by utilizing intermolecular repulsion
It is now shown that the phase of heteromolecular submonolayer films formed by adsorbates with opposite intermolecular interactions can be controlled by tuning the density of the gas phase of the species with repulsive character.
- Caroline Henneke
- , Janina Felter
- & Christian Kumpf
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Article |
Visualizing excitations at buried heterojunctions in organic semiconductor blends
A pump–push–probe time-resolved technique is developed to characterize the dynamics of photoexcitations at buried, disordered interfaces. Applied to organic bulk heterojunctions, the method provides insight on charge separation in photovoltaic films.
- Andreas C. Jakowetz
- , Marcus L. Böhm
- & Richard H. Friend
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Review Article |
Photovoltaic concepts inspired by coherence effects in photosynthetic systems
Lessons learned from coherent phenomena in biological photosynthetic systems may be useful to improve energy- and charge-transport in disordered materials. This Review describes coherence and its potential beneficial effects in photovoltaics.
- Jean-Luc Brédas
- , Edward H. Sargent
- & Gregory D. Scholes
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Article |
Direct–indirect character of the bandgap in methylammonium lead iodide perovskite
Time-resolved photo-conductance and microwave conductance investigations reveal that methylammonium lead iodide perovskites have an indirect bandgap at temperatures relevant to photovoltaic applications.
- Eline M. Hutter
- , María C. Gélvez-Rueda
- & Tom J. Savenije
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Article |
Facet-dependent trapping and dynamics of excess electrons at anatase TiO2 surfaces and aqueous interfaces
Excess electrons from intrinsic defects, dopants and photoexcitation play a key role in TiO2 properties. Simulations now predict that excess electrons depend on the exposed anatase surface, the environment and the character of the electron donor.
- Sencer Selcuk
- & Annabella Selloni
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Article |
Reconstructing solute-induced phase transformations within individual nanocrystals
The phase distribution of multiply twinned palladium nanocrystals causes spatially inhomogeneous hydrogen loading, which was imaged in situ.
- Tarun C. Narayan
- , Andrea Baldi
- & Jennifer A. Dionne
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Article |
Conductance saturation in a series of highly transmitting molecular junctions
The conductance of single-molecule junctions based on oligoacenes is shown to saturate when the molecule length increases. The saturation trend depends on the frontier orbitals of the metals used and on their hybridization with molecular π-orbitals.
- T. Yelin
- , R. Korytár
- & O. Tal
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Letter |
Counting electrons on supported nanoparticles
The electronic interaction between deposited metal nanoparticles and their support material can influence their functionality. Here, a quantification of the charge transfer between platinum nanoparticles and a ceria support is presented.
- Yaroslava Lykhach
- , Sergey M. Kozlov
- & Jörg Libuda
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Article |
Enhanced energy transport in genetically engineered excitonic networks
A super-Förster energy-transfer regime, where coherent and incoherent energy transport processes enhance the diffusion of excitons, is observed at room temperature by tuning the distance between the chromophores’ binding sites in a virus scaffold.
- Heechul Park
- , Nimrod Heldman
- & Angela M. Belcher
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News & Views |
Energy transfer is speeded up in 2D
When efficient energy transfer under high carrier densities is required, two-dimensional nanoplatelets are the material of choice, combining an exceptional suppression of nonlinear fluorescence quenching with ultrafast transfer capabilities.
- Iwan Moreels
Correlated electron–nuclear dynamics of photoinduced water dissociation on rutile TiO2