Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes.

Despite extensive studies, many questions remain about what structural and energetic factors give rise to the remarkable energy transport efficiency of photosynthetic light-harvesting protein complexes, owing largely to the inability to synthetically control such factors in these natural systems. Herein, we demonstrate energy transfer within a biomimetic light-harvesting complex consisting of identical chromophores attached in a circular array to a protein scaffold derived from the tobacco mosaic virus coat protein. We confirm the capability of energy transport by observing ultrafast depolarization in transient absorption anisotropy measurements and a redshift in time-resolved emission spectra in these complexes.

From an antiferromagnetic insulator to a strongly correlated metal in square-lattice MCl(pyrazine) coordination solids.

Electronic synergy between metal ions and organic linkers is a key to engineering molecule-based materials with a high electrical conductivity and, ultimately, metallicity. To enhance conductivity in metal-organic solids, chemists aim to bring the electrochemical potentials of the constituent metal ions and bridging organic ligands closer in a quest to obtain metal-d and ligand-π admixed frontier bands. Herein, we demonstrate the critical role of the metal ion in tuning the electronic ground state of such materials.

Programmable Fabrication of Monodisperse Graphene Nanoribbons via Deterministic Iterative Synthesis.

While enormous progress has been achieved in synthesizing atomically precise graphene nanoribbons (GNRs), the preparation of GNRs with a fully predetermined length and monomer sequence remains an unmet challenge. Here, we report a fabrication method that provides access to structurally diverse and monodisperse "designer" GNRs through utilization of an iterative synthesis strategy, in which a single monomer is incorporated into an oligomer chain during each chemical cycle. Surface-assisted cyclodehydrogenation is subsequently employed to generate the final nanoribbons, and bond-resolved scanning tunneling microscopy is utilized to characterize them.

Measurement of the specific and non-specific binding energies of Mg to RNA.

Determining the non-specific and specific electrostatic contributions of magnesium binding to RNA is a challenging problem. We introduce a single-molecule method based on measuring the folding energy of a native RNA in magnesium and at its equivalent sodium concentration. The latter is defined so that the folding energy in sodium equals the non-specific electrostatic contribution in magnesium.

Zinc Titanium Nitride Semiconductor toward Durable Photoelectrochemical Applications.

Photoelectrochemical fuel generation is a promising route to sustainable liquid fuels produced from water and captured carbon dioxide with sunlight as the energy input. Development of these technologies requires photoelectrode materials that are both photocatalytically active and operationally stable in harsh oxidative and/or reductive electrochemical environments. Such photocatalysts can be discovered based on co-design principles, wherein design for stability is based on the propensity for the photocatalyst to self-passivate under operating conditions and design for photoactivity is based on the ability to integrate the photocatalyst with established semiconductor substrates.

Kirigami Engineering of Suspended Graphene Transducers.

The low mass density and high mechanical strength of graphene make it an attractive candidate for suspended-membrane energy transducers. Typically, the membrane size dictates the operational frequency and bandwidth. However, in many cases it would be desirable to both lower the resonance frequency and increase the bandwidth, while maintaining overall membrane size.

Photosynthetic biohybrid coculture for tandem and tunable CO and N fixation.

Solar-driven bioelectrosynthesis represents a promising approach for converting abundant resources into value-added chemicals with renewable energy. Microorganisms powered by electrochemical reducing equivalents assimilate CO, HO, and N building blocks. However, products from autotrophic whole-cell biocatalysts are limited.

Beam-driven Dynamics of Aluminium Dopants in Graphene.

Substituting heteroatoms into graphene can tune its properties for applications ranging from catalysis to spintronics. The further recent discovery that covalent impurities in graphene can be manipulated at atomic precision using a focused electron beam may open avenues towards sub-nanometer device architectures. However, the preparation of clean samples with a high density of dopants is still very challenging.

Response to Comment on "Reversible disorder-order transitions in atomic crystal nucleation".

Yu . suggested calculating precisely the size ranges of the three parts of our figure 3A, adjusting the free-energy levels in figure 3B, and considering the shape effect in the first-principles calculation. The first and second suggestions raise strong concerns for misinterpretation and overinterpretation of our experiments.

Room-temperature skyrmion lattice in a layered magnet (FeCo)GeTe.

Novel magnetic ground states have been stabilized in two-dimensional (2D) magnets such as skyrmions, with the potential next-generation information technology. Here, we report the experimental observation of a Néel-type skyrmion lattice at room temperature in a single-phase, layered 2D magnet, specifically a 50% Co-doped FeGeTe (FCGT) system. The thickness-dependent magnetic domain size follows Kittel's law.

Spectroscopy signatures of electron correlations in a trilayer graphene/hBN moiré superlattice.

ABC-stacked trilayer graphene/hexagonal boron nitride moiré superlattice (TLG/hBN) has emerged as a playground for correlated electron physics. We report spectroscopy measurements of dual-gated TLG/hBN using Fourier transform infrared photocurrent spectroscopy. We observed a strong optical transition between moiré minibands that narrows continuously as a bandgap is opened by gating, indicating a reduction of the single-particle bandwidth.

Targeting One- and Two-Dimensional Ta-Te Structures via Nanotube Encapsulation.

Fine control over material synthesis on the nanoscale can facilitate the stabilization of competing crystalline structures. Here, we demonstrate how carbon nanotube reaction vessels can be used to selectively create one-dimensional TaTe chains or two-dimensional TaTe nanoribbons with exquisite control of the chain number or nanoribbon thickness and width. Transmission electron microscopy and scanning transmission electron microscopy reveal the detailed atomic structure of the encapsulated materials.

Density of states prediction for materials discovery via contrastive learning from probabilistic embeddings.

Machine learning for materials discovery has largely focused on predicting an individual scalar rather than multiple related properties, where spectral properties are an important example. Fundamental spectral properties include the phonon density of states (phDOS) and the electronic density of states (eDOS), which individually or collectively are the origins of a breadth of materials observables and functions. Building upon the success of graph attention networks for encoding crystalline materials, we introduce a probabilistic embedding generator specifically tailored to the prediction of spectral properties.

Large-gap insulating dimer ground state in monolayer IrTe.

Monolayers of two-dimensional van der Waals materials exhibit novel electronic phases distinct from their bulk due to the symmetry breaking and reduced screening in the absence of the interlayer coupling. In this work, we combine angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy to demonstrate the emergence of a unique insulating 2 × 1 dimer ground state in monolayer 1T-IrTe that has a large band gap in contrast to the metallic bilayer-to-bulk forms of this material. First-principles calculations reveal that phonon and charge instabilities as well as local bond formation collectively enhance and stabilize a charge-ordered ground state.

Direct Evaluation of Rare Events in Active Matter from Variational Path Sampling.

Active matter represents a broad class of systems that evolve far from equilibrium due to the local injection of energy. Like their passive analogs, transformations between distinct metastable states in active matter proceed through rare fluctuations; however, their detailed balance violating dynamics renders these events difficult to study. Here, we present a simulation method for evaluating the rate and mechanism of rare events in generic nonequilibrium systems and apply it to study the conformational changes of a passive solute in an active fluid.

Tunable Orbital Ferromagnetism at Noninteger Filling of a Moiré Superlattice.

The flat bands resulting from moiré superlattices exhibit fascinating correlated electron phenomena such as correlated insulators, ( 2018, 556 (7699), 80-84), ( 2019, 15 (3), 237) superconductivity, ( 2018, 556 (7699), 43-50), ( 2019, 572 (7768), 215-219) and orbital magnetism. ( 2019, 365 (6453), 605-608), ( 2020, 579 (7797), 56-61), ( 2020, 367 (6480), 900-903) Such magnetism has been observed only at particular integer multiples of , the density corresponding to one electron per moiré superlattice unit cell. Here, we report the experimental observation of ferromagnetism at noninteger filling (NIF) of a flat Chern band in a ABC-TLG/hBN moiré superlattice.

Pseudo-atomic orbital behavior in graphene nanoribbons with four-membered rings.

The incorporation of nonhexagonal rings into graphene nanoribbons (GNRs) is an effective strategy for engineering localized electronic states, bandgaps, and magnetic properties. Here, we demonstrate the successful synthesis of nanoribbons having four-membered ring (cyclobutadienoid) linkages by using an on-surface synthesis approach involving direct contact transfer of coronene-type precursors followed by thermally assisted [2 + 2] cycloaddition. The resulting coronene-cyclobutadienoid nanoribbons feature a narrow 600-meV bandgap and novel electronic frontier states that can be interpreted as linear chains of effective p and p pseudo-atomic orbitals.

Spin-dependent vibronic response of a carbon radical ion in two-dimensional WS.

Atomic spin centers in 2D materials are a highly anticipated building block for quantum technologies. Here, we demonstrate the creation of an effective spin-1/2 system via the atomically controlled generation of magnetic carbon radical ions (CRIs) in synthetic two-dimensional transition metal dichalcogenides. Hydrogenated carbon impurities located at chalcogen sites introduced by chemical doping are activated with atomic precision by hydrogen depassivation using a scanning probe tip.

Rationally Designed Topological Quantum Dots in Bottom-Up Graphene Nanoribbons.

Bottom-up graphene nanoribbons (GNRs) have recently been shown to host nontrivial topological phases. Here, we report the fabrication and characterization of deterministic GNR quantum dots whose orbital character is defined by zero-mode states arising from nontrivial topological interfaces. Topological control was achieved through the synthesis and on-surface assembly of three distinct molecular precursors designed to exhibit structurally derived topological electronic states.