Article 28 September 2024 | Open Access Tomography of entangling two-qubit logic operations in exchange-coupled donor electron spin qubits Donors spins in silicon are coherent, high-performance qubits, but scale-up has been challenging. Here the authors present the first experimental demonstration of exchange-based, entangling two qubit gates between electrons bound to 31P donors in Si. Holly G. Stemp, Serwan Asaad & Andrea Morello Article 27 September 2024 | Open Access Concurrent oxygen evolution reaction pathways revealed by high-speed compressive Raman imaging Advancing the oxygen evolution reaction understanding requires probing catalysts’ microscale dynamics in operando but is highly challenging. Here, authors use compressive Raman imaging to unravel the charge compensation pathways in a crystalline oxygen evolution catalyst, α-Li2IrO3. Raj Pandya, Florian Dorchies & Alexis Grimaud Article 27 September 2024 | Open Access Exploring the influence of cell configurations on Cu catalyst reconstruction during CO2 electroreduction The impact of cell configuration on Cu catalyst reconstruction is crucial for optimizing CO2 electroreduction to produce C2+ chemicals. Here, the authors shows that membrane electrode assembly cells uniquely alter Cu reconstructions compared to H-type cells, significantly affecting performance. Woong Choi, Younghyun Chae & Da Hye Won Article 27 September 2024 | Open Access Spontaneous formation of reactive redox radical species at the interface of gas diffusion electrode The gas diffusion electrode interface can boost chemical reactions, yet its microenvironment properties are largely unexplored. Here, the authors report the spontaneous generation of reactive redox radical species at the interface using Janus hydrophobic/hydrophilic porous carbon papers to feed gas. Ruijuan Zhao, Lei Li & Chunhua Cui Article 27 September 2024 | Open Access Construction of acenaphthylenes via C−H activation-based tandem penta- and hexaannulation reactions The synthesis of acenaphthylene-containing polycyclic aromatic hydrocarbons has traditionally required multiple sequential synthetic steps, limiting structural diversity. Herein, the authors present a tandem C−H penta- and hexaannulation reaction of aryl alkyl ketone with acetylenedicarboxylate. Jian Li, Tao Liu & Jingsong You Article 27 September 2024 | Open Access On-chip multifunctional metasurfaces with full-parametric multiplexed Jones matrix The authors demonstrate an on-chip metasurface based on supercell scheme to enable full modulation of Jones matrix. The direction-multiplexed functionality has been implemented by joint control of detour phase, geometric phase and propagation phase, unlocking two independent sets of Jones matrices. Jitao Ji, Jian Li & Tao Li Article 27 September 2024 | Open Access SO2F2 mediated click chemistry enables modular disulfide formation in diverse reaction media Disulfide bonds are widely found in nature and are prevalent in therapeutic contexts due to their dynamic nature. Here, the authors disclose a click chemistry protocol to convert thiols to disulfides using SO2F2, and show its application in aqueous contexts, in flow, and for polymerizations. Hengzhao Li, Mengqi Peng & Jie An Article 27 September 2024 | Open Access Fe-S dually modulated adsorbate evolution and lattice oxygen compatible mechanism for water oxidation The oxygen evolution reaction is crucial for energy conversion but faces challenges in catalyst optimization. Here, the authors present a dual-modulated NiFe oxyhydroxide (R-NiFeOOH@SO4) that enhances OER performance through optimized metal and lattice oxygen sites, achieving a compatible multi-mechanism. Xu Luo, Hongyu Zhao & Shichun Mu Article 27 September 2024 | Open Access The erosion of large primary atmospheres typically leaves behind substantial secondary atmospheres on temperate rocky planets Many rocky planets formed with large, H2-rich atmospheres. Here, the authors show that the loss of these primary atmospheres from temperate planets such as TRAPPIST-1e typically leaves behind secondary atmospheres and habitable surface conditions. Joshua Krissansen-Totton, Nicholas Wogan & Jonathan J. Fortney Article 27 September 2024 | Open Access Spatiotemporally modulated full-polarized light emission for multiplexed optical encryption Here the authors merge spatiotemporal modulation LED device, precise control and efficient polarization emission and programmable patterning/positioning using 3D printing demonstrating encryption in visible light communication (VLC) enabled by polarization state modulation. Jiawei Lv, Jeong Hyun Han & Ki Tae Nam Article 27 September 2024 | Open Access Enhancing the efficiency of high-order harmonics with two-color non-collinear wave mixing in silica High-order harmonic generation in solids could develop into a compact, coherent, short-wavelength source. This study shows that two-colour noncollinear wave mixing in silica significantly enhances HHG efficiency over single-color methods, offering a novel pathway for advancing all-solid XUV sources. Sylvianne D. C. Roscam Abbing, Nataliia Kuzkova & Peter M. Kraus Article 27 September 2024 | Open Access Selective regulation of macrophage lipid metabolism via nanomaterials’ surface chemistry There is a need to understand how nanomaterials interact with biological systems. Here, the authors report the surface chemistry of graphene oxide nanosheets (GOs) influences the structure of low-density lipoprotein and changes lipid metabolism pathways including LDL recognition, uptake, hydrolysis, efflux, and lipid droplet formation. Junguang Wu, Xuan Bai & Liming Wang Article 27 September 2024 | Open Access Artificial olfactory memory system based on conductive metal-organic frameworks A chemical infrastructure for integrating sensing and memory and exhibiting short- and long-term memory responses to alcohols and aldehydes through an artificial olfactory memory system is realized with conductive metal-organic framework Ce-HHTP. Xiaomeng Yin, Hao Zhang & Tie Wang Article 27 September 2024 | Open Access Molecular switching by proton-coupled electron transport drives giant negative differential resistance It is a challenge to develop molecular switches with time-dependent probabilities. Here, the authors present a molecular switch based on proton-coupled electron transfer reaction with demonstration of dynamical and environment-specific modulation of giant negative differential resistance and memory effects. Qian Zhang, Yulong Wang & Christian A. Nijhuis Article 27 September 2024 | Open Access Integrating redox-electrodialysis and electrosorption for the removal of ultra-short- to long-chain PFAS PFAS remediation is challenging due to their diverse chain lengths, complicating water treatment. Here, the authors present an electrochemical approach for the removal of ultra-short to long-chain PFAS in a single process by integrating redox-electrodialysis and electrosorption. Nayeong Kim, Johannes Elbert & Xiao Su Article 27 September 2024 | Open Access Designing water resistant high entropy oxide materials Zhang et al. report an entropy engineering approach to design water-resistant oxide catalysts, (Ni0.2Mg0.2Cu0.2Zn0.2Co0.2)Cr2O4. This material shows excellent water resistance (>100 h) for C3H6 oxidation while other binary oxides deactivate within 20 h. Mengyuan Zhang, Ying Gao & Sheng Dai Article 27 September 2024 | Open Access Main-group element-boosted oxygen electrocatalysis of Cu-N-C sites for zinc-air battery with cycling over 5000 h Balancing the activity and stability of oxygen electrocatalysts is challenging but crucial for rechargeable zinc-air batteries. Here, the authors report a highly active Cu-N-C catalyst boosted by the main-group element for zinc-air battery with a long cycle stability over 5000 h. Yifan Li, Aijian Huang & Ruitao Lv Article 27 September 2024 | Open Access Graphene-enabled laser lift-off for ultrathin displays Laser lift-off (LLO) is a widely utilized process in the manufacturing of flexible electronics, but its application to ultrathin polymeric films can be challenging. Here, the authors report a graphene-enabled LLO method to improve the processability of few-micron-thick polyimide films and organic light-emitting diodes without compromising their quality. Sumin Kang, Jaehyeock Chang & Seungman Kim Article 27 September 2024 | Open Access Optically accessible long-lived electronic biexcitons at room temperature in strongly coupled H- aggregates When excitons in light-harvesting materials meet, they recombine and dissipate their energy. Here, the authors show that pairs of excitons can co-exist in aggregated materials and only annihilate when the aggregates are chemically connected. Siddhartha Sohoni, Indranil Ghosh & Gregory S. Engel Article 27 September 2024 | Open Access A hypergraph model shows the carbon reduction potential of effective space use in housing In this work, authors report a method to describe, evaluate and generate floor plans using hypergraphs. With it, it is shown how spatial efficiency has larger energy saving potential than traditional building upgrade measures and how autogenerated floor plans can increase comfort and building performance. Ramon Elias Weber, Caitlin Mueller & Christoph Reinhart Article 27 September 2024 | Open Access Birdlike broadband neuromorphic visual sensor arrays for fusion imaging Traditional silicon vision chips often challenge in emulating complex biological behaviors. This work reports birdlike broadband neuromorphic visual sensor arrays with 5 bits of in-memory sensing and computing. The built reservoir computing system achieves motion and UV grayscale information extraction, leading to fusion visual imaging. Pengshan Xie, Yunchao Xu & Johnny C. Ho Article 27 September 2024 | Open Access Hydroxylated TiO2-induced high-density Ni clusters for breaking the activity-selectivity trade-off of CO2 hydrogenation Here, the authors report a Ni(cluster)/TiO2 catalyst with strong interactions between Ni and −OH strong to promote CO2 activation with CO adsorption to avoid the activity-selectivity trade-off of the reverse water gas shift reaction. Cong-Xiao Wang, Hao-Xin Liu & Chun-Jiang Jia Article 27 September 2024 | Open Access Robust palladium oxide nano-cluster catalysts using atomic ions and strong interactions for high-performance methane oxidation Optimizing metal catalyst structures to achieve specific states is crucial for efficient surface reactions but remains difficult due to the absence of well-defined precursor materials and weak metal-support interactions. Here the authors design Pd oxide nanoclusters on SSZ-13 as optimal catalysts for complete CH4 oxidation, leveraging atomic ions and strong interactions. Seung-Hee Ryu, Seungeun Kim & Hojin Jeong Article 27 September 2024 | Open Access Predicting the heat release variability of Li-ion cells under thermal runaway with few or no calorimetry data Characterizing the variation in thermal behavior of Li-ion cells during thermal runaway is time-consuming and expensive. Here, authors show that by training a machine learning model on open-access data, the thermal behavior of a Li-ion cell can be predicted with high accuracy using the specifications of the cell and the ejected mass. Karina Masalkovaitė, Paul Gasper & Donal P. Finegan Article 27 September 2024 | Open Access Thermal runaway prevention through scalable fabrication of safety reinforced layer in practical Li-ion batteries The authors present a scalable method for implementing a thermo-responsive safety reinforced layer (SRL) in batteries, which enables immediate shutdown during internal short circuits and reduces the risk of overheating and explosions. In Taek Song, Joonkoo Kang & Kihwan Kim Article 27 September 2024 | Open Access Latent porosity of planar tris(phenylisoxazolyl)benzene Selective encapsulation of molecules within macrocyclic hosts relies on the pore features and nonmacrocyclic crystals for selective molecular encapsulation have yet been challenging. Here, the authors show that planar tris(phenylisoxazolyl)benzene exhibits a porosity without pore behavior and selectively encapsulate cis- over trans-decalin. Yudai Ono, Takehiro Hirao & Takeharu Haino Article 27 September 2024 | Open Access Facile enantioselective synthesis of multi-substituted norbornanes/norbornenes using a latent synthon strategy The development of a new catalytic asymmetric synthetic methodology is of topic of interest. Herein, the authors report a latent synthon strategy, which has been used in the synthesis of a wide range of optically enriched norbornanes with great structural diversity. Zi-An Shen, Jiami Guo & Yixin Lu Article 27 September 2024 | Open Access Exploring the programmability of autocatalytic chemical reaction networks Networks of chemical reactions exhibit emergent properties under out-of-equilibrium conditions and can be utilized to emulate properties important for neuromorphic computing. Here, the authors report a strategy that uses metal ions (Ca2+, La3+, and Nd3+) to control the rate of a trypsin catalysed autocatalytic reaction network, with temporal and history dependent outputs that can be mapped onto a variety of mathematical functions. Dmitrii V. Kriukov, Jurriaan Huskens & Albert S. Y. Wong Article 27 September 2024 | Open Access Metasurface-enabled broadband multidimensional photodetectors The detection of light intensity, polarization, and spectral information with a single device is desired for efficient optical sensing and computing applications. Here, the authors report the realization of metasurface-assisted graphene photodetectors able to simultaneously detect polarization states and wavelengths of broadband infrared light. Hao Jiang, Yinzhu Chen & Weibo Gao Article 27 September 2024 | Open Access Unlocking high photosensitivity direct laser writing and observing atomic clustering in glass Ag clusters dispersed in glass are critical for optical storage media. The authors present fluorine-modified glass with high Ag+ ion solubility, enhancing the formation of Ag clusters under low-energy laser irradiation. The inert network effectively confines Ag clusters uniformly within the glass. Wenyan Zheng, Zhuo Wang & Xianping Fan Article 27 September 2024 | Open Access Agile perching maneuvers in birds and morphing-wing drones Birds’ agile perching maneuvers allow large energy dissipation in short approach flights. Here, authors test an objective that birds are hypothesized to employ in perching maneuvers on an avian-inspired drone and find that it mimics the birds’ behavior, enabling exploration of key morphing actuations. Valentin Wüest, Simon Jeger & Dario Floreano Article 27 September 2024 | Open Access The role of water mobility on water-responsive actuation of silk Water-responsive materials with deformations on humidity changes are potentially useful as actuators, but prediction of stress is challenging. Here, the authors show that nanoconfinement of water is important in determining actuation behaviour in silk materials. Darjan Podbevšek, Yeojin Jung & Xi Chen Article 27 September 2024 | Open Access Pressure-constrained sonication activation of flexible printed metal circuit It is challenging to activate the flexible printed metal circuit to approach the intrinsic conductivity with minimal damage to the substrate. Here, the authors report a large-scale pressure-constrained sonication activation method for various metals and non-metallic inks. Lingxiao Cao, Zhonghao Wang & Zhizhu He Article 27 September 2024 | Open Access Deviceization of high-performance and flexible Ag2Se films for electronic skin and servo rotation angle control The authors design a flexible Ag2Se-based thermoelectric device with optimized electrode materials, structure, and selenization time, capable of various applications including rapid response to human motion signals as electronic skin. Yue-Xing Chen, Xiao-Lei Shi & Zhi-Gang Chen Article 27 September 2024 | Open Access Stereoselective rhodium-catalyzed reaction of allenes with organoboronic reagents for diversified branched 1,3-alkadienes The isoprene unit is widely found in bioactive molecules, but stereoselective synthetic methods for these 1,3-dienes remain limited. Here, the authors disclose an E-selective rhodium-catalyzed synthesis of terminal isoprene units from allenes. Weiyi Wang, Shichao Hong & Shengming Ma Article 27 September 2024 | Open Access Deep learning prediction of electrospray ionization tandem mass spectra of chemically derived molecules Chemical derivatization is widely used, but the lack of reference spectra of chemically derived molecules (CDMs) hinders their identification. Here, the authors describe a deep learning approach enabling accurate prediction of ESIMS/MS spectra for CDMs. Bin Chen, Hailiang Li & Feng Li Article 27 September 2024 | Open Access Probing the alkylidene carbene–strained alkyne equilibrium in polycyclic systems via the Fritsch–Buttenberg–Wiechell rearrangement The generation and observation of strained cyclic alkynes is of fundamental importance to organic chemistry, as the deviations from ideal bond angles further our understanding of reactivity and stability. Here, the authors generate and trap three polycyclic strained carbocyclic compounds through the Fritsch–Buttenberg–Wiechell rearrangement, and discuss the trapped species in the context of computational investigations of the reaction coordinates. T. E. Anderson, Dasan M. Thamattoor & David Lee Phillips Article 27 September 2024 | Open Access Doping strategy in metavalently bonded materials for advancing thermoelectric performance The authors find chemical bonding mechanisms play a key role in tailoring the solubility of dopants and improving the thermoelectric performance of metavalently bonded materials. Ming Liu, Muchun Guo & Jiehe Sui Article 27 September 2024 | Open Access Electrically switchable 2N-channel wave-front control for certain functionalities with N cascaded polarization-dependent metasurfaces The authors proposed to cascade N polarization-multiplexed metasurfaces for 2N electrically switchable channels without intrinsic loss or cross-talk. A 3-layer setup with 8 channels for beam steering and orbital angular momentum (OAM) generation is demonstrated. Zhiyao Ma, Tian Tian & Yidong Huang Article 27 September 2024 | Open Access Catalytic undirected methylation of unactivated C(sp3)−H bonds suitable for complex molecules The addition of a methyl group to drug candidates can confer significant improvement in the potency of the molecule, to the degree that late-stage addition of a CH3 group is a valuable line of inquiry in chemical synthesis. Here, the authors present an undirected methylation of C(sp3)−H bonds, using a nickel catalyst and iridium photosensitizer. Jin-Fay Tan, Yi Cheng Kang & John F. Hartwig Article 27 September 2024 | Open Access Lone-pair activated ferroelectricity and stable charged domain wall in Bi monolayer In most ferroelectric materials, the domain walls are of neutral type due to the high electrostatic energy cost for charged domain walls. Here, the authors observe abundant charged 180° domain walls in elemental ferroelectric Bi monolayer. Shulin Zhong, Xuanlin Zhang & Yunhao Lu Article 27 September 2024 | Open Access Halogenated-edge polymeric semiconductor for efficient spin transport The spin transport mechanism remains unclear for organic semiconductors. Here, authors investigate the effect of halogen substitution in bay-annulated indigo-based polymers and reveal the distance of substitution site from conjugated center and nitrogen atoms play crucial roles in spin relaxation. Xueli Yang, Ankang Guo & Yunlong Guo Article 27 September 2024 | Open Access Fluoropolymer sorbent for efficient and selective capturing of per- and polyfluorinated compounds It is challenging to remove Per- and polyfluoroalkyl substances (PFAS) from water. Here, authors developed a polymer sorbent capable of selectively and efficiently removing PFAS from contaminated water sources to levels below detection limits. Zhuojing Yang, Yutong Zhu & Cheng Zhang Article 27 September 2024 | Open Access Cooperative chemoenzymatic and biocatalytic cascades to access chiral sulfur compounds bearing C(sp3)–S stereocentres Biocatalysis has been widely employed for the generation of carbon-carbon/heteroatom stereocenters, yet its application in chiral C(sp3)–S bond construction is rare. Herein, the authors describe the enantioselective construction of chiral C(sp3)–S bonds through ene-reductase biocatalysed conjugate reduction of prochiral vinyl sulfides. Fei Zhao, Ariane Mattana & Daniele Castagnolo Article 27 September 2024 | Open Access Computer-aided drug design to generate a unique antibiotic family Holo-acyl carrier protein synthase (AcpS) is an enzyme that catalyses the first step in lipid synthesis and is essential for bacterial survival, but no current antibiotics targeting AcpS are known. Here, the authors use computer-aided drug design to develop a structurally unique antibiotic family targeting AcpS. Christopher J. Barden, Fan Wu & Christopher R. McMaster Article 27 September 2024 | Open Access High power density redox-mediated Shewanella microbial flow fuel cells Exoelectrogenic microorganisms provide a sustainable approach for power generation and wastewater treatment. Here the authors report a redox-mediated microbial flow fuel cell, realizing efficient electron/mass transport and high power output. Leyuan Zhang, Yucheng Zhang & Xiangfeng Duan Article 27 September 2024 | Open Access Universal correlation between H-linear magnetoresistance and T-linear resistivity in high-temperature superconductors Understanding “strange metal" behavior in high-temperature superconductors remains an open problem. Here the authors report a correlation between linear-in-magnetic-field magnetoresistance and linear-in-temperature resistivity in several hole-doped cuprate families and discuss its possible implications for superconductivity. J. Ayres, M. Berben & N. E. Hussey Article 27 September 2024 | Open Access Rapid context inference in a thalamocortical model using recurrent neural networks The neural mechanism responsible for context inference remains unknown. Here, the authors show that a PFC-MD neural network with a Hebbian plasticity rule achieves rapid online context inference and alleviates catastrophic forgetting. Wei-Long Zheng, Zhongxuan Wu & Michael M. Halassa Article 27 September 2024 | Open Access Sprayable anti-adhesive hydrogel for peritoneal macrophage scavenging in post-surgical applications Despite advances in adhesion barriers, challenges like off-targeting and handling issues persist. Here, authors report a sprayable adhesion barrier that quickly covers large areas, preventing postsurgical adhesions by scavenging peritoneal macrophages and exerting anti-inflammatory effects. Wonmoon Song, Changyub Lee & Nathaniel S. Hwang Article 27 September 2024 | Open Access Widespread biochemical reaction networks enable Turing patterns without imposed feedback The Turing pattern is crucial for self-organisation in biology, but the search for its mechanisms is often limited to feedback loop intuition derived from minimal systems. Here, authors show that Turing patterns can arise from widespread binding-based reactions without explicit feedback loops. Shibashis Paul, Joy Adetunji & Tian Hong