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| Open AccessCrystallization of molecular layers produced under confinement onto a surface
Molecules arranged in close proximity to a surface form molecular layers, exhibiting distinct properties. However, the creation of these layers is challenging. Here, the authors present a technique for generating molecular layers through crystallization induced by gas blowing onto a surface.
- Jincheng Tong
- , Nathan de Bruyn
- & Cinzia Casiraghi
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Article
| Open AccessObserving growth and interfacial dynamics of nanocrystalline ice in thin amorphous ice films
In-situ cryo-electron microscopy in thin amorphous ice films and ice-dynamics simulations reveal polymorph-dependent growth kinetics of nanoscale ice crystals. Hetero-crystalline ice exhibits anisotropic growth: fast-growing facets are associated with low-density interfaces, driving tetrahedral ordering of interfacial H2O molecules and accelerating ice growth.
- Minyoung Lee
- , Sang Yup Lee
- & Dong June Ahn
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| Open AccessSite-selective chemical reactions by on-water surface sequential assembly
Controlling site-selectivity and reactivity in chemical reactions continues to be a key challenge in modern synthetic chemistry. Here, the authors demonstrate the assembly of amino-substituted porphyrins on a water surface into J-aggregate structures in the presence of charged surfactants.
- Anupam Prasoon
- , Xiaoqing Yu
- & Xinliang Feng
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Article
| Open AccessPorphene and porphite as porphyrin analogs of graphene and graphite
Here the authors report Zn porphene, a member of a new organic metalloporphene family. Similar to graphene, these also are fully conjugated 2D polymers, but are composed of fused metalloporphyrin rings.
- Thomas F. Magnera
- , Paul I. Dron
- & Josef Michl
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| Open AccessExtending on-surface synthesis from 2D to 3D by cycloaddition with C60
On-surface synthesis (OSS) defines a special opportunity to investigate intermolecular coupling at. sub-molecular level and has delivered many appealing polymers but so-far OSS is limited to the. lateral covalent bonding of molecular precursors. Here, the authors demonstrate cycloaddition. between C60 and an aromatic compound allowing covalent coupling perpendicular to the surface and multiple non-planar covalent coupling of C60.
- Pengcheng Ding
- , Shaoshan Wang
- & Miao Yu
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| Open AccessEnzymatic polymerization of enantiomeric L−3,4-dihydroxyphenylalanine into films with enhanced rigidity and stability
L-3,4-Dihydroxyphenylalanine plays an important role in living system. Here, the authors investigated the effect of the molecular chirality of L-3,4-dihydroxyphenylalanine on the improved structural and thermal stability of self-assembled films by tyrosinase-induced oxidative polymerization.
- Yuhe Shen
- , Rongxin Su
- & Wei Qi
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Article
| Open AccessCondensation and asymmetric amplification of chirality in achiral molecules adsorbed on an achiral surface
The origin of homochirality in nature is an important but open question. Here, the authors provide insight into the physicochemical origin of homochirality through surface adsorption on the model of adlayers of achiral carbon monoxide molecules on an achiral Au(111) surface.
- Huiru Liu
- , Heping Li
- & Lan Chen
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Article
| Open AccessSwitchable biomimetic nanochannels for on-demand SO2 detection by light-controlled photochromism
Conventional nanochannel sensors are passively responsive and may be slowly damaged by analytes present in the environment before detection. Here, authors developed a light-controlled inert/active-switchable biomimetic nanochannel sensor to achieve SO2 on-demand detection and long-term preservation.
- Dan Zhang
- , Yongjie Sun
- & Xuanjun Zhang
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Article
| Open AccessSteering carbon dioxide reduction toward C–C coupling using copper electrodes modified with porous molecular films
This study explores how the activity and selectivity of Cu electrodes for CO2 reduction can be tuned with organic films of different porosity and thickness. As a result, the films increase the local CO partial pressures and surface coverages.
- Siqi Zhao
- , Oliver Christensen
- & Kim Daasbjerg
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Article
| Open AccessDirect observation of long-range chirality transfer in a self-assembled supramolecular monolayer at interface in situ
Unravelling the mechanism of chirality transfer in supramolecular assemblies is important to understand the relationship between molecular chirality and supramolecular chirality. Here, the authors use nonlinear spectroscopy and molecular dynamic simulations to study the long-range chirality transfer in a self-assembled supramolecular system.
- Yuening Zhang
- , Xujin Qin
- & Zhen Zhang
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Article
| Open AccessJanus regulation of ice growth by hyperbranched polyglycerols generating dynamic hydrogen bonding
Regulation of ice growth and ice growth inhibition are critical and different materials mimicking anti freeze proteins or ice binding surfaces have been developed. Here, the authors combine both concepts in a hyperbranched polyglycerols to change the ice growth activity.
- Sang Yup Lee
- , Minseong Kim
- & Dong June Ahn
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Article
| Open AccessPhotodimerization induced hierarchical and asymmetric iontronic micropatterns
Hierarchical surface micro/nanopatterns enable iontronic materials to show performance enhancement in piezoionic mechanoreception and skin-interfaced coupling electrode adhesion. Here, the author proposes a facile and robust method to fabricate hierarchical and asymmetrical iontronic micropatterns through programmed regulation of the internal stress distribution and local ionic migration.
- Zehong Wang
- , Tiantian Li
- & Xuesong Jiang
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| Open AccessEvolution of Br⋯Br contacts in enantioselective molecular recognition during chiral 2D crystallization
Halogen-mediated interactions control molecular recognition in many chemical and biological systems. Here, the authors demonstrate two types of Br⋯Br contacts and their importance in chiral on-surface crystallization.
- Zhen-Yu Yi
- , Xue-Qing Yang
- & Li-Jun Wan
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Article
| Open AccessSelf-sorting in macroscopic supramolecular self-assembly via additive effects of capillary and magnetic forces
The selective assembly of μm-to-mm sized components is challenging because of the short-ranged molecular recognition. Here, the authors demonstrate a self-sorting mechanism to automatically identify the surface chemistry via additivity and competence between long-ranged magnetic/capillary forces.
- Minghui Tan
- , Pan Tian
- & Feng Shi
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| Open AccessEnhancement of electrocatalytic oxygen evolution by chiral molecular functionalization of hybrid 2D electrodes
While solar-to-fuel catalysis requires the careful transfer of electrons, there are still challenges understanding how electron spin contributes to reactivity. Here, authors employ chiral fused thiadiazole-helicenes to control spin polarization in oxygen evolution electrocatalysts.
- Yunchang Liang
- , Karla Banjac
- & Magalí Lingenfelder
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Article
| Open AccessSpontaneous water-on-water spreading of polyelectrolyte membranes inspired by skin formation
Stable interfaces between immiscible solvents are crucial for chemical synthesis and assembly, but interfaces between miscible solvents have been less explored. Here the authors report the spontaneous water-on-water spreading and self-assembly of polyelectrolytes.
- Sihan Tang
- , Jiang Gong
- & Qiang Zhao
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| Open Access3D nanoprinting via spatially controlled assembly and polymerization
Additive manufacturing methods at the macroscale have seen significant advances in recent times, but advances for the bottom-up formation of nanoscale polymeric features are yet to be realized. Here, the authors demonstrate that rapid crosslinking of an AFM delivered norbornene crosslinker in presence of a surface-tethered metathesis catalysts facilitates the curing of delivered material in an extremely rapid fashion
- Thomas G. Pattison
- , Shuo Wang
- & Greg G. Qiao
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Article
| Open AccessCatalyst-controlled functionalization of carboxylic acids by electrooxidation of self-assembled carboxyl monolayers
This work leverages substrate self-assembly at an electrode to promote selective substrate electrooxidation in the presence of oxidatively sensitive catalysts. This strategy is applied to decarboxylative coupling of carboxylic acids with olefins.
- Heather A. Hintz
- & Christo S. Sevov
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Article
| Open AccessNanobubbles explain the large slip observed on lubricant-infused surfaces
Why are lubricant-infused surfaces so effective at reducing drag in microfluidic flow? Here, authors reveal that infused nanostructured Teflon wrinkles induce large interfacial slip due to the spontaneous nucleation of surface nanobubbles, a mechanism likely to occur on most rough infused surfaces.
- Christopher Vega-Sánchez
- , Sam Peppou-Chapman
- & Chiara Neto
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| Open AccessSelf-assembly of N-heterocyclic carbenes on Au(111)
Although N-heterocyclic carbenes (NHCs) are a promising class of ligands for forming robust self-assembled monolayers on metals, many questions remain about their behavior on surfaces. Here, the authors address these fundamental questions—such as the factors controlling NHC orientation, mobility, and ability to self-assemble—through an in-depth examination of NHC overlayers on Au(111).
- Alex Inayeh
- , Ryan R. K. Groome
- & Alastair B. McLean
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| Open AccessCreating a regular array of metal-complexing molecules on an insulator surface at room temperature
Arrays of ordered metal atoms on bulk insulating materials are promising for future applications, such as optoelectronics and data storage. Here, the authors demonstrate a strategy to create an ordered metal array based on tailored anchoring and hard-sphere repulsion of metal-complexing molecules.
- Simon Aeschlimann
- , Sebastian V. Bauer
- & Angelika Kühnle
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| Open AccessHigh-resolution combinatorial patterning of functional nanoparticles
Precise patterning of functional nanoparticles can provide a powerful tool for next-generation macroscale devices. Here, the authors report a reliable nanoprinting technique that can pattern various functional nanoparticles on the substrate with a 200 nm pitch and 10 nm position accuracy, and above the millimeter scale.
- Xing Xing
- , Zaiqin Man
- & Zhenda Lu
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Article
| Open AccessElectrochemical deposition of N-heterocyclic carbene monolayers on metal surfaces
N-heterocyclic carbenes (NHCs) have been widely used for the formation of monolayers but self-assembly methods come with drawbacks such as need for dry environment or using specifically-synthesized precursors. Here, the authors demonstrate an approach for surface-anchoring of NHCs which overcomes these limitations by using electrochemically-assisted deprotonation.
- Einav Amit
- , Linoy Dery
- & Elad Gross
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| Open AccessTailoring π-conjugation and vibrational modes to steer on-surface synthesis of pentalene-bridged ladder polymers
Development of strategies for the synthesis of pi-conjugated polymers is hampered by limited solubility. Here, the authors report a synthetic protocol based on the search for specific vibrational modes through an appropriate tailoring of the p-conjugation of the precursors, in order to increase the attempt frequency of a chemical reaction.
- Bruno de la Torre
- , Adam Matěj
- & David Écija
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Article
| Open AccessAssembly of a patchy protein into variable 2D lattices via tunable multiscale interactions
As nanoscale building blocks, proteins offer unique advantages, including monodispersity and atomically tunable interactions, but their self-assembly is limited compared to inorganic or polymeric nanoparticles. Here, the authors show modular self-assembly of an engineered protein into four physicochemically distinct patterned 2D crystals via control of four classes of interactions.
- Shuai Zhang
- , Robert G. Alberstein
- & F. Akif Tezcan
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| Open AccessCombining high-resolution scanning tunnelling microscopy and first-principles simulations to identify halogen bonding
Scanning tunnelling microscopy (STM) is commonly used to study 2D molecular self-assembly but is not always enough to fully solve a supramolecular structure. Here, the authors combine a high-resolution version of STM with first-principles simulations to precisely identify halogen bonding in polycyclic aromatic molecules.
- James Lawrence
- , Gabriele C. Sosso
- & Giovanni Costantini
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Article
| Open AccessSelective self-assembly of 2,3-diaminophenazine molecules on MoSe2 mirror twin boundaries
Mirror twin boundaries (MTBs) have been observed as metallic line defects in 2D transition metal dichalcogenides, but their chemical properties are not well understood. Here, the authors show that MTB defect networks on MoSe2 are more chemically reactive to organic molecules than pristine domains, and can template the self-assembly of hexagonal organic porous structures.
- Xiaoyue He
- , Lei Zhang
- & Andrew Thye Shen Wee
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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 AccessA tightly-bonded and flexible mesoporous zeolite-cotton hybrid hemostat
Zeolites have attracted attention and have been applied as haemostatic agents; however, there are issues associated with released zeolite powder. Here, the authors report on the growth of zeolites on cotton fibres with high stability and haemostatic ability.
- Lisha Yu
- , Xiaoqiang Shang
- & Jie Fan
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| Open AccessTailoring atomic layer growth at the liquid-metal interface
Ultrathin metallic films are most often fabricated by atomic or molecular beam epitaxy under ultrahigh vacuum conditions, where it is difficult to control deposition and growth. Here, the authors describe a wet deposition method, using solution-borne gold nanocluster precursors, to regulate growth of atomically flat gold nanoislands on a surface.
- Hai Cao
- , Deepali Waghray
- & Steven De Feyter
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| Open AccessSelf-assembly directed one-step synthesis of [4]radialene on Cu(100) surfaces
Radialenes have distinct structural, electronic and chemical properties from other hydrocarbons, but their synthesis remains a challenge. Here, the authors report a copper catalyzed one-step synthetic protocol of [4]radialene via the cyclotetramerization of phenylacetylene molecules upon thermal activation.
- Qing Li
- , Jianzhi Gao
- & Minghu Pan
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| Open AccessA biomimetic chiral-driven ionic gate constructed by pillar[6]arene-based host–guest systems
Uptake and release of glucose is regulated by glucose-sensitive ion channels, but complexity of the system impedes investigation of the gating behavior under physiological conditions. Here the authors use a pillararene based artificial ion channel to mimic and investigate chirality driven switching of a glucose ion channel.
- Yue Sun
- , Fan Zhang
- & Haibing Li
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| Open AccessThe mechanisms of crystal growth inhibition by organic and inorganic inhibitors
Although trace compounds are known to inhibit crystal growth, the mechanisms by which they do so are unclear. Here, the authors use a microkinetic model to study the mechanisms of several inhibitors of calcite growth, finding that the processes are quite different for inorganic and organic inhibitors.
- S. Dobberschütz
- , M. R. Nielsen
- & M. P. Andersson
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Article
| Open AccessOptical characterization of surface adlayers and their compositional demixing at the nanoscale
Characterization of adsorbed molecular layers on surfaces is the key to wide-ranging applications, but elucidating the structure and composition of such adlayers remains challenging. Here the authors develop an approach to unveil the nanoscale structure and composition of adlayers through spectrally resolved super-resolution microscopy.
- Limin Xiang
- , Michal Wojcik
- & Ke Xu
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| Open AccessCopper-surface-mediated synthesis of acetylenic carbon-rich nanofibers for active metal-free photocathodes
While photoelectrochemical devices combine light-absorption with fuel and electricity generation, their implementation is hampered by high costs and low output. Here, the authors synthesized acetylene-rich carbon fibers by copper-mediated polymerization for high-activity, metal-free photocathodes.
- Tao Zhang
- , Yang Hou
- & Xinliang Feng
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Article
| Open AccessInsight into induced charges at metal surfaces and biointerfaces using a polarizable Lennard–Jones potential
Molecular dynamics models for predicting the behavior of metallic nanostructures typically do not take into account polarization effects in metals. Here, the authors introduce a polarizable Lennard–Jones potential that provides quantitative insight into the role of induced charges at metal surfaces and related complex material interfaces.
- Isidro Lorenzo Geada
- , Hadi Ramezani-Dakhel
- & Hendrik Heinz
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Article
| Open AccessAbnormal phase transition between two-dimensional high-density liquid crystal and low-density crystalline solid phases
Intermolecular interactions have a crucial role in the adsorption of molecules on a surface, however their role in promoting phase transitions is less well known. Here, the authors report an abnormal phase transition between a high-density liquid crystal and low-density solid in the case of carbon monoxide on Cu(111), driven by intermolecular interactions and entropy.
- Wenbin Li
- , Longjuan Kong
- & Lan Chen
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Article
| Open AccessSupramolecular networks stabilise and functionalise black phosphorus
Few-layered black phosphorus has been exploited in transistors and other devices, but its poor stability under ambient conditions remains problematic. Here, a UK-Swiss collaboration show that a monolayer-thick supramolecular hydrogen-bonded network can protect a black phosphorus surface for over a month.
- Vladimir V. Korolkov
- , Ivan G. Timokhin
- & Peter H. Beton
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Article
| Open AccessA light-regulated host–guest-based nanochannel system inspired by channelrhodopsins protein
Light-controlled gating of ion transport across membranes occurs in nature via channelrhodopsin nanochannels. Here, the authors show facile non-covalent approach towards light-responsive biomimetic nanochannels using host–guest interactions between a negative pillararene host and a positive azobenzene guest.
- Yue Sun
- , Junkai Ma
- & Haibing Li
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Article
| Open AccessOn-surface synthesis of aligned functional nanoribbons monitored by scanning tunnelling microscopy and vibrational spectroscopy
On-surface synthesis, in which molecular units assemble and couple on a defined surface, can access rare reaction pathways and products. Here, the authors synthesize functionalized organic nanoribbons on the Ag(110) surface, and monitor the evolution of the covalent reactions by an unorthodox vibrational spectroscopy approach.
- Nataliya Kalashnyk
- , Kawtar Mouhat
- & Sylvain Clair
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Article
| Open AccessA general patterning approach by manipulating the evolution of two-dimensional liquid foams
Ostwald ripening is thermodynamically favoured in many liquid and gas systems, where small particles tend to dissolve into large ones. Against this effect, Huanget al. use patterned microstructures to guide the evolution of two-dimensional liquid foams as a platform for the assembly of nanoparticles.
- Zhandong Huang
- , Meng Su
- & Yanlin Song
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Article
| Open AccessStacking sequence and interlayer coupling in few-layer graphene revealed by in situ imaging
Controlled preparation of few-layer graphene is a promising, yet challenging technological protocol. Here, the authors perform real-time imaging during chemical vapour deposition growth and hydrogen etching, to gain insight into layer-dependent growth mechanisms and graphene-substrate interaction.
- Zhu-Jun Wang
- , Jichen Dong
- & Marc-Georg Willinger
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Article
| Open AccessSelf-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface
The efficiency of a catalyst relies on the stability of intermediates on its surface. Here, the authors find that van der Waals interactions between acetate adsorbates on Au(110) provide a small but necessary energy contribution to stabilize the acetate and drive restructuring of the Au surface.
- Fanny Hiebel
- , Bonggeun Shong
- & Cynthia M. Friend
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Article
| Open AccessSimple direct formation of self-assembled N-heterocyclic carbene monolayers on gold and their application in biosensing
Self-assembled monolayers (SAMs) have shown tremendous number of applications but can suffer from low stability. Here, the authors report air and bench stable carbene precursors allowing facile SAM formation, and furthermore demonstrate an application in biosensing
- Cathleen M. Crudden
- , J. Hugh Horton
- & Akiko Yagi