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Real-time monitoring of reaction stereochemistry through single-molecule observations of chirality-induced spin selectivity
In situ chirality identification for single-molecule systems is not a straightforward task. Now, real-time chirality identification during a Michael addition reaction has been realized by continuous measurements of spin-polarized currents through a single-molecule junction, providing a promising method for studying symmetry-breaking reactions.
- Chen Yang
- , Yanwei Li
- & Xuefeng Guo
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Review Article |
Advances in single-molecule junctions as tools for chemical and biochemical analysis
The ability to detect and quantify a given analyte at the molecular level is a long-lasting goal for analytical and bioanalytical chemistry. This Review highlights how single-molecule junctions (SMJs) have been used for analytical purposes, from the detection of isomers and reaction intermediates to the detection of proteins and nucleic acids. Different SMJ approaches are discussed, along with their advantages and limitations over bulk analytical techniques.
- Essam M. Dief
- , Paul J. Low
- & Nadim Darwish
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Article |
σ–σ Stacked supramolecular junctions
Supramolecular interactions play an essential role in organic electronic materials and biological systems. Now, it has been demonstrated that the σ–σ stacking interactions between neighbouring non-conjugated molecules can offer an efficient pathway for charge transport through supramolecular junctions, which provides a new guideline for the design and fabrication of organic materials and devices.
- Anni Feng
- , Yu Zhou
- & Wenjing Hong
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Article |
Highly conducting single-molecule topological insulators based on mono- and di-radical cations
Designing long and highly conducting molecular wires has been a great challenge for decades. It has now been shown that a singly oxidized 2.6-nm-long oligophenylene-bridged bis(triarylamine) can show a single-molecule junction conductance over 0.1G0.
- Liang Li
- , Jonathan Z. Low
- & Latha Venkataraman
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Review Article |
Chemical fuels for molecular machinery
Chemically fuelled synthetic molecular machines are capable of driving and sustaining non-equilibrium motion, analogous to the biomachinery that underpins life. This Review discusses the chemical and physical features of biological and synthetic chemical fuels and highlights potential challenges and opportunities for the development of synthetic chemically fuelled machinery.
- Stefan Borsley
- , David A. Leigh
- & Benjamin M. W. Roberts
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Article |
Photogearing as a concept for translation of precise motions at the nanoscale
In a similar fashion to its macroscopic counterpart, molecular gearing is a correlated motion of intermeshed molecular fragments against one another. Now it has been shown that photogearing can be used to actively fuel molecular gearing motions with light and concomitantly shift the axis of rotation.
- Aaron Gerwien
- , Frederik Gnannt
- & Henry Dube
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Article |
Insights from an information thermodynamics analysis of a synthetic molecular motor
Information is physical, but the flow between information, energy and mechanics in chemical systems remains largely unexplored. Now, an autonomous molecular motor has been analysed with information thermodynamics, which relates information to other thermodynamic parameters. This treatment provides a general thermodynamic understanding of molecular motors, with practical implications for machine design.
- Shuntaro Amano
- , Massimiliano Esposito
- & Benjamin M. W. Roberts
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Reagentless biomolecular analysis using a molecular pendulum
A reagentless method for detecting analytes based on the motion of an inverted molecular pendulum has now been developed. The sensor is capable of detecting important physiological markers of stress, allergy, cardiovascular health, inflammation and cancer and works in blood, saliva, urine, tears and sweat. The sensor is also capable of collecting data in living animals.
- Jagotamoy Das
- , Surath Gomis
- & Shana O. Kelley
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Meeting Report |
No small matter
The confined geometry of nanopores enables a wealth of chemistry and analysis to be conducted at the single-molecule scale. Yi-Lun Ying, Aleksandar P. Ivanov and Vincent Tabard-Cossa report on recent developments discussed at the 2020 Nanopore Electrochemistry Meeting.
- Yi-Lun Ying
- , Aleksandar P. Ivanov
- & Vincent Tabard-Cossa
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Article |
Dipolar order in an amphidynamic crystalline metal–organic framework through reorienting linkers
A metal–organic framework (MOF) has been prepared that features dynamic rotors embedded within its crystalline lattice. The dipolar F2-functionalized carboxylate linkers—rapidly rotating at room temperature—show correlated behaviour upon cooling, converting the paraelectric MOF into an ordered antiferroelectric one below 100 K.
- Y.-S. Su
- , E. S. Lamb
- & S. E. Brown
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Perspective |
Molecular spins for quantum computation
Spins in molecules provide a simple platform with which to encode a quantum bit (qubit), the elementary unit of future quantum computers. This Perspective discusses how chemistry can contribute to designing robust spin systems based, in particular, on mononuclear lanthanoid complexes.
- A. Gaita-Ariño
- , F. Luis
- & E. Coronado
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Article |
Non-chemisorbed gold–sulfur binding prevails in self-assembled monolayers
Gold–thiol contacts are ubiquitous across the physical and biological sciences, connecting organic molecules to surfaces. Now, conductance measurements of different sulfur-bound single-molecule junctions show that thiols—in contrast to the prevailing view—are not chemisorbed on gold, which strongly suggests that the thiol hydrogen is retained.
- Michael S. Inkpen
- , Zhen–Fei Liu
- & Latha Venkataraman
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Article |
Catalytic transport of molecular cargo using diffusive binding along a polymer track
One-dimensional diffusive binding represents an important mechanism used by nature to facilitate many fundamental biochemical processes. Now, a completely synthetic system with similar capabilities has been constructed. The system was exploited to significantly speed up bimolecular reactions and to catalytically transport molecular cargo in solution and within physically separated compartments.
- Lifei Zheng
- , Hui Zhao
- & Wilhelm T. S. Huck
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Article |
High phase-purity 1T′-MoS2- and 1T′-MoSe2-layered crystals
The phase in which a crystal exists can have a direct influence over its properties; however, it is usually difficult to control during synthesis. Now it has been shown that micrometre-sized metallic 1T′-MoS2- and 1T′-MoSe2-layered crystals can be prepared in high phase purity on a large scale, and that they display promising electrocatalytic activity towards the hydrogen evolution reaction.
- Yifu Yu
- , Gwang-Hyeon Nam
- & Hua Zhang
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Article |
Ligand-modulated conformational switching in a fully synthetic membrane-bound receptor
A dynamic foldamer scaffold has now been ligated to a water-compatible, metal-centred binding site and a conformationally responsive fluorophore to form a receptor mimic that inserts into the membrane of artificial vesicles. Binding of specific carboxylate ligands induces a global conformational change that depends on the structure of the ligand, and can be detected via fluorescence.
- Francis G. A. Lister
- , Bryden A. F. Le Bailly
- & Jonathan Clayden
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News & Views |
Moving into another dimension
Molecular daisy-chain structures are typically made up of two interlocked components and can exhibit muscle-like contraction and extension in one dimension. Zinc-based multicomponent systems that can operate in two and three dimensions have now been designed and synthesized.
- Karine Fournel-Marotte
- & Frédéric Coutrot
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Article |
Controlled membrane translocation provides a mechanism for signal transduction and amplification
The transmission of chemical information across lipid bilayer membranes is crucial in biological systems. Now, an artificial chemical system able to both transduce and amplify chemical signals across a membrane has been developed. The system works by exploiting the controlled translocation of a synthetic molecule that is embedded within a vesicle membrane.
- Matthew J. Langton
- , Flore Keymeulen
- & Christopher A. Hunter
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Article |
Self-propelled supramolecular nanomotors with temperature-responsive speed regulation
Effective regulation over the motion of self-propelled micro- and nanomotors is a challenging proposition. Now, self-assembled stomatocyte nanomotors with thermoresponsive polymer brushes have been designed that sense changes in local temperature and regulate the accessibility of the hydrogen peroxide fuel — thereby adjusting the speed and behaviour of nanomotor itself.
- Yingfeng Tu
- , Fei Peng
- & Daniela A. Wilson
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News & Views |
Hot holes break the speed limit
Charge transfer through DNA has been well studied over recent decades from both a biological and electronics perspective. It has now been shown that charge transfer can be accelerated one hundredfold by using highly energetic 'hot holes', revealing a new mechanism that could help to create useful electronic biomaterials.
- D. N. Beratan
- & D. H. Waldeck
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Article |
Mechanically controlled quantum interference in individual π-stacked dimers
Single-molecule junctions provide a unique platform to understand how molecular structure affects electronic transport. Now it has been shown that electronic transport through a π-stacked dimer can be precisely controlled when pulling it apart. This behaviour is caused by quantum interference effects that are turned ON or OFF depending on dimer conformation.
- Riccardo Frisenda
- , Vera A. E. C. Janssen
- & Nicolas Renaud
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Article |
Engineering nanometre-scale coherence in soft matter
The existence (or not) of electronic coherence in homopolymers is dependent on a balance between monomer–monomer interactions and environmental heterogeneity. Now, by understanding how even–odd orbital symmetry influences coherence and produces resistance oscillations as a function of distance—it is shown that DNA sequences can be designed to support coherent charge transport.
- Chaoren Liu
- , Limin Xiang
- & Nongjian Tao
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Article |
A chemically powered unidirectional rotary molecular motor based on a palladium redox cycle
Control of motion at the molecular level is an integral requirement for the development of future nanoscale machinery. Now, governed by the fundamental reactivity principles of organometallic chemistry, a biaryl rotor is shown to exhibit 360° unidirectional rotary motion driven by the conversion of two simple fuels.
- Beatrice S. L. Collins
- , Jos C. M. Kistemaker
- & Ben L. Feringa
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Chemical polyglycosylation and nanolitre detection enables single-molecule recapitulation of bacterial sugar export
Capsular polysaccharides are a protective layer enveloping pathogenic bacteria. Understanding their export could guide the design of therapeutics that render bacteria vulnerable to attack by the immune system or other therapeutic agents. Now, a synthetic strategy of polyglycosylation has been developed to obtain defined capsular polysaccharide fragments. Subsequent nanolitre detection enables their export to be studied at the single-molecule level.
- Lingbing Kong
- , Andrew Almond
- & Benjamin G. Davis
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Article |
An autonomous molecular assembler for programmable chemical synthesis
Molecular machines that assemble polymers in a programmed sequence are fundamental to life. Now, synthetic machinery built from DNA has been used to execute a molecular program that produces peptides, or olefin oligomers, with a defined sequence. The oligomeric product is linked to a double-stranded DNA product that records the sequence of reactions that were executed.
- Wenjing Meng
- , Richard A. Muscat
- & Andrew J. Turberfield
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Article |
Molecular rectifier composed of DNA with high rectification ratio enabled by intercalation
Understanding the correlation between structure and charge transport properties of a DNA-based single molecule device is crucial to the creation of nanoscale functional devices. Now, a DNA-based molecular rectifier with a high rectification ratio has been constructed by site-specific intercalation of small molecules (coralyne) into native double-stranded DNA.
- Cunlan Guo
- , Kun Wang
- & Bingqian Xu
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Article |
Pick-up, transport and release of a molecular cargo using a small-molecule robotic arm
Factory assembly lines often feature robots that pick up, reposition and connect components in a programmed manner. Now, it has been shown that a molecular machine is able to pick up a cargo, reposition it, set it down and release it at a site approximately 2 nm away from the starting position.
- Salma Kassem
- , Alan T. L. Lee
- & Jordi Solà
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Article |
Unidirectional rotary motion in achiral molecular motors
Avoiding equal probability for clockwise and anticlockwise rotation is essential for the function of molecular motors, and both biological and synthetic systems take advantage of chirality to control the rotary direction. Now it has been shown, by integrating two rotor moieties in a symmetric meso motor design, that light-driven unidirectional rotary motion can be achieved in an achiral system.
- Jos C. M. Kistemaker
- , Peter Štacko
- & Ben L. Feringa
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News & Views |
Clamping down on cancer detection
An electrochemical clamp assay that enables the rapid and sensitive detection of nucleic acids containing single base mutations has now been developed. It has been shown to differentiate between cancer patient samples featuring a specific mutation, and controls from healthy donors or other cancer patients, all directly in unprocessed serum.
- Irina A. Gorodetskaya
- & Alon A. Gorodetsky
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News & Views |
Chirality transfer takes a jump
The transfer of chirality is known to occur through chemical bonds. Now, chiral biomolecules have been observed to impart some of their optical properties to a spatially separated achiral dye — with the transfer mediated by plasmon resonance from an achiral metallic nanostructure.
- Vladimiro Mujica
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Article |
Through-space transfer of chiral information mediated by a plasmonic nanomaterial
Surface-enhanced resonant Raman optical activity (SERROA) reveals the through-space transfer of chirality from biomolecules to achiral benzotriazole dye-conjugated nanotags. The chiroptical responses generated by the stereoisomers of ribose and tryptophan establish this as the basis for a stereoselective nanosensor platform.
- Saeideh Ostovar pour
- , Louise Rocks
- & Ewan W. Blanch
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Article |
Intermediate tunnelling–hopping regime in DNA charge transport
Charge transport in molecular systems is typically through coherent tunnelling over a short distance or incoherent hopping over a long distance. An intermediate regime between those two transport mechanisms has now been found for DNA systems with stacked guanine–cytosine sequences.
- Limin Xiang
- , Julio L. Palma
- & Nongjian Tao
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Article |
Molecular length dictates the nature of charge carriers in single-molecule junctions of oxidized oligothiophenes
Understanding the intrinsic electronic properties of building blocks in conjugated materials can provide powerful design guidelines to control charge transport, such as tuning the nature of the charge carriers. Now, single-molecule transport studies of a family of oxidized oligothiophenes have shown that their molecular length determines the dominant carrier type.
- Emma J. Dell
- , Brian Capozzi
- & Luis M. Campos
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Self-powered enzyme micropumps
Self-powered micropumps that are turned on by the presence of their respective substrates are formed from surface-immobilized, ATP-independent enzymes. Coupling substrate-sensing with transport enables the design of devices that deliver cargo in response to specific stimuli. Demonstrated here is the release of insulin at a rate proportional to ambient glucose concentration.
- Samudra Sengupta
- , Debabrata Patra
- & Ayusman Sen
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News & Views |
Knowing your neighbours
Quantitatively studying how the rate of a chemical reaction is affected by a reactant's atomic-scale environment is extremely challenging. This has now been achieved at the single-molecule level using scanning tunnelling microscopy to monitor tautomerization in an atomically well-defined environment.
- Peter Liljeroth
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Article |
Controlling intramolecular hydrogen transfer in a porphycene molecule with single atoms or molecules located nearby
The rate of an intramolecular hydrogen transfer reaction in a single porphycene molecule resting on a copper surface can be controlled by placing a copper adatom close to it. Cooperativity effects are also observed in rows of porphycene molecules, where the reaction rate of each individual molecule depends on the precise tautomer state of its neighbours.
- Takashi Kumagai
- , Felix Hanke
- & Leonhard Grill
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Article |
End-to-end conformational communication through a synthetic purinergic receptor by ligand-induced helicity switching
Biological receptors communicate information through ligand-induced conformational changes. A synthetic receptor with a boron-containing binding site that can selectively and reversibly complex a ligand (such as a purine nucleoside) is shown to function in a similar fashion. The resulting conformational change is relayed through the receptor, communicating structural information about the ligand to a spectroscopic reporter more than 2 nm away.
- Robert A. Brown
- , Vincent Diemer
- & Jonathan Clayden
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Article |
Water lubricates hydrogen-bonded molecular machines
Although much is understood about the mechanical behaviour of macroscopic machinery, less is known about their molecular equivalents. It is now shown that for molecular machinery consisting of hydrogen-bonded components their relative motion is strongly accelerated by adding small amounts of ‘lubricating’ water, whereas other protic liquids have much weaker or opposite effects.
- Matthijs R. Panman
- , Bert H. Bakker
- & Sander Woutersen
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Article |
Conditionally fluorescent molecular probes for detecting single base changes in double-stranded DNA
A molecular probe has been designed that distinguishes double-stranded DNA with single base-pair specificity. In this approach, two destabilizing bubbles, in which the base pairs are mismatched, are generated for each point mutation in the target DNA.
- Sherry Xi Chen
- , David Yu Zhang
- & Georg Seelig
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News & Views |
A molecular production line
A small molecule that mimics the sequence-specific peptide synthesis of nature's ribosomes paves the way for more elaborate artificial molecular synthesizers.
- Paul R. McGonigal
- & J. Fraser Stoddart
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Article |
Ultrafast dynamics in the power stroke of a molecular rotary motor
The light-driven power stroke of a unidirectional molecular motor is studied using ultrafast fluorescence spectroscopy. The evolution on the excited-state energy surface is observed on the 100 fs timescale and is accompanied by damped coherent molecular motion. The implications of these observations for the operation of the molecular motors are discussed.
- Jamie Conyard
- , Kiri Addison
- & Stephen R. Meech
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Article |
Optimizing the specificity of nucleic acid hybridization
High-fidelity pairing of nucleic acid polymers is important in the development of sensors and for the application of DNA nanotechnology. Here, a set of hybridization probes is described that discriminates single-base changes with high specificity. The probes function robustly across many different temperatures, salinities and nucleic acid concentrations.
- David Yu Zhang
- , Sherry Xi Chen
- & Peng Yin
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News & Views |
Fuelling movement at the nanoscale
Autonomous propulsion of microparticles using catalytic olefin polymerization, and directional rotation of a molecule on a metal surface using electrons from the tip of a scanning tunnelling microscope.
- Ben Feringa
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Article |
A robust molecular platform for non-volatile memory devices with optical and magnetic responses
The creation of ‘smart surfaces’ that can act as switches or memory devices will rely on systems with bistable states that can be interconverted externally. Now, a low-voltage and robust surface-confined switch that transduces an electrical input into an optical and magnetic output is described.
- Cláudia Simão
- , Marta Mas-Torrent
- & Concepció Rovira
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Review Article |
Dynamic DNA nanotechnology using strand-displacement reactions
The programmable and reliable hybridization of DNA strands has enabled the preparation of a wide variety of structures. This Review discusses how, in addition to these static assemblies, the process of displacing — and ultimately replacing — strands also makes possible the construction of dynamic systems such as logic gates or autonomous walkers.
- David Yu Zhang
- & Georg Seelig