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Articles by Mischa Bonn
Organic two-dimensional van der Waals heterostructures
Abstract Van der Waals heterostructures based on graphene and inorganic two-dimensional (2D) crystals enable exquisite control of interlayer coupling, and emergent electronic and optical phenomena1,2. Extending this concept to organic 2D crystals has been hindered by weak, non-directional interlayer interactions that frustrate lattice registry. Here we introduce a bottom-up strategy for programmable lattice engineering in organic van der Waals heterostructures of 2D polymers.
Sequence-encoded hexagonal lattices in multichannel peptide nanofibrils
Abstract Structural complexity in biological matter arises from molecular information that encodes supramolecular assembly across length scales1,2,3. Here we show that minimal nine-residue peptides can encode discrete lateral interaction motifs that direct supramolecular organization. These motifs generate hexagonal pores and hierarchically tile into multichannel nanofibrils with defined topology.
Suppressed excitonic effects enable high mobility and high-yield photoconductivity in a pyridine-coordinated two-dimensional polymer crystal
Abstract Two-dimensional polymers (2DPs) and their layer-stacked covalent organic frameworks (2D COFs) offer modular, atomically precise platforms for organic optoelectronics, yet their photoconductive responses remain fundamentally constrained by strong excitonic effects and localized charge transport. Here, we demonstrate that a diyne-linked 2DP crystal with axial pyridine coordination overcomes this limitation, enabling simultaneous efficient free-carrier generation and band-like transport.
Cold stimulus during the fibrillation lag phase induces molecularly distinct amyloid strains
Abstract Amyloid polymorphism is important in neurodegenerative and metabolic disease. Understanding fibril molecular polymorphism is critical to understanding why certain protein aggregates made from the same protein are pathogenic while others are benign. Here, we generate two polymorphs of human insulin, as a model system, induced by a thermal change in the nucleation (lag) phase.
Modulating nonequilibrium electron – phonon interactions and energy relaxation in MXenes by surface-anchored Mo 3 S 7 nanoclusters
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Abstract Electron–phonon (e–ph) interactions govern photoinduced nonequilibrium dynamics of MXenes, determining hot-carrier relaxation and parasitic heat accumulation. However, strategies to deliberately modulate these interactions through chemical control, together with mechanistic understanding, remain underexplored.
By Jiaxu Zhang, Rafael Muñoz-Mármol, Zijie Xiao, Dongqi Li, Shuai Fu, Xiaodong Li, Andrea Iudica, Valentino Romano, Pengfei Cao, Jingwei Du, Xingyuan Chu, Nicolas Perez Verified, Kornelius Nielsch, Giuseppe Maria Paterno, Lei Gao, Mischa Bonn, Minghao Yu, Xinliang Feng, Juliane Scheiter, Eva A. A. Pogna, Francesco Scottognella
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Nature
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Chemical and physical equilibria shape dual ice-nucleation pathways in an organic crystal
Abstract Organic crystals critically influence ice formation in natural environments, yet the molecular mechanisms of their ice nucleation activity remain poorly understood. Here we reveal that the exceptional freezing efficiency of phloroglucinol (PGL), a simple polyhydroxylated aromatic compound, arises from a dynamic interplay of chemical and physical equilibria that generate two concurrent nucleation pathways.
Cyclophane-based shielding strategy for singly dispersed graphene nanoribbons
Abstract Structurally precise graphene nanoribbons (GNRs) hold great promise for nanoelectronic devices owing to their tunable bandgaps and unique electronic properties. However, their practical integration into single-ribbon devices remains impeded by strong inter-ribbon aggregation.
Stereoelectronic and hydrogen-bonding effects on hydroxyproline conformation
Abstract Collagen’s structural integrity and biological function derive from its characteristic triple helix, governed by a unique amino acid sequence containing the rare residue (2S,4R)-hydroxyproline (4R-Hyp). Substituting 4R-Hyp with its diastereomer 4S-Hyp markedly reduces triple-helix thermal stability and impairs collagen function. The origins of this destabilization have mostly been ascribed to stereoelectronic effects such as the gauche effect and n → π* interactions.
Impact of Perfluorinated Organic Acids on Bacterial Ice Nucleators
Introduction Click to copy section linkSection link copied! Biological ice nucleators (INs) influence freezing processes across atmospheric and terrestrial environments, yet little is known about the influence of anthropogenic contaminants on their activity. Among the most efficient biological INs are ice-nucleating bacteria, such as Pseudomonas syringae, (1,2) which catalyze ice formation at temperatures close to 0 °C through specialized ice-nucleating proteins (INpros).
Diketopyrrolopyrrole-based two-dimensional poly(arylene vinylene)s with high charge carrier mobility - Nature Communications
Abstract Layered two-dimensional conjugated polymers (2D CPs), or 2D conjugated covalent organic frameworks, are promising semiconductor materials for (opto)electronics and photocatalysis, but their performance is often limited by insufficient in-plane conjugation and poor charge transport. Guided by density functional theory calculations, we report two donor-acceptor-type 2D poly(arylene vinylene)s constructed from thienyl-benzodithiophene and diketopyrrolopyrrole units.
Towards single-crystalline two-dimensional poly(arylene vinylene) covalent organic frameworks - Nature Chemistry
Abstract Vinylene-linked two-dimensional (2D) conjugated covalent organic frameworks, or 2D poly(arylene vinylene)s (2D PAVs), are promising polymer semiconductors for (opto-)electronics, photocatalysis and electrochemistry. However, conventional solvothermal synthesis often produces 2D PAVs that are poorly crystalline or difficult to access.
Unlocking ultrafast hot hole transport in transition metal oxides governed by the nature of optical transitions - Nature Communications
Abstract The intrinsically low carrier mobility of transition metal oxides within the polaron transport framework fundamentally limits their optoelectronic performance. Although optical transitions profoundly impact carrier generation and transport dynamics in oxide systems, the underlying mechanisms remain elusive. Here we demonstrate that the nature of optical transitions decisively regulates hot-hole transport in representative oxides, Co3O4 and α-Fe2O3.
Spontaneous dissociation of excitons in polymeric photocatalysts for overall water splitting - Nature Communications
Abstract Poly (Triazine Imide) (PTI), like other polymeric semiconductors, suffers from the high exciton binding energy, which intrinsically impedes the separation of photo-induced charge carriers. Herein, we present a crystal structure engineering strategy that exploits the lattice mismatch between the CaCl2 (12) growth template and basal planes of PTI to synthesize unusual PTI nanoplates featuring spontaneous exciton dissociation.
Hydrate-melt electrolyte design for aqueous aluminium-bromine batteries with enhanced energy-power merits - Nature Communications
Abstract Aluminium-based aqueous batteries hold promises for next-generation sustainable and large-scale energy storage due to the favorable metrics of Al and water-based electrolytes. However, the performance of current aluminium-based aqueous batteries falls significantly below theoretical expectations, with a critical bottleneck of realizing cathodes with high areal capacities.
Ballistic diffusion fronts in biomolecular condensates - Nature Nanotechnology
Abstract Biomolecular condensates in cells compartmentalize vital processes by enriching molecules through molecular recognition. However, it remains elusive how transport occurs in biomolecular condensates and how it relates to their dynamic and/or viscoelastic state. We show that the transport of molecules in DNA model condensates does not follow classical Fickian diffusion, which has a blurry front with a square root of time dependence.
Mode-resolved, non-local electron–phonon coupling in two-dimensional spectroscopy - Nature Physics
Abstract Electron–phonon coupling is fundamental to condensed-matter physics, governing various physical phenomena and properties in both conventional and quantum materials. Here we propose and demonstrate two-dimensional electron–phonon coupling spectroscopy that can directly extract the electron–phonon coupling matrix elements for specific phonon modes and different electron energies.
Experimental quantification of nuclear quantum effects on the hydrogen bond of liquid water
Abstract Nuclear quantum effects (NQEs) significantly influence material properties upon isotopic substitution, particularly with light atoms such as hydrogen. While water is rich in hydrogen, its hydrogen-bonded structure exhibits only moderate NQEs. Simulations ascribe this to competing zero-point energies (ZPEs): Intermolecular ZPEs stabilize hydrogen-bonds, while intramolecular ZPEs destabilize them.
Dimensional evolution of charge mobility and porosity in covalent organic frameworks - Nature Communications
Abstract Covalent organic frameworks are an emerging class of covalently linked polymers with programmable lattices and well-defined nanopores. Developing covalent organic frameworks with both high porosity and excellent charge transport properties is crucial for widespread applications, including sensing, catalysis, and organic electronics. However, achieving the combination of both features remains challenging due to the lack of overarching structure-property correlations.
Spontaneous ordering of identical materials into a triboelectric series - Nature
Abstract When two insulating, neutral materials are contacted and separated, they exchange electrical charge1. Experiments have long suggested that this ‘contact electrification’ is transitive, with different materials ordering into ‘triboelectric series’ based on the sign of charge acquired2. At the same time, the effect is plagued by unpredictability, preventing consensus on the mechanism and casting doubt on the rhyme and reason that series imply3.
Reactivatable stimulated emission depletion microscopy using fluorescence-recoverable nanographene - Nature Communications
Abstract Stimulated emission depletion (STED) microscopy, a key optical super-resolution imaging method, has extended our ability to view details to resolution levels of tens of nanometers. Its resolution depends on fluorophore de-excitation efficiency, and increases with depletion laser power. However, high-power irradiation permanently turns off the fluorescence due to photo-bleaching of the fluorophores. As a result, there is a trade-off between spatial resolution and imaging time.
Dynamic anti-correlations of water hydrogen bonds - Nature Communications
Abstract Water is characterized by strong intermolecular hydrogen bonds (H-bonds) between molecules. The two hydrogen atoms in one water molecule can form H-bonds of dissimilar length. Although intimately connected to water’s anomalous properties, the details and the origins of the asymmetry have remained elusive. We study water’s H-bonds using the O-D stretching vibrations as sensitive reporters of H-bonding of D2O and HOD in dimethylformamide.
Acid-Induced Fluorescence Enhancement of Piperazinylphenyl-substituted Nanographene
Acid-Induced Fluorescence Enhancement of Piperazinylphenyl-substituted Nanographene A dibenzo[hi,st]ovalene (DBOV) derivative bay-substituted with two piperazinylphenyl (PZP) groups (DBOV–PZP) was synthesized. Comprehensive investigations of its photophysical properties revealed acid-induced fluorescence enhancement through the protonation of PZP units, leading to the suppression of the photoinduced electron transfer.
MXenes with ordered triatomic-layer borate polyanion terminations - Nature Materials
Abstract Surface terminations profoundly influence the intrinsic properties of MXenes, but existing terminations are limited to monoatomic layers or simple groups, showing disordered arrangements and inferior stability. Here we present the synthesis of MXenes with triatomic-layer borate polyanion terminations (OBO terminations) through a flux-assisted eutectic molten etching approach.
Two Regioisomeric Ladder Polymers with a Fully Conjugated or Cross-Conjugated Polyacene-Type Skeleton
Download Hi-Res ImageDownload to MS-PowerPointCite This:Macromolecules 2024, XXXX, XXX RETURN TO ARTICLES ASAPPREVArticleNEXT Marvin T. Unruh Macromolecular Chemistry Group (buwmakro) and Wuppertal Center for Smart Materials and Systems (CM@S), Gauss-Str. 20, D-42119 Wuppertal, Germany , , , Silvio Osella Chemical and Biological Systems Simulation Lab, Centre of New Technologies, University of Warsaw, Banacha 2C, 02-097 Warsaw, Poland , * Hai I.
A solid beta-sheet structure is formed at the surface of FUS droplets during aging - Nature Chemical Biology
Abstract Phase transitions are important to understand cell dynamics, and the maturation of liquid droplets is relevant to neurodegenerative disorders. We combined NMR and Raman spectroscopies with microscopy to follow, over a period of days to months, droplet maturation of the protein fused in sarcoma (FUS). Our study reveals that the surface of the droplets plays a critical role in this process, while RNA binding prevents it.
Porphyrin-fused graphene nanoribbons - Nature Chemistry
Abstract Graphene nanoribbons (GNRs), nanometre-wide strips of graphene, are promising materials for fabricating electronic devices. Many GNRs have been reported, yet no scalable strategies are known for synthesizing GNRs with metal atoms and heteroaromatic units at precisely defined positions in the conjugated backbone, which would be valuable for tuning their optical, electronic and magnetic properties. Here we report the solution-phase synthesis of a porphyrin-fused graphene nanoribbon (PGNR).
Substrate effect on charging of electrified graphene/water interfaces
Substrate effect on charging of electrified graphene/water interfaces† Graphene, a transparent two-dimensional (2D) conductive electrode, has brought extensive new perspectives and prospects to electrochemical systems, such as chemical sensors, energy storage, and energy conversion devices. In many of these applications, graphene, supported on a substrate, is in contact with an aqueous solution.
Biological lipid hydration: distinct mechanisms of interfacial water alignment and charge screening for model lipid membranes
Biological lipid hydration: distinct mechanisms of interfacial water alignment and charge screening for model lipid membranes Studying lipid monolayers as model biological membranes, we demonstrate that water molecules interfacing with different model membranes can display preferential orientation for two distinct reasons: due to charges on the membrane, and due to large dipole fields resulting from zwitterionic headgroups.
Soft matter-water interface: general discussion
E. H. G. Backus, G. Ben Ari, S. Benaglia, M. Bonn, A. T. Bui, S. J. Cox, F. Della Pia, J. Fraxedas, G. Goel, Y. Jiang, D. Jin, K. Koga, D. Laage, S. Miao, A. Michaelides, K. Morgenstern, T. Mukherjee, Y. Nagata, H. Naito, O. Nir, M. Olvera de la Cruz, H. Orlikowska-Rzeznik, D. Pan, S. L. B. Rempe, C. G. Salzmann, A. Taira, A. Vilangottunjalil, S. Wang, A. P. Willard, Y. Yao and J.
Dynamics and nano-rheology of interfacial water: general discussion
X. R. Advincula, K. E. Blow, M. Bonn, A. T. Bui, Y. Cheng, S. J. Cox, F. Della Pia, U. Diebold, L. Fumagalli, G. Goel, J. A. Hayton, Y. Jiang, V. Kapil, N. Kavokine, K. Koga, D. Laage, M. Lahav, S. Miao, A. Michaelides, P. Montero de Hijes, K. Morgenstern, T. Mukherjee, N. O'Neill, D. Pan, P. M. Piaggi, S. L. B. Rempe, M. Salvalaglio, C. G. Salzmann, T. Sayer, M. Shepelenko, G. C. Sosso, S. Wang, B. Webber, A. P. Willard and Y.
Electrified/charged aqueous interfaces: general discussion
X. R. Advincula, E. H. G. Backus, M. Bonn, S. J. Cox, U. Diebold, A. Fellows, A. R. Finney, G. Goel, J. Hedley, Y. Jiang, D. Jin, V. Kapil, N. Kavokine, J. Klein, D. Laage, N. Mohandas, K. Morgenstern, T. Mukherjee, M. Olvera de la Cruz, H. Orlikowska-Rzeznik, S. Perkin, Pablo M. Piaggi, C. G. Rodellar, P. Ryan, T. Sayer, M. Seyffertitz, M. Shepelenko, G. C. Sosso, M. Thämer, A. Vilangottunjalil, R. Walker-Gibbons, Y. Wang, A. P. Willard and P.
Tribute to Hiro-o Hamaguchi: Expanding the Boundaries of Raman Spectroscopy
Figures References Support Info This publication has no figures. This publication has no References. Supporting Information Supporting Information The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcb.3c08380. Table of contents for the Hiro-o Hamaguchi Festschrift (PDF) Terms & Conditions Most electronic Supporting Information files are available without a subscription to ACS Web Editions.
Concluding remarks for Faraday Discussion on Water at Interfaces
Concluding remarks for Faraday Discussion on Water at Interfaces Water at interfaces is a fascinating and multifaceted topic that has garnered significant attention in various scientific fields due to its relevance and implications. This Faraday Discussion explored the complexity of water at different interfaces. Many of the reports highlight the need for a molecular-level understanding. The Discussion was lively and constructive.
Site-selective chemical reactions by on-water surface sequential assembly - Nature Communications
Abstract Controlling site-selectivity and reactivity in chemical reactions continues to be a key challenge in modern synthetic chemistry. Here, we demonstrate the discovery of site-selective chemical reactions on the water surface via a sequential assembly approach. A negatively charged surfactant monolayer on the water surface guides the electrostatically driven, epitaxial, and aligned assembly of reagent amino-substituted porphyrin molecules, resulting in a well-defined J-aggregated structure.
Efficient photocatalytic production of hydrogen peroxide using dispersible and photoactive porous polymers - Nature Communications
Abstract Developing efficient artificial photocatalysts for the biomimetic photocatalytic production of molecular materials, including medicines and clean energy carriers, remains a fundamentally and technologically essential challenge. Hydrogen peroxide is widely used in chemical synthesis, medical disinfection, and clean energy. However, the current industrial production, predominantly by anthraquinone oxidation, suffers from hefty energy penalties and toxic byproducts.
Transiently delocalized states enhance hole mobility in organic molecular semiconductors - Nature Materials
Abstract Evidence shows that charge carriers in organic semiconductors self-localize because of dynamic disorder. Nevertheless, some organic semiconductors feature reduced mobility at increasing temperature, a hallmark for delocalized band transport. Here we present the temperature-dependent mobility in two record-mobility organic semiconductors: dinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]-thiophene (DNTT) and its alkylated derivative, C8-DNTT-C8.
Biological Lipid Hydration: Distinct Mechanisms of Interfacial Water Alignment and Charge Screening for Model Lipid Membranes
Biological Lipid Hydration: Distinct Mechanisms of Interfacial Water Alignment and Charge Screening for Model Lipid Membranes Clara-Magdalena Saak, Lisa Dreier, Kevin Machel, Mischa Bonn and Ellen H.G. Backus Abstract Studying lipid monolayers as model biological membranes, we demonstrate that water molecules interfacing with different model membranes can display preferential orientation for two distinct reasons: due to charges on the membrane, and due to large dipole fields resulting from...
D2O as an Imperfect Replacement for H2O: Problem or Opportunity for Protein Research?
Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. B 2023, 127, 38 RETURN TO ISSUEPREVPerspectiveNEXT * , , and * Cite this: J. Phys. Chem. B 2023, 127, 38 Copyright © 2022 The Authors. Published by American Chemical Society.
Electron cooling in graphene enhanced by plasmon–hydron resonance - Nature Nanotechnology
Abstract Evidence is accumulating for the crucial role of a solid’s free electrons in the dynamics of solid–liquid interfaces. Liquids induce electronic polarization and drive electric currents as they flow; electronic excitations, in turn, participate in hydrodynamic friction. Yet, the underlying solid–liquid interactions have been lacking a direct experimental probe. Here we study the energy transfer across liquid–graphene interfaces using ultrafast spectroscopy.
Substrate Effect on Charging of Electrified Graphene/water Interfaces
Substrate Effect on Charging of Electrified Graphene/water Interfaces Yongkang Wang, Yuki Nagata and Mischa Bonn Abstract Graphene, a transparent two-dimensional (2D) conductive electrode, has brought extensive new perspectives and prospects to electrochemical systems, such as chemical sensors, energy storage, and energy conversion devices. In many of these applications, graphene, supported on a substrate, is in contact with an aqueous solution.
Exceptionally high charge mobility in phthalocyanine-based poly(benzimidazobenzophenanthroline)-ladder-type two-dimensional conjugated polymers - Nature Materials
Abstract Two-dimensional conjugated polymers (2DCPs), composed of multiple strands of linear conjugated polymers with extended in-plane π-conjugation, are emerging crystalline semiconducting polymers for organic (opto)electronics. They are represented by two-dimensional π-conjugated covalent organic frameworks, which typically suffer from poor π-conjugation and thus low charge carrier mobilities.
SynDLP is a dynamin-like protein of Synechocystis sp. PCC 6803 with eukaryotic features - Nature Communications
Abstract Dynamin-like proteins are membrane remodeling GTPases with well-understood functions in eukaryotic cells. However, bacterial dynamin-like proteins are still poorly investigated. SynDLP, the dynamin-like protein of the cyanobacterium Synechocystis sp. PCC 6803, forms ordered oligomers in solution. The 3.7 Å resolution cryo-EM structure of SynDLP oligomers reveals the presence of oligomeric stalk interfaces typical for eukaryotic dynamin-like proteins.
Ion-Specific Interactions at a Mineral-Water Interface Revealed by Surface-Sensitive Spectroscopy under Flow Conditions
A solid surface in contact with an aqueous solution is typically charged. When put in contact with an aqueous electrolyte solution, the surface charge and composition are crucially affected by the composition of the aqueous phase due to ion-specific interactions between ions and the solid surface. In this study, we combine surface-sensitive vibrational sum frequency generation (v-SFG) spectroscopy and flow experiments to investigate ion-specific interactions at the fluorite-water interface.
Nonmonotonic Friction due to Water Capillary Adhesion and Hydrogen Bonding at Multiasperity Interfaces
Abstract Capillary adhesion due to water adsorption from the air can contribute to friction, especially for smooth interfaces in humid environments. We show that for multiasperity (naturally oxidized) Si-on-Si interfaces, the friction coefficient goes through a maximum as a function of relative humidity. An adhesion model based on the boundary element method that takes the roughness of the interfaces into account reproduces this nonmonotonic behavior very well.
Ion Adsorption and Desorption at the CaF2‐Water Interface Probed by Flow Experiments and Vibrational Spectroscopy
Results and Discussion We performed experiments with and without applied flow at the fluorite-water interface under acidic conditions (1 mM HCl) and systematically varied the fluoride bulk concentration by adding different amounts of sodium fluoride to the hydrochloric solution.
Intrinsically Disordered Osteopontin Fragment Orders During Interfacial Calcium Oxalate Mineralization
Abstract Calcium oxalate (CaC2O4) is the major component of kidney stone. The acidic osteopontin (OPN) protein in human urine can effectively inhibit the growth of CaC2O4 crystals, thereby acting as a potent stone preventer. Previous studies in bulk solution all attest to the importance of binding and recognition of OPN at the CaC2O4 mineral surface, yet molecular level insights into the active interface during CaC2O4 mineralization are still lacking.
Distinguishing different excitation pathways in two-dimensional terahertz-infrared-visible spectroscopy
EXPERIMENTAL IMPLEMENTATION To implement the QS procedure, we modify the experimental setup described in our previous work.66. M. Grechko, T. Hasegawa, F. D’Angelo, H. Ito, D. Turchinovich, Y. Nagata, and M. Bonn, Nat. Commun. 9, 885 (2018). https://doi.org/10.1038/s41467-018-03303-y The procedure requires an increased time delay between the 2D TIRV signal and LO pulses at the detector. This time delay needs to be stable during the measurements with fluctuations ≪1 fs.
Between a hydrogen and a covalent bond
The concept of a molecule as a unit of bound atoms can be traced to Robert Boyle's 1661 treatise “The Sceptical Chymist” (1). Chemists often depict the strong covalent bonds in molecules formed through electronic interactions of atoms by sticks or springs. By contrast, much weaker attractive forces between molecules in liquids and solids, such as van der Waals forces, are typically unspecific and nondirectional and cannot be represented by sticks or springs.
Between a hydrogen and a covalent bond
Abstract References and Notes Abstract The concept of a molecule as a unit of bound atoms can be traced to Robert Boyle's 1661 treatise “The Sceptical Chymist” (1). Chemists often depict the strong covalent bonds in molecules formed through electronic interactions of atoms by sticks or springs. By contrast, much weaker attractive forces between molecules in liquids and solids, such as van der Waals forces, are typically unspecific and nondirectional and cannot be represented by sticks or springs.
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