All Events

perovskites are among the most promising materials for next-generation solar cells, offering exceptionalefficiency gains and driving major investment in large-scale production. Yet, as the technology moves toward realworlddeployment, corrosion has emerged as a critical but often overlooked challenge. It arises not only fromenvironmental exposure but also from the intrinsic reactivity of the perovskite itself, which can attack metalelectrodes such as gold through complex chemical pathways.This show highlights why corrosion in perovskite devices is both subtle and important. Light and heat can triggerchemical changes that produce reactive species, either directly corroding metals or transforming the perovskite intoa more aggressive state. By connecting principles from corrosion science and semiconductor physics, we revealhow these reactions originate and what must be done to control them at their source.

Synthetic chemistry has enabled the creation of materials with remarkable properties, yet they often lack thedynamic nature exhibited by biological systems. In contrast, living matter is self-organizing and responsive, whichis critical for processes such as cell differentiation, sensing, transport, actuation, structural support, and—morebroadly—adaptation to internal and external stimuli. Intriguingly, the application of DNA nanotechnology tosynthetic materials has opened avenues for achieving a range of features and a level of control reminiscent ofbiological systems. These materials have begun to emulate key cellular mechanisms, including the modulation ofviscoelastic properties in the extracellular matrix, cytoskeletal shape changes, control of molecular transport, andthe localization of processes in biomolecular condensates. In this talk, I will describe our progress in developingsuch programmable materials and highlight two recent examples. First, I will introduce a novel precision matrix forculturing cells and organoids. By integrating customizable mechanics with predictable, responsive features, thismatrix both guides and probes cellular development. Second, I will present an exotic form of soft matter that isself-assembled from more than 16,000 unique molecular components. This material demonstrates that highcompositional complexity can yield unique molecular architectures with emergent properties distinct from thoseof conventional polymers.References:* Speed et al. J. Polym. Sci. 2023, 61, 1713.* Peng et al., Nature Nanotech. 2023, 18, 1463.* Krieg & Shih, Angew. Chem. Int. Ed. 2018, 57, 714.* Gupta & Krieg, Nucl. Acids Res. 2024, 52, e80.* Prakash et al., Nature Nanotech. 2021, 16, 2021.* Speed et al., BioRxiv 2024. https://doi.org/10.1101/2024.07.12.603212

Hard coatings are integral to modern manufacturing, significantly impacting the optical properties, friction, hardness,corrosion resistance, and wear resistance of various surfaces. The global market for hard coatings is valued at $1.2 billion,with strong growth expected in the coming years, offering opportunities for the direct application of fundamentalresearch in industrial settings. One key challenge in this field is the low toughness of protective coatings, particularly innitrogen-based PVD/CVD hard coatings, where this issue is compounded by the low cohesive energy of grain boundaries.Due to their lack of ductility, nitrogen-based ceramic materials are prone to grain boundary cracking under mechanicalload, leading to the degradation of protective layers and reduced lifetime of coated parts. Our research focuses onunderstanding the structure-property relationships of these materials.Commercial coatings are typically a few micrometers thick, with microstructures consisting of grains ranging fromnanometers to micrometers, making them well-suited for study using modern electron microscopy. By combiningpicoindentors for in situ SEM and TEM with FIB-based manufacturing, we developed in situ testing approaches to assesskey mechanical properties such as Young's modulus, fracture stress, and fracture toughness, as well as to explore theunderlying fracture mechanisms. In this talk, I will present our findings on the design of grain boundaries, materialcomposition, and transformation toughening strategies, which have significantly enhanced the mechanical properties ofhard coatings.

In nature, sequence-specific biopolymers, such as peptides and nucleic acids, are essential to various biological systems and processes. These biopolymers are utilized in materials science to achieve precise property control. Typically, variations in amino acid sequences focus on functional regulation while nucleotides are used for structural control. This raises the question: How can we integrate peptide-based functionality with the spatial precision of DNA nanotechnology for innovative material design? Here, I will present examples illustrating the incredible properties of peptide self-assembly from my PhD, and the remarkable nanoarchitecture design achieved through DNA nanotechnology from my Postdoc. These two key elements establish a vision of utilizing and synergizing peptide functionality with structural control achieved by DNA nanotechnology.Specifically, I will show how subtle changes in the molecular environment influence the morphology and behavior of peptide assemblies such as diphenylalanine crystals and enable control over their growth and disassembly processes, revealing insights into peptide-based material manipulation (Nat. Commun., 2016). Another example is that of the amorphous assemblies of tri-tyrosine peptides, where we linked the molecular arrangement to unique mechanical and optical properties of glass-like peptide structures (Nature, 2024).Next, I will introduce the principles of DNA nanotechnology for advanced structural control. By designing DNA nano-frames capable of self-assembling into organized lattices, we created micron-scale 3D materials. We discovered that a minor modification in DNA linker length induces a crystalline phase transition, from simple cubic to face-centered cubic structures, altering lattice geometry. In addition, we established a method using acoustic waves to achieve scalable and morphologically controllable DNA assemblies at the millimetric scale (Nat. Commun., 2024). This approach highlights how DNA nanotechnology provides unparalleled spatial control, decoupling structural architecture from functional elements such as peptides and nanoparticles. Together, these projects illustrate how peptides and DNA nanotechnology can be potentially integrated to engineer novel materials and enhance our capacity to design materials with tailored properties across scales.

The development of high energy density, long running rechargeable batteries like Li ion batteries, that power so successfully all mobile electronic devices, can be considered as the greatest success of modern electrochemistry. However, the basis for this success was the capability of exploring most complex electrodes, electrolyte solutions and reactive interfaces by most sophisticated electroanalytical tools in conjunction with advanced spectroscopic and microscopic was a first-rate leader in electroanalytical ז"ל techniques. Professor Israel Rubinstein chemistry. I learned a lot from him. The main theme of this presentation is to examine what is the true horizons for advanced high energy density batteries that can promote the electro-mobility revolution. The limiting factor in Li-ion batteries in terms of energy density, cost, potential, durability and cycling efficiency are the cathode materials used. We will examine most energetic cathode materials and novel approaches we developed for their stabilization. We describe in this lecture which electrode materials can be relevant, methodologies of their stabilization by doping, coating, and affecting electrodes surface chemistry by the use of active additives. Most important cathode materials are comprising the 5 elements Li,Ni,Co,Mn,O at different stoichiometries that determine voltage and specific capacities. We will explain how the stoichiometry dictates basic cathodes properties.1,2 We will discuss the renaissance of Li metal-based rechargeable batteries.3 We have learned how the stabilize Li metal anodes in rechargeable batteries using reactive electrolyte solutions that induce excellent passivation through controlled surface reactions. The emphasis is on fluorinated co-solvents that open the door for a very rich surface chemistry that forms passivating surface films that behave as ideal solid electrolyte interphase on both anodes and cathodes in advanced secondary Li batteries. This field provides fascinating examples how systematic basic scientific work leads to development of most practical devices for energy storage & conversion.

The efficiency of a thermoelectric (TE) device depends on the extent to which, in response to a given temperature gradient, its electron/hole transport symmetry at the Fermi level is broken. This requirement makes molecular junctions highly promising for TE applications due to their non-linear transmission properties. Yet, in the absence of an efficient method to tune the position of the Fermi level within the transmission landscape of these junctions, the Seebeck values of metal-molecules-metal junctions are typically |S|≤50μV/K, while based on their electrical and thermal conductance, it should be |S|≥1mV/K to be relevant for applications. I will describe our effort to reach this goal, which recently has culminated in molecular junctions with the semimetal Bismuth (Bi) as one of their leads and with |S| in the required mV/K range. Unlike the conventional approach to tweak the transmission properties by modifying the structure of the molecules, here the high Seebeck is a result of molecularly induced deterministic changes in the density of states within the Bi lead in the form of quantized 2D interfacial states, that in turn result in highly non-linear transport properties. I will argue that this effect is just one glimpse into the very rich and complex terra incognita of molecular layers on semimetals.

This talk tells my outlook on the development of electric-field-mediated-chemistry/biochemistry and predicts a vision of its future state.1 The talk discusses applications of oriented electric-fields (OEFs) to chemical and biochemical reactions e.g., Diels  Alder reactions, and reactions of the enzyme Cytochrome P450. As shall be demonstrated, the orientation of the OEF controls reaction-rate (acceleration/inhibition), chemo-selectivity, enantio-selectivity, and solvent effect. This will be followed by showing relevant experimental verifications of the impact of OEF on structure and reactivity. Subsequently, the talk will outline other ways of generating OEFs, e.g. by use of; pH-switchable charges, ionic additives, water droplets, and so on. I shall further describe the application of static vs. oscillating OEFs to decompose peptide plaques (e.g., Amyloid Plaques in Alzheimer’s disease). The second part of the talk consists of conceptual principles for understanding and predicting OEF effects, e.g., the “reaction-axis rule”, the capability of OEFs to act as tweezers that orient reactants and accelerate their reaction, etc. Finally, I shall discuss the prospects of up-scaling applications of various OEF-sources to Molar concentrations. The talk ends with the vision that, in the forthcoming years, OEF usage will change chemical education, if not also the art of making new molecules.

Electrocatalytically driven reactions that produce alternative fuels and chemicals are considered as a useful means to store renewable energy in the form of chemical bonds. in recent years there has been a significant increase in research efforts aiming to develop highly efficient electrocatalysts that are able to drive those reactions. Yet, despite having made significant progress in this field, there is still a need for developing new materials that could function both as active and selective electrocatalysts. In that respect, Metal–Organic Frameworks (MOFs), are an emerging class of hybrid materials with immense potential in electrochemical catalysis. Yet, to reach a further leap in our understanding of electrocatalytic MOF-based systems, one also needs to consider the welldefined structure and chemical modularity of MOFs as another important virtue for efficient electrocatalysis, as it can be used to fine-tune the immediate chemical environment of the active site, and thus affect its overall catalytic performance. Our group utilizes Metal-Organic Frameworks (MOFs) based materials as a platform for imposing molecular approaches to control and manipulate heterogenous electrocatalytic systems. In this talk, I will present our recent study on electrocatalytic schemes involving MOFs, acting as: a) electroactive unit that incorporates molecular electrocatalysts, or b) non-electroactive MOF-based membranes coated on solid heterogenous catalysts.

Learning from data has led to paradigm shifts in a multitude of disciplines, including web, text and image search and generation, speech recognition, as well as bioinformatics. Can machine learning enable similar breakthroughs in understanding (quantum) molecules and materials? Aiming towards a unified machine learning (ML) model of molecular interactions in chemical space, I will discuss the potential and challenges for using ML techniques in chemistry and physics. ML methods can not only accurately estimate molecular properties of large datasets, but they can also lead to new insights into chemical similarity, aromaticity, reactivity, and molecular dynamics. For example, the combination of reliable molecular data with ML methods has enabled a fully quantitative simulation of protein dynamics in water (https://arxiv.org/abs/2205.08306). While the potential of machine learning for revealing insights into molecules and materials is high, I will conclude my talk by discussing the many remaining challenges.

Biomass is characterized as "material of biological origin, excluding material embedded in geological formations or fossilized." It serves as a valuable resource for energy production and as a foundational material for the synthesis of various commodity and specialty materials. The composition of biomass is notably more diverse and intricate than that of crude oil, resulting in significant distinctions between a conventional petroleum refinery and a biomass refinery, often referred to as a biorefinery. Unlike crude oil, which is typically abundant in gaseous, liquid, and solid hydrocarbons featuring a high carbon-to-oxygen (C/O) ratio, biomass primarily consists of complex biomacromolecules with a considerably lower C/O ratio. The conversion of biomass into commodity chemicals presents a promising approach to diminish society's reliance on fossil fuel resources—the predominant challenge of the 21st century. This challenge necessitates the development of tools and technologies to facilitate the transition from a predominantly petroleum-based to an alternative bio-based chemical industry. The objective of this seminar is to showcase the recent advancements we have made in enhancing bio-based platform molecules for the production of commodity or specialty chemicals. We achieve this through the utilization of C2 to C6 bio-based platforms, exemplified by polyols (e.g., glycerol), furanoids (e.g., furfural), and carboxylic acids (e.g., levulinic acid).

Understanding mechanisms of work for a wide range of applied nanomaterials begins with identifying “active units” in operating conditions, zooming in on the “active sites” and ends with a model explaining their role for functioning of the material or device. There are two main hurdles that we are particularly interested in overcoming: 1) heterogeneity of active species and sites and 2) their dynamics that can be directly responsible for their mechanisms. One possible method, ideally suitable for capitalizing on these challenges for rational design of new catalytic pathways, is the Aufhebung (sublation) principle from the Hegelian dialectics. It describes the process of advancing knowledge by integrating the two opposites: the thesis and antithesis. We adopt this principle to leverage the inherent heterogeneity of catalytic active species and active sites in metal catalysts for understanding and predicting new catalytic pathways for CO and CO2 conversion reactions. Starting with atomically dispersed (the thesis) Pt on ceria support, we use multimodal, operando characterization for monitoring formation of nanoparticles (the antithesis), identify reaction active species and unique active sites at the metal-support interface. With this knowledge, we design the “single-atoms” catalysts (synthesis) possessing the same active sites and enhanced stability in reaction conditions. I will highlight the role of oxygen vacancies for enhancing the dynamicity of Pt atoms and opening new reaction pathways for direct and reverse water gas shift reactions and CO oxidation reaction.

atom-probe tomograph (APT) can dissect a nanotip shaped specimen (radius

Innovative battery electrode materials are essential for unlocking the full potential of Li-ion batteries in various aspects of modern life. A primary focus is identifying novel materials with greater elemental diversity that offer improved stability, rapid charge capabilities, and high performance. Promising candidates, like early transition metal oxides, are earth-abundant and present opportunities for next-generation anode materials due to their redox voltage and more than a single stable oxidation state. Exploring fundamental design principles for improved de/lithiation mechanisms will influence battery functionality and advance energy storage capabilities. The first part will delve into the impact of the insulator-metal transition during lithiation, focusing on two distinctive Wadsley-Roth (WR) structures. Our findings underscore the critical role of disorder within these structures in determining kinetics and retained capacities for these anodes. The second part proposes a novel strategy leveraging the induction effect to reduce the operation voltage of Mo-oxide-based anodes. This reduction opens the door for Mo-based oxide anodes as an alternative to graphene. Understanding these key aspects can guide the search for alternatives to existing anodes for advancing the development of Li-ion batteries with enhanced performance in the energy storage field.

Noble metal thin films have attracted significant interest owing to their distinctive properties and structures, which make them ideal for applications in microelectronics, catalysis, energy, and photovoltaics. While several parameters influence the properties of these metals for such applications, the deposition process remains a critical factor. Atomic Layer Deposition (ALD) stands out as a prevalent deposition technique due to its surface-sensitive nature. The ALD process is characterized by its self-limiting surface reactions, promoting a layer-by-layer growth mechanism and allowing for precise control over film thickness and conformality. However, challenges arise in achieving continuous, pinhole-free noble metal ALD layers on oxide surfaces, often resulting in low film quality. These challenges can be traced back to the lack of adequate nucleation sites and the poor wettability of the low-surface energy substrates. The research studied the impact of substrate surface functionalization using organometallic molecules, such as trimethylaluminum (TMA) and diethylzinc (DEZ), on the nucleation and growth of Ru layers. The results reveal an enhancement in both nucleation density and the average diameter of the Ru nanoparticles deposited, and these improvements were attributed to an increase in both nucleation sites and elevated surface diffusivity. The latter effect is speculated to result from a reduction in the substrate's surface free energy. The study also examines the influence of substrate surface characteristics, including surface termination and crystallinity, on the nucleation and growth of Ru metal via ALD. The morphologies of the resulting Ru thin films are studied using scanning electron microscopy (SEM), atomic force microscopy (AFM), and grazing incidence small angle x-ray scattering (GISAXS). These analytical results are integrated with an experimental model to elucidate the differences in growth mechanisms observed across substrates. The findings underscore the importance of substrate choice in the ALD process and broaden our understanding of Ru metal growth. This research serves as an important step in optimizing the ALD process for various applications by tailoring substrate selection.

Processes in nature are often long-lasting, but they have a common goal, i.e., to advance structures or constructions. Especially for the composition of materials, it is worth having a closer look and mimic the natural concept for improving the properties of the known materials and in this way opening doors for new application fields. Among the concepts in nature there is the hybridization of materials, i.e., the blend of organic and inorganic materials with the goal of outperforming both constituting components. The engineering of such hybrid materials can be done in synthetic wet-chemical or in physical ways and often the results, i.e., the properties of the materials, will differ, even if their composition is identical. This may result from different qualities of interactions between the constituting materials. The quality of interactions can be controlled by the choice of the chemicals and/or the choice of hybridization process. Two recently developed approaches for hybridization base on vapor phase chemistry and are derived from atomic layer deposition (ALD) and result in hybrid thin film growth (molecular layer deposition, MLD) or subsurface hybridization of polymers (vapor phase infiltration, VPI). Both approaches open a plethora of new options for materials design for future applications. In this talk, some approaches of our group will be discussed that show great promise of vapor phase-grown hybrid films for innovation in technological fields beyond the microelectronics industry. Examples, where mechanical and electronic properties of polymeric materials have been significantly improved through nanoscale coatings and infiltration, will be shown. Furthermore, new concepts towards self-healing of semiconducting thin films, enabled by hybrid materials, will be shown. In most cases, the chemical or physical properties of the initial substrate are altered, typically improved, and new functionalities are added.

Wetting describes the ability of liquids to maintain contact with a solid surface, a phenomenon that is ubiquitous in nature.1 However, in engineering and medical applications, contact of solid surfaces with aqueous media leads to undesirable phenomena such as corrosion, chemo- and biofouling, which have extremely negative economic, health, and environmental impacts. Therefore, control of wetting on solid surfaces is key to mitigating its detrimental effects. The latter can be achieved by minimizing the contact of the solid substrate with aqueous media, so-called superhydrophobic surfaces (SHS). Although SHS have been studied for decades to overcome wetting challenges,2 they are still rarely used in engineering applications. When immersed underwater, a special type of SHS can trap air on its surface, so-called air plastron, also known as an aerophilic surface. To date, plastrons have been reported to be impractical for underwater engineering due to their short lifetime. Here, I will describe aerophilic surfaces made of titanium alloy (Ti) with an extended lifetime of plastron conserved for months underwater.3 The extended methodology was developed to unambiguously describe the wetting regime on such aerophilic surfaces since conventional goniometric measurements are simply impractical. My aerophilic surfaces drastically reduce the adhesion of blood, and when immersed in aqueous media, prevent the adhesion of bacteria, and marine organisms such as barnacles, and mussels. Applying thermodynamic stability theories, we describe a generic strategy to achieve long-term stability of plastron on aerophilic surfaces for demanding and hitherto unattainable applications. (1) Quéré, D. Wetting and Roughness. Annual Review of Materials Research 2008, 38 (1), 71-99. (2) Cassie, A. B. D.; Baxter, S. Wettability of porous surfaces. Transactions of the Faraday Society 1944, 40, 546-551. (3) Tesler, A.B.;* Kolle, S.; Prado, L.H.; Thievessen, I.; Böhringer, D.; Backholm, M.; Karunakaran, B.; Nurmi, H.A.; Latikka, M.; Fischer, L.; Stafslien, S.; Cenev, Z.M.; Timonen, J.V.I.; Bruns, M.; Mazare, A.; Lohbauer, U.; Virtanen, S.; Fabry, B.; Schmuki, P.; Ras, R.H.A.; Aizenberg, J.; Goldmann, W.H. Long-Lasting Aerophilic Metallic Surfaces Underwater. Nature Materials 2023, accepted. *Corresponding author

In recent years, covalently bound dimers of chromophores have attracted significant interest as singlet fission (SF) material because of better control of coupling of different electronic states to the gateway 1(TT) by means of intramolecular vibrational modes.1 It has been shown that charge transfer (CT) plays a crucial role in mediating the S1-1(TT) interaction and their influence can be conveniently tuned by solvent polarity. Motivated by the experimental and theoretical work of Alvertis et al.,1 we have investigated the electronic states relevant to the SF for the covalently bound tetracene dimer with the goal to provide a broader picture of the occurring photodynamical processes.2 For that purpose, the second-order algebraic diagrammatic construction (ADC(2)) method in combination with the conductor-like screening model (COSMO) has been used. Vertical excitations and potential energy curves for excitonic and CT states along low-frequency symmetric and antisymmetric normal modes have been computed. These results have been combined with those obtained by density functional theory/multireference configuration interaction (DFT/MRCI) calculations for the 1(TT) state since its doubly-excited wavefunction is not accessible to the ADC(2) method. In the second part of the talk, DFT/MRCI calculations on dimer and trimer TIPS-Pn will be presented with the goal of a first theoretical understanding of the photodynamics of the 1(TT) state monitored by time-resolved mid-IR absorption spectroscopy.3

Organic/printed electronics is a technology enabling the fabrication of mechanically flexible/stretchable electronic circuits and devices using low-temperature, possibly by additive, solution processing methodologies. In this presentation we report the development of novel materials, as well as thin-film processing and morphology engineering, for flexible and stretchable organic and inorganic thin film transistors, electrolyte gated transistors and circuits. On material development, we present that “soft” small-molecules and polymers can be synthesized by co-polymerizing naphthalenediimide (NDI) or diketopyrrolopyrrole (DPP) units with proper co-monomer building blocks or properly designed additives. Furthermore, we also report the fabrication of stretchable inorganic metal oxide fiber network by spry coating metal salts+thermally labile polymer formulations. New transistor architectures using semiconductor film porosity as the key element for enhancing mechanical flexibility and tune charge transport are also demonstrated. These films, combined with elastomeric pre-stretching, enables unprecedentedly stable current-output characteristic upon mechanical deformation, which are used for sensing analytes, strain, light, temperature and physiological parameters. Finally, we report our recent work on molecular n-doping of organic semiconductors using a novel strategy involving catalysts.

Fundamental understanding of physiological processes that occur at biological membranes, such as membrane fusion, necessitates addressing not only the biochemical aspects, but also biophysical aspects such as membrane mechanical properties and membrane curvature. In this talk, I will show how we combine membrane model systems, micropipette aspiration, optical tweezers and confocal fluorescence microscopy to study membrane shaping and membrane fusion processes. I will describe a new tool we developed, where we form membrane bilayers supported on polystyrene microspheres which can be trapped and manipulated using optical tweezers. Using this approach, we demonstrate successful measurements of the interaction forces between the Spike protein of SARS CoV-2 and its human receptor, ACE2. We further use bead-supported membranes interacted with aspirated vesicles to reveal the inhibitory effect of membrane tension on hemifusion. I will also describe a particular case of membrane shaping during the formation of the newly discovered organelle termed migrasome. We show that tetraspanin proteins involved in migrasome formation strongly partition into curved membrane tethers, and we reveal a novel, two-step process of migrasome biogenesis.

Femtosecond pump-probe experiments on nanocrystals are interpreted primarily in terms of state filling of the states involved in the intense band edge absorption features, and bi-exciton shifting which changes the resonance energy of the probe pulse due to presence of pump induced excitations. Results have been interpreted to show 1) that “hot” excitons will relax to the lowest available levels in the conduction band in ~1 ps, and 2) that said intense band edge exciton transition will be bleached linearly with excitons until the underlying states are completely filled. In the talk we describe a new approach involving “spectator excitons” to test these accepted views. It consists of comparing pump-probe experiments on pristine samples, with equivalent scans conducted on the same sample after it has been saturated in cold mono-excitons. We show how this method has uncovered previously unrecognized spin blockades in the relaxation of hot multi-exciton states in CdSe NCs, and simply detects stimulated emission signals even in presence of overlapping absorption. We report specific difficulties of applying this approach on perovskite crystals leading to controversial determination that in quantum confined CsPbBr3 bi-exciton interactions are positive (repulsive) and describe recent time resolved emission data which challenges this result.

  Energy materials are crystalline, solid-state substances with technological applications in energy-conversion or storage devices that include solar cells and batteries. In our work, we are particularly interested in scenarios where these systems show unusual structural dynamical effects. These effects trigger many puzzling questions in regard to updated structure-property relations and improved theoretical understandings of these solids. In my talk, I will present our recent findings regarding theoretical treatments of structural dynamics in energy materials and how we may use them to improve our understanding of their finite-temperature properties. The results will focus on halide perovskite as well as nitride semiconductors and solid-state ion conductors, which we typically investigate in tandem with experiment.

The development of sustainable methods for the closed-loop production and recycling of plastics is an important challenge of current times. Reactions based on catalytic (de)hydrogenation are atom-economic, and sustainable routes for organic transformations.1 Using the following examples, this lecture will discuss the application of homogeneous (de)hydrogenative catalysis for the synthesis and degradation of polymers to enable a circular economy: (a) synthesis of polyamides/nylons from the ruthenium catalysed dehydrogenative coupling of diamines and diols and its reverse reaction i.e. hydrogenative depolymerisation of nylons,2 (b) synthesis of polyureas from the ruthenium/manganese catalysed dehydrogenative coupling of diamines3,4 and methanol, and its reverse reaction, i.e. hydrogenative depolymerisation of polyureas (Figure 1B)5, (c) Synthesis of polyethyleneimines from manganese catalysed coupling of ethylene glycol and ethylenediamine or the self-coupling of ethanolamine,6 and (d) Synthesis of polyureas and polyurethanes from the dehydrogenative coupling of diformamides and diamines/diols and its reverse reaction i.e. hydrogenative depolymerisation of polyureas and polyurethanes to diformamides and diamines/diols.7 Some applications of some of the polymers made using dehydrogenative processes in the field of batteries will also be discussed.8

Scanning transmission electron microscopy (STEM) is one of the most popular materials science methods to characterize the structure and chemistry of nanoscale samples, owing to its high resolution and many flexible operating modes. In a conventional STEM experiment, we focus the electron beam down to a probe from nanometer to sub-angstrom scale, and scan it over the sample surface while recording diffracted signals which are transmitted through the specimen. STEM can also record analytic signals such as x-rays generated by the electron beam to measure composition, or energy loss of the transmitted electrons to probe the electronic structure of samples. Conventional STEM imaging detectors experiments produce only a few intensity values at each probe position, but modern high-speed detectors allow us to measure a full 2D diffraction pattern, over a grid of 2D probe positions, forming a four dimensional (4D)-STEM dataset. These 4D-STEM datasets record information about the local phase, orientation, deformation, and other parameters, for both crystalline and amorphous materials. 4D-STEM datasets can contain millions of images and therefore require highly automated and robust software codes to extract the target properties. In this talk, I will introduce our open source py4DSTEM analysis toolkit, and show how we use these codes to perform data-intensive studies of material properties over functional length scales. I will also demonstrate some applications of modern machine learning tools, to perform measurements on electron diffraction patterns where property signals have been scrambled by multiple scattering of the electron beam.

Finding new materials for the conversion of CO2 into useful products is a complex task. Simulations can provide mechanistic and stability insights trying to accelerate the process. In my talk I will present the different degrees of complexity that we try to address in the simulations and which are the major challenges in the field.

Liquid-Liquid phase separation (LLPS) has been of fundamental importance in the assembly of thermally driven materials and has recently emerged as an organizational principle for living systems. Biological phase separation is driven out of equilibrium through complex enzyme composition, chemical reactions, and mechanical activity, which reveals a gap in our understanding of this fundamental phenomenon. Here we study the impact of mechanical activity on LLPS. We design a DNA-based LLPS system coupled to flows through molecular motors and a cytoskeleton network. Active stress at an interface of a liquid droplet suppressed phase separation and stabilized a single-phase regime well beyond the equilibrium binodal curve. The phase diagram out of equilibrium revealed a 3-dimensional phase space that depends on temperature and local molecular activity. Similar dynamics and structures are observed in simulations, suggesting that suppression of liquid phase separation by active stress is a generic feature of liquid phase separation.

Machine learning (ML) became a premier tool for modeling chemical processes and materials properties. For instance, ML interatomic potentials have become an efficient alternative to computationally expensive quantum chemistry simulations. In the case of reactive chemistry designing high-quality training data sets is crucial to overall model accuracy. To address this challenge, we develop a general reactive ML interatomic potential through unbiased active learning with an atomic configuration sampler inspired by nanoreactor molecular dynamics. The resulting model is then applied to study five distinct condensed-phase reactive chemistry systems: carbon solid-phase nucleation, graphene ring formation from acetylene, biofuel additives, combustion of methane and the spontaneous formation of glycine from early-earth small molecules. In all cases, the results closely match experiment and/or previous studies using traditional model chemistry methods. Altogether, explosive growth of user-friendly ML frameworks, designed for chemistry, demonstrates that the field is evolving towards physics-based models augmented by data science. I will also overview some applications of Non-adiabatic EXcited-state Molecular Dynamics (NEXMD) framework developed at several institutions. The NEXMD code is able to simulate tens of picoseconds photoinduced dynamics in large molecular systems. As an application, I will exemplify ultrafast coherent excitonic dynamics guided by intermolecular conical intersections. Here X-ray Raman signals are able to sensitively monitor the coherence evolution. The observed coherences have vibronic nature that survives multiple conical intersection passages for several hundred femtoseconds at room temperature. These spectroscopic signals are possible to measure at XFEL facilities and our modeling results allow us to understand and potentially manipulate excited state dynamics and energy transfer pathways toward optoelectronic applications. References: 1. N. Fedik, R. Zubatyuk, N. Lubbers, J. S. Smith, B. Nebgen, R. Messerly, Y. W. Li, M. Kulichenko, A. I. Boldyrev, K. Barros, O. Isayev, and S. Tretiak “Extending machine learning beyond interatomic potentials for predicting molecular properties” Nature Rev. Chem. 6, 653 (2022). 2. G. Zhou, N. Lubbers, K. Barros, S. Tretiak, B. Nebgen, “Deep Learning of Dynamically Responsive Chemical Hamiltonians with Semi-Empirical Quantum Mechanics,” Proc. Nat. Acad. Sci. USA, 119 e2120333119 (2022) 3. S. Zhang, M. Z. Makos, R. B. Jadrich, E. Kraka, B. T. Nebgen, S. Tretiak, O. Isayev, N. Lubbers, R. A. Messerly, and J. S. Smith “Exploring the frontiers of chemistry with a general reactive machine learning potential,” (2023) https://chemrxiv.org/engage/chemrxiv/article-details/6362d132ca86b84c77ce166c 4. A. De Sio, E. Sommer, X. T. Nguyen, L. Gross, D. Popović, B. Nebgen, S. Fernandez-Alberti, S. Pittalis, C. A. Rozzi, E. Molinari, E. Mena-Osteritz, P. Bäuerle, T. Frauenheim, S. Tretiak, C. Lienau, “Intermolecular conical intersections in molecular aggregates” Nature Nanotech. 16, 63 – 68 (2021). 5. V. M. Freixas, D. Keefer, S. Tretiak, S. Fernandez-Alberti, and S. Mukamel, “Ultrafast coherent photoexcited dynamics in a trimeric dendrimer probed by X-ray stimulated-Raman signals,” Chem. Sci., 13, 6373 – 6384 (2022).

Proteins are the fundamental building blocks of life. They form high performance materials and carry out cellular functions. They are able to fulfil these roles by assembling together to form sophisticated structures and architectures, which in many cases extend to mesoscopic liquid or solid phases. This talk focuses on understanding the transitions between these phases, their fundamental material properties and the way that the modulate biological function and malfunction. I will then discuss two areas opened up by the control of protein assembly. I will first focus on the understanding of the mechanism of protein aggregation and the discovery of molecules that can ameliorate malfunctioning protein self-assembly in a range of age-associated disease states. I will then outline some of our efforts to control protein self-assembly to form silk-inspired sustainable materials

Magnetism is one of the largest, most fundamental, and technologically most relevant fields of condensed-matter physics. Traditionally, two elementary magnetic phases have been distinguished - ferromagnetism and antiferromagnetism. The spin polarization in the electronic band structure reflecting the magnetization in ferromagnetic crystals underpins the broad range of time-reversal symmetry-breaking responses in this extensively explored and exploited type of magnets. By comparison, antiferromagnets have vanishing net magnetization. Recently, there have been observations of materials in which strong time-reversal symmetry-breaking responses and spin-polarization phenomena, typical of ferromagnets, are accompanied by antiparallel magnetic crystal order with vanishing net magnetization, typical of antiferromagnets [1]. A classification and description based on spin-symmetry principles offers a resolution of this apparent contradiction by establishing a third distinct elementary magnetic phase, dubbed altermagnetism [2]. We will start the talk with an overview of the still emerging unique phenomenology of this unconventional d-wave (or higher even-parity wave) magnetic phase, and of the wide array of altermagnetic materials. We will then show how altermagnetism can facilitate a development of ultra-fast and low-dissipation spintronic information technologies, and can have impact on a range of other modern areas of condensed matter physics and nanoelectronics. References [1] L. Šmejkal, A. H. MacDonald, J. Sinova, S. Nakatsuji, T. Jungwirth, Nature Reviews Mater. 7, 482 (2022). [2] L. Šmejkal, J. Sinova & T. Jungwirth, Phys. Rev. X (Perspective) 12, 040501 (2022).

Magnetism is one of the largest, most fundamental, and technologically most relevant fields of condensed-matter physics. Traditionally, two elementary magnetic phases have been distinguished - ferromagnetism and antiferromagnetism. The spin polarization in the electronic band structure reflecting the magnetization in ferromagnetic crystals underpins the broad range of time-reversal symmetry-breaking responses in this extensively explored and exploited type of magnets. By comparison, antiferromagnets have vanishing net magnetization. Recently, there have been observations of materials in which strong time-reversal symmetry-breaking responses and spin-polarization phenomena, typical of ferromagnets, are accompanied by antiparallel magnetic crystal order with vanishing net magnetization, typical of antiferromagnets [1]. A classification and description based on spin-symmetry principles offers a resolution of this apparent contradiction by establishing a third distinct elementary magnetic phase, dubbed altermagnetism [2]. We will start the talk with an overview of the still emerging unique phenomenology of this unconventional d-wave (or higher even-parity wave) magnetic phase, and of the wide array of altermagnetic materials. We will then show how altermagnetism can facilitate a development of ultra-fast and low-dissipation spintronic information technologies, and can have impact on a range of other modern areas of condensed matter physics and nanoelectronics. References [1] L. Šmejkal, A. H. MacDonald, J. Sinova, S. Nakatsuji, T. Jungwirth, Nature Reviews Mater. 7, 482 (2022). [2] L. Šmejkal, J. Sinova & T. Jungwirth, Phys. Rev. X (Perspective) 12, 040501 (2022).

Multiple proteins function as nanomachines, and carry out multiple specific tasks in the cell by alternating chemical steps with conformational transitions. Single-molecule FRET spectroscopy is a powerful tool for studying the internal motions of proteins. In recent years, we have been using this technique to study a range of protein machines, surprisingly finding in each case microsecond-time-scale internal dynamics. What is the role of these fast motions in the much-slower functional cycles of these machines?

Click chemistry has revolutionized many facets of the molecular sciences, with the realization of reactions that are ‘‘modular, wide in scope, give very high yields, generate only inoffensive byproducts that can be removed by nonchromatographic methods and are stereospecific”. Yet surprisingly little attention has been given to the development of intrinsically chiral click reactions (potentially enantiospecific, rather than ‘only’ enantioselective due to chiral auxiliary groups), while the modularity of many click reactions is best compared to one-dimensional LEGO. Of course, much could be done within the constraints – hence forementioned revolution – but it drove attention towards an extension of available click chemistries. Kolb, H. C.; Finn, M.; Sharpless, K. B., Click chemistry: diverse chemical function from a few good reactions. Angew. Chem. Int. Ed. 2001, 40, 2004-2021. The talk will focus on the resulting investigations in the field of S(VI) exchange chemistry, with specific emphasis on two fields: a) the development of the intrinsically enantiospecific click reactions and their use to e.g. make synthetic polymers with 100% backbone chirality that combine stability & degradabbility, and b) the development of multimodular click chemistry and single-polymer studies by a combination of AFM, TEM, scanning Auger microscopy

The remarkable properties of excitons in transition-metal-dichalcogenides (TMDs), together with the ability to readily control their charge carriers, have attracted a significant amount of interest in recent years. Despite the atomic dimensions of the hosting 2D semiconductors, TMD excitons exhibit strong interaction with light, both in absorption and photoemission processes, and practically dominate the optical response of these 2D materials. In this talk, I will introduce several approaches for achieving extremely strong light-exciton interactions. First, by optical and electrical manipulation of TMD excitons inside a van der Waals heterostructure cavity [1], second, via the formation of highly-confined, in-plane exciton polaritons [2], and third, through the realization of valley-polarized hyperbolic exciton polaritons [3]. These enhanced light–exciton interactions may provide a platform for studying excitonic phase-transitions, quantum nonlinearities and the enablement of new possibilities for 2D semiconductor-based optoelectronic devices. [1] I. Epstein et al, "Near-unity Light Absorption in a Monolayer WS2 Van der Waals Heterostructure Cavity", Nano letters 20 (5), 3545-3552 (2020). [2] I. Epstein et al, "Highly Confined In-plane Propagating Exciton-Polaritons on Monolayer Semiconductors", 2D Materials 7, 035031 (2020). [3] T. Eini, T. Asherov, Y. Mazor, and I. Epstein, "Valley-polarized Hyperbolic Exciton Polaritons in Multilayer 2D Semiconductors at Visible Frequencies", Phys. Rev. B 106, L201405 (2022).

Medicine is taking its first steps toward patient-specific cancer care. Nanoparticles have many potential benefits for treating cancer, including the ability to transport complex molecular cargoes, including siRNA and protein, as well as targeting specific cell populations. The talk will explain the fundamentals of nanotechnology, from ‘barcoded nanoparticles’ that target sites of cancer where they perform a programmed therapeutic task. Specifically, liposomes diagnose the tumor and metastasis for their sensitivity to different medications, providing patient-specific drug activity information that can be used to improve the medication choice. The talk will also describe how liposomes can be used for degrading the pancreatic stroma to allow subsequent drug penetration into pancreatic adenocarcinoma and how nanoparticle’ biodistribution and anti-cancer efficacy are impacted by the patient’s sex and, more specifically, the menstrual cycle. The evolution of drug delivery systems into synthetic cells, programmed nanoparticles that have an autonomous capacity to synthesize diagnostic and therapeutic proteins inside the body, and their promise for treating cancer and immunotherapy, will be discussed. References: 1) Theranostic barcoded nanoparticles for personalized cancer medicine, Yaari et al. Nature Communications, 2016, 7, 13325 2) Collagenase nanoparticles enhance the penetration of drugs into pancreatic tumors, Zinger et al., ACS Nano, 13 (10), 11008-11021, 2019 3) Targeting neurons in the tumor microenvironment with bupivacaine nanoparticles reduces breast cancer progression and metastases, Science Advances, Kaduri et al., 7 (41), eabj5435, 2021 4) Nanoparticles accumulate in the female reproductive system during ovulation affecting cancer treatment and fertility, Poley et al., ACS nano, 2022

Over years’ transition metal-catalyzed C-H activation has propelled the field of organic synthesis for the construction of structurally complex and diverse molecules in resource-economical fashion. In this context, non-directed C-H activation has gained unprecedented attention for attaining region-specific C-H functionalizations in a step-economic mode. Unlike traditional Fujiwara-Moritani reaction, this approach relies on ligand assistance and thus uses arene as the limiting reagent. However, all existing non-directed C-H functionalizations utilize high thermal energy to induce the functional group which eventually put the regioselectivity at stake. In addition, use of super stoichiometric costly silver salts to regenerate the catalyst produces unwanted metal waste. In aid of developing a more sustainable and environmentally benign approach, we have established a photoredox catalytic system by a merger of palladium/organo-photocatalyst(PC) which forges highly regeiospecific C-H olefination of diverse arenes and heteroarenes. Visible light nullifies the requirement of silver salts and thermal energy in executing “region-resolved” Fujiwara-Moritani reaction.

The major concerns about industrially used catalytic systems today are: i) the high cost of catalysts; ii) the toxicity of heavy transition metals; iii) difficulties in removing trace amounts of toxic-metal residues from the desired product; and, finally, iv) rare transition metal depletion, which does not meet the requirement of sustainable development. Developing environmentally friendly catalysts is an excellent option in this regard. Naturally, the most recent catalyst development trend heralded a new era of metal-free catalysis or catalysts based on earth-abundant, nontoxic, and low-cost metals. This talk will go over our recent advances [1-4] in using small molecules to systematically mimic transition metal-based catalysis. We designed electron transfer catalysis using the smallest polycyclic odd alternant hydrocarbon, phenalenyl (PLY)-based molecules, which was inspired by a completely different field of molecular spin materials [5]. This talk will focus on how to avoid transition metals when performing various cross-coupling catalysis.

Layered materials exhibit unique charge and energy transfer characteristics, making them promising candidates for emerging photophysical and photochemical applications, and particularly in energy conversion and quantum information science. In two-dimensional systems, spatial confinement in a certain dimension causes reduced dielectric screening and enhanced Coulomb interaction compared to bulk materials. Upon light excitation, the relaxation processes of the charge and energy carriers, as well as their rearrangement in the lateral plane, allow for unique and structure-specific interaction dynamics of the electrons and holes in these systems and of their bound states - neutral and charged excitons. In particular, these dimensionality effects induce strong exciton-electron and exciton-hole interactions in doped or gated systems, where optical excitations coexist alongside electronic excitations. These interactions dominate the exciton decay and diffusion and introduce bound three-particle states in such systems. A many-particle theoretical picture of the formation and propagation of these states is crucial for proper tracking and understanding of the interaction pathways, crystal momentum effects, the involved particle-particle coupling and their relation to the underlying structure, dimensionality, and symmetry.