@article{19024, abstract = {Aqueous two-phase systems (ATPSs), phase-separating solutions of water soluble but mutually immiscible molecular species, offer fascinating prospects for selective partitioning, purification, and extraction. Here, we formulate a general Brownian dynamics based coarse-grained simulation model for an ATPS of two water soluble but mutually immiscible polymer species. Including additional solute species into the model is straightforward, which enables capturing the assembly and partitioning response of, e.g., nanoparticles (NPs), additional macromolecular species, or impurities in the ATPS. We demonstrate that the simulation model captures satisfactorily the phase separation, partitioning, and interfacial properties of an actual ATPS using a model ATPS in which a polymer mixture of dextran and polyethylene glycol (PEG) phase separates, and magnetic NPs selectively partition into one of the two polymeric phases. Phase separation and NP partitioning are characterized both via the computational model and experimentally, under different conditions. The simulation model captures the trends observed in the experimental system and quantitatively links the partitioning behavior to the component species interactions. Finally, the simulation model reveals that the ATPS interface fluctuations in systems with magnetic NPs as a partitioned species can be controlled by the magnetic field at length scales much smaller than those probed experimentally to date.}, author = {Scacchi, Alberto and Rigoni, Carlo and Haataja, Mikko and Timonen, Jaakko V.I. and Sammalkorpi, Maria}, issn = {1095-7103}, journal = {Journal of Colloid and Interface Science}, pages = {1135--1146}, publisher = {Elsevier}, title = {{A coarse-grained model for aqueous two-phase systems: Application to ferrofluids}}, doi = {10.1016/j.jcis.2025.01.256}, volume = {686}, year = {2025}, } @misc{19033, abstract = {This data set contains the simulation input files, scripts, and figures data belonging to the publication Alberto Scacchi, Carlo Rigoni, Mikko P. Haataja, Jakko V. I. Timonen, and Maria Sammalkorpi, "A Coarse-grained Model for Aqueous Two-phase Systems: Application to Ferrofluids", Journal of Colloids and Interface Science (2025). https://doi.org/10.1016/j.jcis.2025.01.256.}, author = {Scacchi, Alberto}, publisher = {Fairdata}, title = {{2025_SCACCHI_JCIS}}, doi = {10.23729/4fb80194-cdb2-4f49-94f4-f8a87b8e29c1}, year = {2025}, } @article{19277, abstract = {Light-driven molecular rotary motors perform chirality-controlled unidirectional rotations fueled by light and heat. This unique function renders them appealing for the construction of dynamic molecular systems, actuating materials, and molecular machines. Achieving a combination of high photoefficiency, visible-light responsiveness, synthetic accessibility, and easy tuning of dynamic properties within a single scaffold is critical for these applications but remains a longstanding challenge. Herein, a series of highly photoefficient visible-light–responsive molecular motors (MMs), featuring various rotary speeds, was obtained by a convenient one-step formylation of their parent motors. This strategy greatly improves all aspects of the performance of MMs—red-shifted wavelengths of excitation, high photoisomerization quantum yields, and high photostationary state distributions of isomers—beyond the state-of-the-art light-responsive MM systems. The development of this late-stage functionalization strategy of MMs opens avenues for the construction of high-performance molecular machines and devices for applications in materials science and biological systems, representing a major advance in the synthetic toolbox of molecular machines.}, author = {Sheng, Jinyu and Van Beek, Carlijn L.F. and Stindt, Charlotte N. and Danowski, Wojciech and Jankowska, Joanna and Crespi, Stefano and Pooler, Daisy R.S. and Hilbers, Michiel F. and Buma, Wybren Jan and Feringa, Ben L.}, issn = {2375-2548}, journal = {Science Advances}, number = {8}, publisher = {AAAS}, title = {{General strategy for boosting the performance of speed-tunable rotary molecular motors with visible light}}, doi = {10.1126/sciadv.adr9326}, volume = {11}, year = {2025}, } @article{20933, abstract = {Photo-responsive systems based on azobenzenes usually require UV light for E→Z isomerization, limiting their applicability, especially in biomedical contexts. Disequilibration by sensitization of azobenzene under confinement (DESC) has recently emerged as a supramolecular strategy to bypass this limitation without the need to derivatize the azobenzene scaffold. Here, we expand DESC to water-soluble azopolymers obtained by RAFT polymerization and systematically investigate the interplay between the polymer structure and DESC efficiency. Using this approach, we achieved as much as 85% of the direct photoexcitation (UV) switching efficiency, while utilizing low-energy (yellow) light. These results establish general design principles for combining DESC with polymeric systems, opening new opportunities for the development of functional materials driven with low-energy light.}, author = {Meteling, Henning Jörn and Gemen, Julius and Häkkinen, Satu and Klajn, Rafal and Priimagi, Arri}, issn = {1521-3773}, journal = {Angewandte Chemie International Edition}, publisher = {Wiley}, title = {{Sensitized disequilibration of water-soluble azopolymers}}, doi = {10.1002/anie.202523447}, year = {2025}, } @article{18451, abstract = {Inorganic nanoparticles can be assembled into superlattices with unique optical and magnetic properties arising from collective behavior. Protein cages can be utilized to guide this assembly by encapsulating nanoparticles and promoting their assembly into ordered structures. However, creating ordered multi-component structures with different protein cage types and sizes remains a challenge. Here, the co-crystallization of two different protein cages (cowpea chlorotic mottle virus and ferritin) characterized by opposing surface charges and unequal diameter is shown. Precise tuning of the electrostatic attraction between the cages enabled the preparation of binary crystals with dimensions up to several tens of micrometers. Additionally, binary metal nanoparticle superlattices are achieved by loading gold and iron oxide nanoparticles inside the cavities of the protein cages. The resulting structure adopts an AB2FCC configuration that also impacts the dipolar coupling between the particles and hence the optical properties of the crystals, providing key insight for the future preparation of plasmonic and magnetic nanoparticle metamaterials.}, author = {Zhou, Yu and Shaukat, Ahmed and Seitsonen, Jani and Rigoni, Carlo and Timonen, Jaakko V.I. and Kostiainen, Mauri A.}, issn = {2198-3844}, journal = {Advanced Science}, number = {45}, publisher = {Wiley}, title = {{Protein cage directed assembly of binary nanoparticle superlattices}}, doi = {10.1002/advs.202408416}, volume = {11}, year = {2024}, } @article{17054, abstract = {Photoisomerization and photoluminescence are two distinct energy dissipation pathways in light-driven molecular motors. The photoisomerization properties of discrete molecular motors have been well established in solution, but their photoluminescent properties have been rarely reported—especially in aggregates. Here, it is shown that an overcrowded alkene-based molecular motor exhibits distinct dynamic properties in solution and aggregate states, for example, gel and solid states. Despite the poor emissive properties of molecular motors in solution, a bright emission is observed in the aggregate states, including in gel and the crystalline solid. The emission wavelength is highly dependent on the nature of the supramolecular packing and order in the aggregates. As a result, the fluorescent color can be readily tuned reversibly via mechanical grinding and vapor fuming, which provides a new platform for developing multi-stimuli functional materials.}, author = {Shan, Yahan and Sheng, Jinyu and Zhang, Qi and Stuart, Marc C.A. and Qu, Da Hui and Feringa, Ben L.}, issn = {2692-4560}, journal = {Aggregate}, number = {5}, publisher = {Wiley}, title = {{Multi-state photoluminescent properties of an overcrowded alkene-based molecular motor in aggregates}}, doi = {10.1002/agt2.584}, volume = {5}, year = {2024}, } @article{17105, abstract = {The development of photoresponsive systems with non-invasive orthogonal control by distinct wavelengths of light is still in its infancy. In particular, the design of photochemically triggered-orthogonal systems integrated into solid materials that enable multiple dynamic control over their properties remains a longstanding challenge. Here, we report the orthogonal and reversible control of two types of photoswitches in an integrated solid porous framework, that is, visible-light responsive o-fluoroazobenzene and nitro-spiropyran motifs. The properties of the constructed material can be selectively controlled by different wavelengths of light thus generating four distinct states providing a basis for dynamic multifunctional materials. Solid-state NMR spectroscopy demonstrated the selective transformation of the azobenzene switch in the bulk, which in turn modulates N2 and CO2 adsorption.}, author = {Sheng, Jinyu and Perego, Jacopo and Bracco, Silvia and Cieciórski, Piotr and Danowski, Wojciech and Comotti, Angiolina and Feringa, Ben L.}, issn = {1521-3773}, journal = {Angewandte Chemie International Edition}, number = {23}, publisher = {Wiley}, title = {{Orthogonal photoswitching in a porous organic framework}}, doi = {10.1002/anie.202404878}, volume = {63}, year = {2024}, } @article{17409, abstract = {Light-driven rotary molecular motors are among the most promising classes of responsive molecular machines and take advantage of their intrinsic chirality which governs unidirectional rotation. As a consequence of their dynamic function, they receive considerable interest in the areas of supramolecular chemistry, asymmetric catalysis and responsive materials. Among the emerging classes of responsive photochromic molecules, multistate first-generation molecular motors driven by benign visible light remain unexplored, which limits the exploitation of the full potential of these mechanical light-powered systems. Herein, we describe a series of all-visible-light-driven first-generation molecular motors based on the salicylidene Schiff base functionality. Remarkable redshifts up to 100 nm in absorption are achieved compared to conventional first-generation motor structures. Taking advantage of all-visible-light-driven multistate motor scaffolds, adaptive behaviour is found as well, and potential application in multistate photoluminescence is demonstrated. These functional visible-light-responsive motors will likely stimulate the design and synthesis of more sophisticated nanomachinery with a myriad of future applications in powering dynamic systems.}, author = {Van Vliet, Sven and Sheng, Jinyu and Stindt, Charlotte N. and Feringa, Ben L.}, issn = {2041-1723}, journal = {Nature Communications}, publisher = {Springer Nature}, title = {{All-visible-light-driven salicylidene schiff-base-functionalized artificial molecular motors}}, doi = {10.1038/s41467-024-50587-4}, volume = {15}, year = {2024}, } @article{14664, abstract = {The architecture of self-assembled host molecules can profoundly affect the properties of the encapsulated guests. For example, a rigid cage with small windows can efficiently protect its contents from the environment; in contrast, tube-shaped, flexible hosts with large openings and an easily accessible cavity are ideally suited for catalysis. Here, we report a “Janus” nature of a Pd6L4 coordination host previously reported to exist exclusively as a tube isomer (T). We show that upon encapsulating various tetrahedrally shaped guests, T can reconfigure into a cage-shaped host (C) in quantitative yield. Extracting the guest affords empty C, which is metastable and spontaneously relaxes to T, and the T⇄C interconversion can be repeated for multiple cycles. Reversible toggling between two vastly different isomers paves the way toward controlling functional properties of coordination hosts “on demand”.}, author = {Hema, Kuntrapakam and Grommet, Angela B. and Białek, Michał J. and Wang, Jinhua and Schneider, Laura and Drechsler, Christoph and Yanshyna, Oksana and Diskin-Posner, Yael and Clever, Guido H. and Klajn, Rafal}, issn = {1520-5126}, journal = {Journal of the American Chemical Society}, number = {45}, pages = {24755--24764}, publisher = {American Chemical Society}, title = {{Guest encapsulation alters the thermodynamic landscape of a coordination host}}, doi = {10.1021/jacs.3c08666}, volume = {145}, year = {2023}, } @article{13340, abstract = {Photoisomerization of azobenzenes from their stable E isomer to the metastable Z state is the basis of numerous applications of these molecules. However, this reaction typically requires ultraviolet light, which limits applicability. In this study, we introduce disequilibration by sensitization under confinement (DESC), a supramolecular approach to induce the E-to-Z isomerization by using light of a desired color, including red. DESC relies on a combination of a macrocyclic host and a photosensitizer, which act together to selectively bind and sensitize E-azobenzenes for isomerization. The Z isomer lacks strong affinity for and is expelled from the host, which can then convert additional E-azobenzenes to the Z state. In this way, the host–photosensitizer complex converts photon energy into chemical energy in the form of out-of-equilibrium photostationary states, including ones that cannot be accessed through direct photoexcitation.}, author = {Gemen, Julius and Church, Jonathan R. and Ruoko, Tero-Petri and Durandin, Nikita and Białek, Michał J. and Weissenfels, Maren and Feller, Moran and Kazes, Miri and Borin, Veniamin A. and Odaybat, Magdalena and Kalepu, Rishir and Diskin-Posner, Yael and Oron, Dan and Fuchter, Matthew J. and Priimagi, Arri and Schapiro, Igor and Klajn, Rafal}, issn = {1095-9203}, journal = {Science}, number = {6664}, pages = {1357--1363}, publisher = {American Association for the Advancement of Science}, title = {{Disequilibrating azoarenes by visible-light sensitization under confinement}}, doi = {10.1126/science.adh9059}, volume = {381}, year = {2023}, }