@article{MTMT:34755606, title = {Water–lipid interface in lipidic mesophases with excess water}, url = {https://m2.mtmt.hu/api/publication/34755606}, author = {Yao, Yang and Catalini, Sara and Foggi, Paolo and Mezzenga, Raffaele}, doi = {10.1039/D3FD00118K}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, volume = {249}, unique-id = {34755606}, issn = {1359-6640}, abstract = {We study the influence of excess water on the phase transition of lipidic mesophases from the cubic to reverse hexagonal phase. Excess water permeates the interface and forms additional hydrogen bonds with lipids, accelerating the lipid dynamics.}, year = {2024}, eissn = {1364-5498}, pages = {469-484}, orcid-numbers = {Yao, Yang/0000-0002-4487-651X; Catalini, Sara/0000-0002-8169-3552; Foggi, Paolo/0000-0002-2985-6721; Mezzenga, Raffaele/0000-0002-5739-2610} } @article{MTMT:34450268, title = {Are SAXS and SANS suitable to extract information on the role of water for electric-double-layer formation at the carbon-aqueous-electrolyte interface?}, url = {https://m2.mtmt.hu/api/publication/34450268}, author = {Seyffertitz, M. and Stock, S. and Rauscher, M.V. and Prehal, C. and Haas, S. and Porcar, L. and Paris, O.}, doi = {10.1039/d3fd00124e}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, volume = {249}, unique-id = {34450268}, issn = {1359-6640}, year = {2024}, eissn = {1364-5498}, pages = {363-380} } @article{MTMT:34771104, title = {Substrate effect on charging of electrified graphene/water interfaces}, url = {https://m2.mtmt.hu/api/publication/34771104}, author = {Wang, Y. and Nagata, Y. and Bonn, M.}, doi = {10.1039/d3fd00107e}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, volume = {249}, unique-id = {34771104}, issn = {1359-6640}, year = {2023}, eissn = {1364-5498}, pages = {303-316} } @article{MTMT:34658455, title = {Reducing undesired solubility of squarephaneic tetraimide for use as an organic battery electrode material}, url = {https://m2.mtmt.hu/api/publication/34658455}, author = {Ding, Bowen and Bhosale, Manik and Bennett, Troy L. R. and Heeney, Martin and Plasser, Felix and Esser, Birgit and Gloecklhofer, Florian}, doi = {10.1039/d3fd00145h}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, unique-id = {34658455}, issn = {1359-6640}, year = {2023}, eissn = {1364-5498}, orcid-numbers = {Heeney, Martin/0000-0001-6879-5020; Plasser, Felix/0000-0003-0751-148X; Esser, Birgit/0000-0002-2430-1380} } @article{MTMT:34608759, title = {Morphology, dynamic disorder, and charge transport in an indoloindole-based hole-transporting material from a multi-level theoretical approach}, url = {https://m2.mtmt.hu/api/publication/34608759}, author = {Perez-Escribano, Manuel and Fernandez-Alarcon, Alberto and Orti, Enrique and Arago, Juan and Cerda, Jesus and Calbo, Joaquin}, doi = {10.1039/d3fd00144j}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, unique-id = {34608759}, issn = {1359-6640}, abstract = {The exponential effort in the design of hole-transporting materials (HTMs) during the last decade has been motivated by their key role as p-type semiconductors for (opto)electronics. Although structure-property relationships have been successfully rationalized to decipher optimal site substitutions, aliphatic chain lengths or efficient aromatic cores for enhanced charge conduction, the impact of molecular shape, material morphology and dynamic disorder has been generally overlooked. In this work, we characterize by means of a multi-level theoretical approach the charge transport properties of a novel planar small-molecule HTM based on the indoloindole aromatic core (IDIDF), and compare it with spherical spiro-OMeTAD. Hybrid DFT calculations predict moderate band dispersions in IDIDF associated to the main transport direction characterized by pi-pi stacked molecules, both between the indoloindole cores and the thiophene groups. Strongly coupled dimers show relevant non-covalent interactions (NCI), indicating that NCI surfaces are a necessary but not exclusive requirement for large electronic couplings. We evidence remarkable differences in the site energy standard deviation and electronic coupling distributions between the conduction paths of IDIDF and spiro-OMeTAD. Despite the spherical vs. planar shape, theoretical calculations predict in the static crystal strong direction-dependent charge transport in the two HTMs, with ca. one-order-of-magnitude higher mobility (mu) for IDIDF. The dynamical disorder promoted by finite temperature effects in the crystal leads to a reduction in the hole transport properties in both HTMs, with maximum mu values of 2.42 and 4.2 x 10-2 cm2 V-1 s-1 for IDIDF and spiro-OMeTAD, respectively, as well as a significant increase in the transport anisotropy in the latter. Finally, the impact of the material amorphousness in the hole mobility is analysed by modelling a fully random distribution of HTM molecules. An average (lower-bound) mobility of 1.1 x 10-3 and 4.9 x 10-5 cm2 V-1 s-1 is predicted for planar IDIDF and spherical spiro-OMeTAD, respectively, in good accord with the experimental data registered in thin-film devices. Our results demonstrate the strong influence of molecular shape, dynamic structural fluctuations and crystal morphology on the charge transport, and pose indoloindole-based HTMs as promising materials for organic electronics and photovoltaics.A multi-level theoretical protocol is developed to characterize the charge transport of a novel indoloindole-based hole-transporting material. The implications of molecular shape, dynamic disorder and amorphousness on the hole mobilities are discussed.}, year = {2023}, eissn = {1364-5498}, orcid-numbers = {Orti, Enrique/0000-0001-9544-8286; Arago, Juan/0000-0002-0415-9946} } @article{MTMT:34311923, title = {How do water-mediated interactions and osmotic second virial coefficients vary with particle size?}, url = {https://m2.mtmt.hu/api/publication/34311923}, author = {Naito, Hidefumi and Sumi, Tomonari and Koga, Kenichiro}, doi = {10.1039/d3fd00104k}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, unique-id = {34311923}, issn = {1359-6640}, abstract = {We examine quantitatively the solute-size dependences of the effective interactions between nonpolar solutes in water and in a simple liquid. The potential w(r) of mean force and the osmotic second virial coefficients B are calculated with high accuracy from molecular dynamics simulations. As the solute diameter increases from methane's to C-60's with the solute-solute and solute-solvent attractive interaction parameters fixed to those for the methane-methane and methane-water interactions, the first minimum of w(r) lowers from -1.1 to -4.7 in units of the thermal energy kT. Correspondingly, the magnitude of B (<0) increases proportional to sigma(alpha) with some power close to 6 or 7, which reinforces the solute-size dependence of B found earlier for a smaller range of sigma [H. Naito, R. Okamoto, T. Sumi and K. Koga, J. Chem. Phys., 2022, 156, 221104]. We also demonstrate that the strength of the attractive interactions between solute and solvent molecules can qualitatively change the characteristics of the effective pair interaction between solute particles, both in water and in a simple liquid. If the solute-solvent attractive force is set to be weaker (stronger) than a threshold, the effective interaction becomes increasingly attractive (repulsive) with increasing solute size.}, year = {2023}, eissn = {1364-5498}, orcid-numbers = {Sumi, Tomonari/0000-0002-4230-5908; Koga, Kenichiro/0000-0002-1153-5831} } @article{MTMT:34303997, title = {Substrate effect on charging of electrified graphene/water interfaces}, url = {https://m2.mtmt.hu/api/publication/34303997}, author = {Wang, Yongkang and Nagata, Yuki and Bonn, Mischa}, doi = {10.1039/d3fd00107}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, unique-id = {34303997}, issn = {1359-6640}, 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. An increasing number of studies indicate that the substrate, rather than graphene, determines the organization of water in contact with graphene, i.e., the electric double layer (EDL) structure near the electrified graphene, and the wetting behavior of the graphene: the graphene sheet is transparent in terms of its supporting substrate. By applying surface-specific heterodyne-detected sum-frequency generation (HD-SFG) spectroscopy to the silicon dioxide (SiO2)-supported graphene electrode/aqueous electrolyte interface and comparing the data with those for the calcium fluoride (CaF2)-supported graphene [Y. Wang et al., Angew. Chem., Int. Ed., 2023, 62, e202216604], we discuss the impact of the different substrates on the charging of both the graphene and the substrate upon applying potentials. The SiO2-supported graphene shows pseudocapacitive behavior, consistent with the CaF2-supported graphene case, although the surface charges on SiO2 and CaF2 differ substantially. The SiO2 surface is already negatively charged at +0.57 V (vs. Pd/H2), and the negative surface charge is doubled when negative potentials are applied, in contrast with the CaF2 case, where the positive charge is reduced when negative potentials are applied. Interestingly, the charging of the graphene sheet is almost identical between the negatively charged SiO2 surface and positively charged CaF2 surface, demonstrating that the graphene charging is decoupled from the charging of the substrates.Surface-specific spectroscopy study of buried graphene electrodes, supported on different substrates, reveals that graphene charging is decoupled from the charging of its substrate. The substrate governs the reorganization of interfacial water.}, year = {2023}, eissn = {1364-5498}, orcid-numbers = {Bonn, Mischa/0000-0001-6851-8453} } @article{MTMT:34300181, title = {The limit of macroscopic homogeneous ice nucleation at the nanoscale}, url = {https://m2.mtmt.hu/api/publication/34300181}, author = {Hayton, John A. and Davies, Michael B. and Whale, Thomas F. and Michaelides, Angelos and Cox, Stephen J.}, doi = {10.1039/d3fd00099}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, unique-id = {34300181}, issn = {1359-6640}, abstract = {Nucleation in small volumes of water has garnered renewed interest due to the relevance of pore condensation and freezing under conditions of low partial pressures of water, such as in the upper troposphere. Molecular simulations can in principle provide insight on this process at the molecular scale that is challenging to achieve experimentally. However, there are discrepancies in the literature as to whether the rate in confined systems is enhanced or suppressed relative to bulk water at the same temperature and pressure. In this study, we investigate the extent to which the size of the critical nucleus and the rate at which it grows in thin films of water are affected by the thickness of the film. Our results suggest that nucleation remains bulk-like in films that are barely large enough accommodate a critical nucleus. This conclusion seems robust to the presence of physical confining boundaries. We also discuss the difficulties in unambiguously determining homogeneous nucleation rates in nanoscale systems, owing to the challenges in defining the volume. Our results suggest any impact on a film's thickness on the rate is largely inconsequential for present day experiments.We investigate the extent to which the size of the critical nucleus and the rate at which it grows in thin films of water are affected by the thickness of the film.}, year = {2023}, eissn = {1364-5498} } @article{MTMT:34298296, title = {The chemical inventory of the inner regions of planet-forming disks - the JWST/MINDS program}, url = {https://m2.mtmt.hu/api/publication/34298296}, author = {Kamp, Inga and Henning, Thomas and Arabhavi, Aditya M. and Bettoni, Giulio and Christiaens, Valentin and Gasman, Danny and Grant, Sierra L. and Morales-Calderon, Maria and Tabone, Benoit and Abergel, Alain and Absil, Olivier and Argyriou, Ioannis and Barrado, David and Boccaletti, Anthony and Bouwman, Jeroen and Garatti, Alessio and van Dishoeck, Ewine F. and Geers, Vincent and Glauser, Adrian M. and Guedel, Manuel and Guadarrama, Rodrigo and Jang, Hyerin and Kanwar, Jayatee and Lagage, Pierre-Olivier and Lahuis, Fred and Mueller, Michael and Nehme, Cyrine and Olofsson, Goeran and Pantin, Eric and Pawellek, Nicole and Perotti, Giulia and Ray, Tom P. and Rodgers-Lee, Donna and Samland, Matthias and Scheithauer, Silvia and Schreiber, Juergen and Schwarz, Kamber and Temmink, Milou and Vandenbussche, Bart and Vlasblom, Marissa and Waelkens, Christoffel and Waters, L. B. F. M. and Wright, Gillian}, doi = {10.1039/d3fd00013c}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, volume = {245}, unique-id = {34298296}, issn = {1359-6640}, abstract = {The understanding of planet formation has changed recently, embracing the new idea of pebble accretion. This means that the influx of pebbles from the outer regions of planet-forming disks to their inner zones could determine the composition of planets and their atmospheres. The solid and molecular components delivered to the planet-forming region can be best characterized by mid-infrared spectroscopy. With Spitzer low-resolution (R = 100, 600) spectroscopy, this approach was limited to the detection of abundant molecules, such as H2O, C2H2, HCN and CO2. This contribution will present the first results of the MINDS (MIRI mid-INfrared Disk Survey, PI:Th Henning) project. Due do the sensitivity and spectral resolution provided by the James Webb Space Telescope (JWST), we now have a unique tool to obtain the full inventory of chemistry in the inner disks of solar-type stars and brown dwarfs, including also less-abundant hydrocarbons and isotopologues. The Integral Field Unit (IFU) capabilities will enable at the same time spatial studies of the continuum and line emission in extended sources such as debris disks, the flying saucer and also the search for mid-IR signatures of forming planets in systems such as PDS 70. These JWST observations are complementary to ALMA and NOEMA observations of outer-disk chemistry; together these datasets will provide an integral view of the processes occurring during the planet-formation phase.}, year = {2023}, eissn = {1364-5498}, pages = {112-137}, orcid-numbers = {Bettoni, Giulio/0000-0002-5115-2464; Christiaens, Valentin/0000-0002-0101-8814; Gasman, Danny/0000-0002-1257-7742; Argyriou, Ioannis/0000-0003-2820-1077; Perotti, Giulia/0000-0002-8545-6175} } @article{MTMT:34136908, title = {Model - State-of-the-art modelling and computational analysis of reactive sites: General discussion}, url = {https://m2.mtmt.hu/api/publication/34136908}, author = {Chanbasha, B. and Costas, M. and Echeverría, J. and Eisenstein, O. and Greenhalgh, M. and Kennepohl, P. and Kirrander, A. and Linnebank, P.R. and MacGregor, S.A. and Mahmudov, K.T. and Martín-Fernández, C. and Meeus, E. and Morris, J. and Perutz, R.N. and Poater, A. and Reek, J.N.H. and Rouse, I. and Toste, D. and Trujillo, C. and Ward, T.R. and Weinstein, J.A. and Weller, A.S.}, doi = {10.1039/d3fd90015k}, journal-iso = {FARADAY DISCUSS}, journal = {FARADAY DISCUSSIONS}, volume = {244}, unique-id = {34136908}, issn = {1359-6640}, year = {2023}, eissn = {1364-5498}, pages = {336-355} }