Highly ordered and highly cooperative water with properties of both solid and liquid states has been observed by means of neutron scattering in hydrophobic one-dimensional channels with van der Waals diameter of 0.78 nm. We have found that in the initial stages of adsorption water molecules occupy niches close to pore walls, followed later by the filling of the central pore area. Intensified by confinement, intermolecular water interactions lead to the formation of well-ordered hydrogen-bonded water chains and to the onset of cooperative vibrations. On the other hand, the same intermolecular interactions lead to two relaxation processes, the faster of which is the spontaneous position exchange between two water molecules placed 3.2-4 Å from each other. Self-diffusion in an axial pore direction is the result of those spontaneous random exchanges and is substantially slower than the self-diffusion in bulk water.
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http://dx.doi.org/10.1021/acs.jpclett.9b02303 | DOI Listing |
J Phys Chem Lett
January 2025
Graphene Composite Research Center, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, P. R. China.
The oxygen evolution reaction (OER) is a critical half-reaction in water splitting and metal-air cells. The sensitivity of the OER to the composition and structure of the electrocatalyst presents a significant challenge in elucidating the structure-property relationship. In this study, highly stable single-crystal cobalt carbonate hydroxide [Co(OH)CO, CoCH] was used as a model to investigate the correlations among structure, composition, and reactivity.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, P. R. China.
Crystalline organic semiconductors, recognized for their highly ordered structures and high carrier mobility, have emerged as a focal point in the field of high-performance optoelectronic devices. Nevertheless, the intrinsic unipolar properties, characterized by imbalanced hole and electron transport capabilities, have continuously represented a significant challenge in the advancement of high-performance crystalline thin-film organic light-emitting diodes (C-OLEDs). Here, a bipolar solid-solution thin film with a maintained crystal structure has been fabricated using 2-(4-(9H-carbazol-9-yl)phenyl)-1(3,5-difluorophenyl)-1H-phenanthro [9,10-d]imidazole (2FPPICz) and 4-(1-(3,5-difluorophenyl)-1H-imidazo[4,5-][1,10]phenanthrolin-2-yl)-N,N-diphenylaniline (2Fn) via a weak epitaxial growth (WEG) process, exhibiting nearly equivalent hole and electron mobilities (10-10 cm V s).
View Article and Find Full Text PDFAcc Chem Res
January 2025
Department of Chemistry, Ben-Gurion University of the Negev, Be'er Sheva 84105, Israel.
ConspectusA key challenge in modern chemistry research is to mimic life-like functions using simple molecular networks and the integration of such networks into the first functional artificial cell. Central to this endeavor is the development of signaling elements that can regulate the cell function in time and space by producing entities of code with specific information to induce downstream activity. Such artificial signaling motifs can emerge in nonequilibrium systems, exhibiting complex dynamic behavior like bistability, multistability, oscillations, and chaos.
View Article and Find Full Text PDFSci Adv
January 2025
Department of Biomedical Engineering, Duke University, Durham, NC, USA.
Designing binders to target undruggable proteins presents a formidable challenge in drug discovery. In this work, we provide an algorithmic framework to design short, target-binding linear peptides, requiring only the amino acid sequence of the target protein. To do this, we propose a process to generate naturalistic peptide candidates through Gaussian perturbation of the peptidic latent space of the ESM-2 protein language model and subsequently screen these novel sequences for target-selective interaction activity via a contrastive language-image pretraining (CLIP)-based contrastive learning architecture.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
Institute of Physical Chemistry, RWTH Aachen University, Aachen 52074, Germany.
Exploring the conformational space of molecules remains a challenge of fundamental importance to quantum chemistry: identification of relevant conformers at ambient conditions enables predictive simulations of almost arbitrary properties. Here, we propose a novel approach, called TTConf, to enable conformational sampling of large organic molecules where the combinatorial explosion of possible conformers prevents the use of a brute-force systematic conformer search. We employ tensor trains as a highly efficient dimensionality reduction algorithm, effectively reducing the scaling from exponential to polynomial.
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