We have numerically examined the effect of site-dependent reorganization on the dynamics of coherent electronic excitation energy transfer in a donor and acceptor pair of photosynthetic pigment-protein complex. Using the quasi-adiabatic propagator path integral method (QUAPI), we have found that a specific proportionality between the site-energy mismatch ϵ and the site-reorganization energy mismatch λ simultaneously increases the length and robustness of the quantum coherence. This behavior is associated with a Rabi type resonance that is manifested in the amplitude and frequency in the coherent portion of the population dynamics. Impact of the resonance on robustness of the coherence under static disorder is also discussed.
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January 2025
Fujian Provincial Key Laboratory of Quantum Manipulation and New Energy Materials, College of Physics and Energy, Fujian Normal University, Fuzhou, Fujian, 350117, China.
Single-atom materials provide a platform to precisely regulate the electrochemical redox behavior of electrode materials with atomic level. Here, a multifield-regulated sintering route is reported to rapidly prepare single-atom zinc with a very high loading mass of 24.7 wt.
View Article and Find Full Text PDFJ Mater Chem B
January 2025
Department of Physics, The Chinese University of Hong Kong, Shatin, Hong Kong SAR, China.
The transmembrane potential of plasma membranes and membrane-bound organelles plays a fundamental role in cellular functions such as signal transduction, ATP synthesis, and homeostasis. Rhodamine voltage reporters (RhoVRs), which operate based on the photoinduced electron transfer (PeT) mechanism, are non-invasive, small-molecule voltage sensors that can detect rapid voltage changes, with some of them specifically targeting the inner mitochondrial membrane. In this work, we conducted extensive molecular dynamics simulations and free-energy calculations to investigate the physicochemical properties governing the orientation as well as membrane permeation barriers of three RhoVRs.
View Article and Find Full Text PDFSmall
January 2025
Department of Polymers & Functional Materials, CSIR-Indian Institute of Chemical Technology (IICT), Tarnaka, Hyderabad, Telangana, 500007, India.
Heterostructures comprise two or more different semiconducting materials stacked either as co-assemblies or self-sorted based on their dynamics of aggregates. However, self-sorting in heterostructures is rather significant in improving the short exciton diffusion length and charge separation. Despite small organic molecules being known for their self-sorting nature, macrocyclic are hitherto unknown owing to unrestrained assemblies from extended π-conjugated systems.
View Article and Find Full Text PDFChem Sci
January 2025
Hunan Key Laboratory of Micro & Nano Materials Interface Science, College of Chemistry and Chemical Engineering, Central South University Changsha 410083 P. R. China
The layer-stacking mode of a two-dimensional (2D) material plays a dominant role either in its topology or properties, but remains challenging to control. Herein, we developed alkali-metal ion-regulating synthetic control on the stacking structure of a vinylene-linked covalent triazine framework (termed spc-CTF) for improving hydrogen peroxide (HO) photoproduction. Upon the catalysis of EtONa in Knoevenagel polycondensation, a typical eclipsed stacking mode (spc-CTF-4@AA) was built, while a staggered one (spc-CTF-4@AB) was constructed using LiOH.
View Article and Find Full Text PDFIn biological systems, heme-copper oxidase (HCO) enzymes play a crucial role in the oxygen reduction reaction (ORR), where the pivotal O-O bond cleavage of the (heme)Fe-peroxo-Cu intermediate is facilitated by active-site (peroxo core) hydrogen bonding followed by proton-coupled electron transfer (PCET) from a nearby (phenolic) tyrosine residue. A useful approach to comprehend the fundamental relationships among H-bonding/proton/H-atom donors and their abilities to induce O-O bond homolysis involves the investigation of synthetic, bioinspired model systems where the exogenous substrate properties (such as p and bond dissociation energy (BDE)) can be systematically altered. This report details the reactivity of a heme-peroxo-copper HCO model complex (LS-4DCHIm) toward a series of substituted catechol substrates that span a range of p and O-H bond BDE values, exhibiting different reaction mechanisms.
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