ACS Physical Chemistry Au最新文献

There has been a recent interest in quantum algorithms for the modeling and prediction of nonunitary quantum dynamics using current quantum computers. The field of quantum biology is one area where these algorithms could prove to be useful as biological systems are generally intractable to treat in their complete form but amenable to an open quantum systems approach. Here, we present the application of a recently developed singular value decomposition (SVD) algorithm to two systems in quantum biology: excitonic energy transport through the Fenna–Matthews–Olson complex and the radical pair mechanism for avian navigation. We demonstrate that the SVD algorithm is capable of capturing accurate short- and long-time dynamics for these systems through implementation on a quantum simulator and conclude that while the implementation of this algorithm is beyond the reach of current quantum computers, it has the potential to be an effective tool for the future study of systems relevant to quantum biology.

Conventional electrodes and electrocatalysts possess complex compositional and structural motifs that impact their overall electrochemical activity. These motifs range from defects and crystal orientation on the electrode surface to layers and composites with other electrode components, such as binders. Therefore, it is vital to identify how these individual motifs alter the electrochemical activity of the electrode. Scanning electrochemical cell microscopy (SECCM) is a powerful tool that has been developed for investigating the electrochemical properties of complex structures. An example of a complex electrode surface is Zn–Al alloys, which are utilized in various sectors ranging from cathodic protection of steel to battery electrodes. Herein, voltammetric SECCM and correlative microstructure analysis are deployed to probe the electrochemical activities of a range of microstructural features, with 651 independent voltammetric measurements made in six distinctive areas on the surface of a Zn–Al alloy. Energy-dispersive X-ray spectroscopy (EDS) mapping reveals that specific phases of the alloy structure, particularly the α-phase Zn–Al, favor the early stages of metal dissolution (i.e., oxidation) and electrochemical reduction processes such as the oxygen reduction reaction (ORR) and redeposition of dissolved metal ions. A correlative analysis performed by comparing high-resolution quantitative elemental composition (i.e., EDS) with the corresponding spatially resolved cyclic voltammograms (i.e., SECCM) shows that the nanospot α-phase of the Zn–Al alloy contains high Al content (30–50%), which may facilitate local Al dissolution as the local pH increases during the ORR in unbuffered aqueous media. Overall, SECCM-based high-throughput electrochemical screening, combined with microstructure analysis, conclusively demonstrates that structure-composition heterogeneity significantly influences the local electrochemical activity on complex electrode surfaces. These insights are invaluable for the rational design of advanced electromaterials.

Water and ice are routinely studied with X-rays to reveal their diverse structures and anomalous properties. We employ a hybrid collisional-radiative/molecular-dynamics method to explore how femtosecond X-ray pulses interact with hexagonal ice. We find that ice makes a phase transition into a crystalline plasma where its initial structure is maintained up to tens of femtoseconds. The ultrafast melting process occurs anisotropically, where different geometric configurations of the structure melt on different time scales. The transient state and anisotropic melting of crystals can be captured by X-ray diffraction, which impacts any study of crystalline structures probed by femtosecond X-ray lasers.

Genetically encoded voltage indicators (GEVIs) have found wide applications as molecular tools for visualization of changes in cell membrane potential. Among others, several classes of archaerhodopsin-3-based GEVIs have been developed and have proved themselves promising in various molecular imaging studies. To expand the application range for this type of GEVIs, new variants with absorption band maxima shifted toward the first biological window and enhanced fluorescence signal are required. Here, we integrate computational and experimental strategies to reveal structural factors that distinguish far-red bright archaerhodopsin-3-based GEVIs, Archers, obtained by directed evolution in a previous study (McIsaac et al., PNAS, 2014) and the wild-type archaerhodopsin-3 with an extremely dim fluorescence signal, aiming to use the obtained information in subsequent rational design. We found that the fluorescence can be enhanced by stabilization of a certain conformation of the protein, which, in turn, can be achieved by tuning the pK_a value of two titratable residues. These findings were supported further by introducing mutations into wild-type archeorhodopsin-3 and detecting the enhancement of the fluorescence signal. Finally, we came up with a rational design and proposed previously unknown Archers variants with red-shifted absorption bands (λ_max up to 640 nm) and potential-dependent bright fluorescence (quantum yield up to 0.97%).

The recent discovery of spin-exciton and magnon-exciton coupling in a layered antiferromagnetic semiconductor, CrSBr, is both fundamentally intriguing and technologically significant. This discovery unveils a unique capability to optically access and manipulate spin information using excitons, opening doors to applications in quantum interconnects, quantum photonics, and opto-spintronics. Despite their remarkable potential, materials exhibiting spin-exciton and magnon-exciton coupling remain limited. To broaden the library of such materials, we explore key parameters for achieving and tuning spin-exciton and magnon-exciton couplings. We begin by examining the mechanisms of couplings in CrSBr and drawing comparisons with other recently identified two-dimensional magnetic semiconductors. Furthermore, we propose various promising scenarios for spin-exciton coupling, laying the groundwork for future research endeavors.