The nonequilibrium Fermi's golden rule (NE-FGR) describes the time-dependent rate coefficient for electronic transitions when the nuclear degrees of freedom start out in a nonequilibrium state. In this paper, the linearized semiclassical (LSC) approximation of the NE-FGR is used to calculate the photoinduced charge transfer (CT) rates in the carotenoid-porphyrin-C molecular triad dissolved in explicit tetrahydrofuran. The initial nonequilibrium state corresponds to impulsive photoexcitation from the equilibrated ground state to the ππ* state, and the porphyrin-to-C and carotenoid-to-C CT rates are calculated. Our results show that accounting for the nonequilibrium nature of the initial state significantly enhances the transition rate of the porphyrin-to-C CT process. We also derive the instantaneous Marcus theory (IMT) from LSC NE-FGR, which casts the CT rate coefficients in terms of a Marcus-like expression, with explicitly time-dependent reorganization energy and reaction free energy. IMT is found to reproduce the CT rates in the system under consideration remarkably well.
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http://dx.doi.org/10.1021/acs.jpcb.0c06306 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
Henan University of Technology, School of Chemistry and Chemical Engineering, CHINA.
Developing of molecular crystalline materials with light-induced multiple dynamic deformation in space dimension and photochromism on time scales has attracted much attention for its potential applications in actuators, sensoring and information storage. Nevertheless, organic crystals capable of both photoinduced dynamic effects and static color change are rare, particularly for multi-component cocrystals system. In this study, we first report the construction of charge transfer co-crystals allows their light-induced solid-to-liquid transition and photochromic behaviors to be controlled by trans-stilbene (TSB) as an electron donor and 3,4,5,6-Tetrafluorophthalonitrile (TFP) as an electron acceptor.
View Article and Find Full Text PDFChem Commun (Camb)
January 2025
College of Chemistry, Baicheng Normal University, Baicheng 137018, P. R. China.
Herein, the construction of potential donor-acceptor (D-A) structures was guided using density-functional theory (DFT) calculations. The photocatalytic nitrogen fixation performance of TAPT-CHF was then experimentally determined to be 327.58 μmol g h, which was attributed to its efficient photo-induced charge separation and migration ability.
View Article and Find Full Text PDFSensors (Basel)
January 2025
Institute of Physics, University of Tartu, EE-50411 Tartu, Estonia.
Low-power gas sensors that can be used in IoT (Internet of Things) systems, consumer devices, and point-of-care devices will enable new applications in environmental monitoring and health protection. We fabricated a monolithic chemiresistive gas sensor by integrating a micro-lightplate with a 2D sensing material composed of single-layer graphene and monolayer-thick TiO. Applying ultraviolet (380 nm) light with quantum energy above the TiO bandgap effectively enhanced the sensor responses.
View Article and Find Full Text PDFSmall
January 2025
Department of Botany and Microbiology, College of Science, King Saud University, P.O. Box 2455, Riyadh, 11451, Saudi Arabia.
A polyacrylamide gel method has been used to synthesize a variety of polyvalent-transition-metal-doped Ni position of high entropy spinel oxides (NiZnMgCuCo)AlO-800 °C (A) on the basis of NiAlO, and the catalytic activity of A is studied under the synergistic action of peroxymonosulfate (PMS) activation and simulated sunlight. The A containing polyvalent transition metals (Ni, Cu, and Co) can effectively activate PMS and efficiently degrade levofloxacin (LEV) and tetracycline hydrochloride (TCH) under simulated sunlight irradiation. After 90 min of light exposure, the degradation percentages of LEV (50 mg L) and TCH (100 mg L) degrade by the A/PMS/vis system reach 87.
View Article and Find Full Text PDFAnal Chim Acta
February 2025
Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University) Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing, PR China. Electronic address:
Background: Sensitive and accurate detection of important cancer markers MicroRNAs (miRNAs) is critical to prevent and treat disease. Among many detection techniques, surface-enhanced Raman scattering(SERS) has attracted much attention due to its advantages such as narrow spectral peak, low interference and non-destructive detection. Interestingly, non-noble metal SERS substrates show good prospects due to their outstanding spectral reproducibility and biocompatibility.
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