Understanding how the conformational change of conjugated molecules with acceptor-donor-acceptor (A-D-A) architecture affects their physical and optoelectronic properties is critical for determining their ultimate performance in organic electronic devices. Here, we utilized femtosecond transient absorption, time-resolved upconversion photoluminescence spectroscopy, and tunable femtosecond-stimulated Raman spectroscopy, aided by quantum chemical calculations, to systematically investigate the excited state structural dynamics of the intramolecular charge transfer of the tetramethoxy anthracene-based fluorophore 2,3,6,7-tetramethoxy 9,10-dibenzaldehydeanthracene (AnDA) and its derivative 2,3,6,7-tetramethoxy 9,10-diphenylanthracene (TMDPAn) in chloroform. In the AnDA molecule, the tetramethoxy anthracene and benzaldehyde moieties exhibit a strong ability to donate and withdraw electrons. Upon photoexcitation, AnDA shows intriguing ultrafast fluorescence switch-on and red shift dynamics on charge transfer states, and the temporal evolution of AnDA recorded by ultrafast spectroscopy reveals a dynamic picture of two-step intramolecular charge transfer assisted by ultrafast conformational changes and solvation processes. Removing the aldehyde group from TMDPAn significantly decreases the electron pulling capacity of the phenyl unit and disables charge transfer characteristics.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1021/acs.jpcb.1c05936 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Data-Driven Discovery of High-Performance Heterobilayer Transition Metal Dichalcogenide-Based Sliding Ferroelectrics.
ACS Appl Mater Interfaces
January 2025
Department of Mechanical Engineering, National University of Singapore, Singapore 117575, Singapore.
The development of efficient sliding ferroelectric (FE) materials is crucial for advancing next-generation low-power nanodevices. Currently, most efforts focus on homobilayer two-dimensional materials, except for the experimentally reported heterobilayer sliding FE, MoS/WS. Here, we first screened 870 transition metal dichalcogenide (TMD) bilayer heterostructures derived from experimentally characterized monolayer TMDs and systematically investigated their sliding ferroelectric behavior across various stacking configurations using high-throughput calculations.
View Article and Find Full Text PDFDeciphering and Enhancing Rate-Determining Step of Sodium Deposition towards Ultralow-Temperature Sodium Metal Batteries.
Angew Chem Int Ed Engl
January 2025
National University of Singapore, Chemistry, 3 Science Drive 3, 117543, Singapore, SINGAPORE.
Achieving high ionic conductivity and stable performance at low temperatures remains a significant challenge in sodium-metal batteries (SMBs). In this study, we propose a novel electrolyte design strategy that elucidates the solvation structure-function relationship within mixed solvent systems. A mixture of diglyme and 1,3-dioxolane was developed to optimize the solvation structure towards superior low-temperature electrolyte.
View Article and Find Full Text PDFManipulating Charge Distribution at Organic-inorganic Interface via Optimizing Substituents for Sustainable Water Electrolysis.
Angew Chem Int Ed Engl
January 2025
Anhui Normal University, School of Chemistry and Materials Science, CHINA.
The space charge effect induced by high-quality heterojunctions is essential for efficient electrocatalytic processes. Herein, we delicately manipulate intermolecular charge transfer by modifying substituents (-g = -CH3, -H, -NO2) with various electron donating/withdrawing capabilities in CoPc-g/CoS organic-inorganic heterostructures. CoPc-CH3, as a typical electron donor, transfers more electrons to CoS due to the presence of -CH3, forming the strongest space electric field and thus regulating the dual active sites at the interface.
View Article and Find Full Text PDFIngeniously regulating the conformational equilibrium and ESPT mechanism of HBT-DPI by solvent environment: A novel perspective.
Spectrochim Acta A Mol Biomol Spectrosc
January 2025
Jilin Key Laboratory of Solid-State Laser Technology and Application, School of Physics, Changchun University of Science and Technology, Changchun 130022 China. Electronic address:
HBT-DPI was a single-molecule multi-conformational fluorescent material and had unique applications for hydrophobic/hydrophilic mapping on large-scale heterogeneous surfaces. In this paper, the different proton transfer processes and luminescence mechanisms of HBT-DPI in Dichloromethane (DCM, no hydrogen bond (HB) receptor) and N, N-Dimethylformamide (DMF, HB receptor) solvents were systematically studied. Using the quantum chemistry method, the stable structures of HBT-DPI in two solvents were determined based on the Boltzmann distribution.
View Article and Find Full Text PDFPolyaniline-ZnTi-LDH heterostructure with d-π coupling for enhanced photocatalysis of pollutant removal.
J Colloid Interface Sci
January 2025
School of Chemistry and Chemical Engineering, Central South University, Changsha 410083, Hunan, China. Electronic address:
Heterointerface engineering is an effective strategy to design and construct high-performance photocatalysts. Herein, polyaniline (PANI) nanoparticles and ZnTi layered double hydroxide (ZnTi-LDH) nanosheets were integrated to form organic-inorganic heterostructure (PANI/LDH) via d-π electronic coupling using in-situ polymerization for photocatalytic oxidation/reduction towards tetracycline (TC) and Cr(VI). The photocatalytic activity was closely related to feed amount of aniline (Ani) in the polymerization process, which the abundant PANI nanoparticles were evenly distributed on the surface of ZnTi-LDH nanosheets at the proper Ani feed amount, and thus reinforced d-π electronic coupling at the organic-inorganic interfaces more efficiently.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!