Oct 2026· ACS Central Science· 0 citations· 49 references
Abstract
Organic radicals with spin-polarized excited-state manifolds are attractive molecular platforms for quantum information technologies. A central challenge lies in the understanding of how emissive doublet states can communicate with higher-spin quartet states while maintaining efficient luminescence. In this context, we propose here a series of donor-bridge-acceptor radicals based on anthracene or naphthalene donors coupled to the tris(trichlorophenyl)methyl (TTM•) radical acceptor. By combining excited-state electronic-structure analysis with interpolated coordinate pathways, we reveal how the locally excited (LE) states and charge-transfer (CT) states govern the accessibility of quartet manifolds and enable radical-enhanced reverse intersystem crossing (ERISC). Structural variations, including steric hindrance and donor–acceptor spatial separation, are shown to modulate the CT-state characteristics and reshape the LE-CT energy landscape. Our results identify the electronic-structure requirements and molecular design strategies for achieving both optically addressable emission and manipulation of quartet states, two key ingredients for molecular qudit architectures.
Compact naphthalimide-based donor–acceptor–radical triads, together with their corresponding radical-free donor–acceptor dyads, were prepared as a tunable platform for manipulating long-lived excited-state spin dynamics in closely coupled organic multispin systems. Structural analysis and DFT calculations support a com...
Y. Kandrashkin, M. Imran, A. Sukhanov et al.· Chemical Science· 0 citations
The development of near-infrared (NIR) organic lasers has long been constrained by inefficient excited-state intramolecular proton transfer (ESIPT) and limited electronic delocalization, which restrict both performance and scalability. In this study, we demonstrate that subtle molecular modifications can improve lase...
Lei Wang, Jun-Jie Wu, Chang-Cun Yan et al.· Chemistry of Materials· 0 citations
In molecular complexes, ligand-to-metal charge transfer (LMCT) excited states enable efficient photoinduced charge separation and strong redox reactivity, but their operation is typically limited to short ultraviolet excitation. Extending LMCT absorption into the visible region utilizing strongly donating ligands often...
Tian-Na Liu, Wen-Zhe Shang, Wei Che et al.· Angewandte Chemie· 0 citations
Triarylmethyl radicals are among the most prominent stable organic open-shell emitters, combining strong photoluminescence with well-defined spin states. Extending these systems to bridged diradicals introduces spin-spin interactions that are highly sensitive to the radical-radical distance. In this contribution, I wil...
A. Kühne· Organic and Hybrid Light Emi...· 0 citations
Photoinduced symmetry-breaking charge separation (SB-CS) is an electron-transfer between two identical molecules (M) following photoexcitation of one of them (M* + M → M˙+ + M˙-). Compared to conventional photoinduced electron transfer with distinct donor and acceptor moieties, SB-CS offers several advantages for light...
Johannes Wega, E. Vauthey· Physical Chemistry, Chemical...· 0 citations
Substitution of C═C bonds with B-E units (E = N, O, P, etc.) provides a powerful strategy to modulate the electronic structure of π-conjugated frameworks with minimal skeletal perturbation. However, precise control over excited-state processes through heteroatom incorporation remains challenging. Herein, we present a m...
Zhao-Bo Liu, Qing-Yun Ni, Guang-Rui Yang et al.· Angewandte Chemie· 0 citations
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