Tailoring Spin–Spin Dipolar Interactions by Conformational Locking Toward Room‐Temperature Molecular Qubits
Abstract
Abstract Chichibabin's hydrocarbons (CHs) typically exhibit resonance equilibrium between closed‐shell quinoidal and open‐shell diradical configurations due to the flexible rotation of the molecule structure. We herein report a series of conformationally rigidified CHs achieved through lockage of chiral binaphthalene frameworks. Systematic enhancement of open‐shell character was observed with increasing dihedral angles between naphthalene moieties, as evidenced by electronic spectroscopy and pulse electron paramagnetic resonance (EPR) technique. This conformational locking strategy enables precise engineering of spin–spin dipolar interactions, unambiguously revealed by zero‐field splitting parameters derived from EPR studies. Specifically, CH(2) exhibits excellent ambient stability and exceptional spin coherence at room temperature, with attractive spin‐lattice relaxation time ( T 1 ) of 1207 ns and spin dephasing time ( T m ) of 205 ns. Our findings establish a molecular design paradigm for controlling electronic coupling in diradical systems, providing critical insights for developing next‐generation quantum materials with tailored spin functionalities.
Article Details
Authors (8)
Zhibin Feng
State Key Laboratory of Luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology Guangzhou 510640 P. R. China
Shengyang Chen
Jiadong Zhou
Bohan Wang
Xiaozhen Chen
State Key Laboratory of Luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology Guangzhou 510640 P. R. China
Linlin Liu
Xianfeng Qiao
State Key Laboratory of Luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology Guangzhou 510640 P. R. China
Zengqi Xie
State Key Laboratory of Luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology Guangzhou 510640 P. R. China