Stable organic radicals represent a unique type of functional materials for a broad scope of applications in optoelectronic and spintronic devices. A central challenge toward these applications is how to suppress the inter-radical aggregation that often causes aggregation-induced photoluminescence quenching and limits the correlation lifetime of the electron spins from the radicals. Here, we report an effective approach to fine-tuning luminescence and spin dynamics using a series of polyester-tethered single radicals, with a common core of carbazole-triphenylmethyl radical but different chains of polyesters with distinct glass transition temperature and rigidity. The rigidity of the polymeric matrices plays a critical role in tuning the luminescence and electron spin resonance of the radicals. The tunable properties of luminescence and electron spin dynamics as well as the robust photostability of such polymer-tethered single radicals represent important attributes for cutting-edge applications in optoelectronic devices and quantum information technologies.
Electronic or nuclear spins such as inorganic ‘nitrogen-vacancy’ centers in diamond and other defects in silicon represent a promising type of quantum bits (qubits) for applications in quantum information processing, data storage as well as quantum sensing. However, it remains challenging to achieve scalable and spatially defined organization of a large number of spins as qubits. Therefore, development of new materials and technologies to regulate spin-spin distance and interaction plays an important role in preservation of quantum coherence and realization of coherent exchange of information between spin qubits. Herein, we report that spatially defined organization of organic radicals as electronic spins can be realized via a strategy of block copolymer self-assembly. We demonstrate quantum coherence and spin-lattice relaxation of organic luminescent radical spins can be facilely tuned using a library of well-defined star-like block copolymers containing a common core of tris[4-(p-benzyl)-2,6-dichlorophenyl]methyl radical in the center, from which diblock polyesters are grafted via controllable ring-opening polymerization. The fine tuning of the incompatibility and the volume ratio of the two blocks of polyesters leads to not only a series of self-assembling patterns (i.e., spheres, cylinders, lamellae, and gyroids) with phase-separation of the spins in the nanometer scale, but also tunable spin-lattice relaxation dynamics and spin coherence lifetimes that strongly depend on the lengths and rigidities of the polymeric matrices surrounding the organic radicals as molecular spins. Such strategy of block copolymer self-assembly may offer a generally applicable approach to integrating and organizing molecular spins as promising qubits into scalable architectures and functional devices towards cutting-edge applications in quantum information processing, quantum computation and spintronics.
Stable organic radicals represent a unique type of functional materials for a broad scope of applications in optoelectronic and spintronic devices. A central challenge towards these applications is how to suppress the inter-radical aggregation that often causes aggregation-induced photoluminescence quenching and limits the correlation lifetime of the electron spins from the radicals. Here we report an effective approach to fine-tuning luminescence and spin dynamics using a series of polyester-tethered single radicals, with a common core of carbazole-triphenylmethyl radical but different chains of polyesters with distinct glass transition temperature and rigidity. The rigidity of the polymeric matrices plays a critical role in tuning the luminescence and electron spin resonance of the radicals. The tunable properties of luminescence and electron spin dynamics as well as robust photostability of such polymer-tethered single radicals represent important attributes for cutting-edge applications in optoelectronic devices and quantum information technologies.
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