TY - JOUR VL - 14 JF - NPG Asia Materials PB - Springer Science and Business Media LLC UR - https://doi.org/10.1038/s41427-022-00392-6 Y1 - 2022/05/20/ ID - discovery10149351 N1 - This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article?s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article?s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. TI - Triplet-radical spin entanglement: potential of molecular materials for high-temperature quantum information processing AV - public KW - Magnetic properties and materials KW - Organic chemistry KW - Quantum optics KW - Theory and computation KW - Ultrafast photonics N2 - Recently, spin-bearing molecules have been experimentally demonstrated to have great potential as building blocks for quantum information processing due to their substantial advantages including tunability, portability, and scalability. Here, we propose a theoretical model based on the theory of open quantum systems for spin dynamics in a molecule containing one radical, which can interact with the triplet state arising from another part of the molecule owing to optical excitation and intersystem crossing. With the initial state being a classical mixture of a radical 1/2-spin, the exchange interaction between the radical and the triplet produces a spin coherent state, which could potentially be used for a qubit-qutrit quantum entangling gate. Our calculations for the time-resolved electron paramagnetic resonance spectra showed good qualitative agreement with the related experimental results for radical-bearing molecules at high temperature (~77?K, the boiling point of liquid nitrogen). This work therefore lays a solid theoretical cornerstone for optically driven quantum gate operations in radical-bearing molecular materials, aiming toward high-temperature quantum information processing. SN - 1884-4049 A1 - Ma, Lin A1 - Chang, Jiawei A1 - Chen, Qiuyuan A1 - Zou, Taoyu A1 - Wu, Wei A1 - Wang, Hai ER -