Molecular Engineering of Emissive Molecular Qubits Based on Spin-Correlated Radical Pairs,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Molecular Engineering of Emissive Molecular Qubits Based on Spin-Correlated Radical Pairs
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2025-03-19 , DOI: 10.1021/jacs.4c16164
Neo Lin ₁ , Miu Tsuji ₁ , Isabella Bruzzese ₁ , Angela Chen ₁ , Michael Vrionides ₁ , Noen Jian ₁ , Farhan Kittur _{1,

2} , Thomas P Fay ₃ , Tomoyasu Mani _{1,

4}

Affiliation

Spin chemistry of photogenerated spin-correlated radical pairs (SCRPs) offers a practical approach to control chemical reactions and molecular emissions by using weak magnetic fields. This capability to harness magnetic field effects (MFEs) paves the way for developing SCRPs-based molecular qubits. Here, we introduce a new series of donor–chiral bridge–acceptor (D−χ–A) molecules that demonstrate significant MFEs on fluorescence intensity and lifetime in solution at room temperature─critical for quantum sensing. By precisely tuning the donor site through torsional locking, distance extension, and planarization, we achieved remarkable control over key quantum properties, including field-response range and line width. In the most responsive systems, emission lifetimes increased by over 200%, and the total emission intensity was modulated by up to 30%. This level of tunability shows the power of synthetic spin chemistry. The rational design principle of optically addressable SCRP-based molecular systems, presented in this work, represents a major leap toward functional synthetic molecular qubits, advancing the field of molecular quantum technologies.

中文翻译：

基于自旋相关自由基对的发射分子量子比特的分子工程

光生自旋相关自由基对（SCRP）的自旋化学提供了一种通过使用弱磁场来控制化学反应和分子发射的实用方法。这种利用磁场效应（MFE）的能力为开发基于 SCRP 的分子量子比特铺平了道路。在这里，我们介绍了一系列新的供体-手性桥-受体（D-χ-A）分子，这些分子在室温下对荧光强度和溶液中的寿命表现出显着的 MFE，这对量子传感至关重要。通过扭转锁定、距离延伸和平面化精确调整供体位点，我们实现了对关键量子特性的显着控制，包括场响应范围和线宽。在响应速度最快的系统中，排放寿命延长了 200% 以上，总排放强度调节了高达 30%。这种可调性水平显示了合成自旋化学的力量。这项工作中提出的基于光学寻址的 SCRP 分子系统的合理设计原则代表了向功能性合成分子量子比特的重大飞跃，推动了分子量子技术领域的发展。

更新日期：2025-03-19

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南