Molecular Engineering of Emissive Molecular Qubits Based on Spin-Correlated Radical Pairs

IF 14.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-03-19 DOI:10.1021/jacs.4c16164

Neo Lin, Miu Tsuji, Isabella Bruzzese, Angela Chen, Michael Vrionides, Noen Jian, Farhan Kittur, Thomas P. Fay, Tomoyasu Mani

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Abstract

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.

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光生自旋相关自由基对（SCRPs）的自旋化学提供了一种利用弱磁场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）的能力为开发基于自旋相关自由基对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，它们在室温下的溶液中对荧光强度和寿命具有显著的磁场效应--这对于量子传感至关重要。通过扭转锁定、距离扩展和平面化来精确调节供体位点，我们实现了对关键量子特性的显著控制，包括场响应范围和线宽。在反应最灵敏的系统中，发射寿命增加了 200% 以上，总发射强度最多可调 30%。这种可调节性显示了合成自旋化学的威力。这项工作中提出的基于 SCRP 的可光学寻址分子系统的合理设计原理，是向功能合成分子量子比特迈出的一大步，推动了分子量子技术领域的发展。

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.