Ultrafast all-optical coherence of molecular electron spins in room-temperature water solution

• 成果类型: Article
• 署名作者: Sutcliffe, Erica; Kazmierczak, Nathanael P.; Hadt, Ryan G.
• 署名单位: California Institute of Technology
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11999
• DOI: 10.1126/science.ads0512
• 发表日期: 2024-11-22
• 页码: 888-892
• 关键词: magnetic circular-dichroism; quantum; manipulation; transitions; DYNAMICS; epr

摘要

The tunability and spatial precision of paramagnetic molecules makes them attractive for quantum sensing. However, usual microwave-based detection methods have poor temporal and spatial resolution, and optical methods compatible with room-temperature solutions have remained elusive. In this study, we utilized pump-probe polarization spectroscopy to initialize and track electron spin coherence in a molecule. Designed to efficiently couple spins to light, aqueous potassium hexachloroiridate(IV) enabled detection of few-picosecond free-induction decay at room temperature and micromolar concentrations. Viscosity was found to strongly vary decoherence lifetimes. This approach has improved the experimental time resolution by up to five orders of magnitude, making it possible to observe molecular electron spin coherence in a system that only exhibits coherence below 25 kelvin with traditional techniques.