School of Chemistry and University of Sydney Nano Institute, University of Sydney Sydney, NSW 2006, Australia.
SUPA, School of Physics and Astronomy, University of St Andrews, St Andrews KY16 9SS, U.K.
J Phys Chem Lett. 2021 Jul 8;12(26):6143-6151. doi: 10.1021/acs.jpclett.1c01303. Epub 2021 Jun 28.
Coherence-enhanced light harvesting has not been directly observed experimentally, despite theoretical evidence that coherence can significantly enhance light-harvesting performance. The main experimental obstacle has been the difficulty in isolating the effect of coherence in the presence of confounding variables. Recent proposals for externally controlling coherence by manipulating the light's degree of polarization showed that coherent efficiency enhancements would be possible, but they were restricted to light-harvesting systems weakly coupled to their environment. Here, we show that increases in system-bath coupling strength can amplify coherent efficiency enhancements, rather than suppress them. This result dramatically broadens the range of systems that could be used to conclusively demonstrate coherence-enhanced light harvesting or to engineer coherent effects into artificial light-harvesting devices.
相干增强光捕获虽然有理论依据表明相干性可以显著提高光捕获性能，但在实验中尚未直接观察到。主要的实验障碍是在存在混杂变量的情况下难以分离相干性的影响。最近提出的通过操纵光的偏振度来外部控制相干性的建议表明，相干效率增强是可能的，但它们仅限于与环境弱耦合的光捕获系统。在这里，我们表明增加系统-浴耦合强度可以放大相干效率增强，而不是抑制它们。这一结果极大地拓宽了可以用来明确证明相干增强光捕获或在人工光捕获器件中设计相干效应的系统范围。
