Direct observation of chirality-induced spin selectivity in electron donor-acceptor molecules

• 成果类型: Article
• 署名作者: Eckvahl, Hannah J.; Tcyrulnikov, Nikolai A.; Chiesa, Alessandro; Bradley, Jillian M.; Young, Ryan M.; Carretta, Stefano; Krzyaniak, Matthew D.; Wasielewski, Michael R.
• 署名单位: Northwestern University; Northwestern University; University of Parma
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-13502
• DOI: 10.1126/science.adj5328
• 发表日期: 2023-10-13
• 页码: 197-201
• 关键词: photosynthetic reaction centers; ion-pair formation; radical pair; photosystem-i; envelope modulation; transient epr; qubit pairs; DYNAMICS; echo; distance

摘要

The role of chirality in determining the spin dynamics of photoinduced electron transfer in donor-acceptor molecules remains an open question. Although chirality-induced spin selectivity (CISS) has been demonstrated in molecules bound to substrates, experimental information about whether this process influences spin dynamics in the molecules themselves is lacking. Here we used time-resolved electron paramagnetic resonance spectroscopy to show that CISS strongly influences the spin dynamics of isolated covalent donor-chiral bridge-acceptor (D-B chi-A) molecules in which selective photoexcitation of D is followed by two rapid, sequential electron-transfer events to yield D center dot+-B chi-A(center dot-). Exploiting this phenomenon affords the possibility of using chiral molecular building blocks to control electron spin states in quantum information applications.