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科研人员实现振动能的传输和集中从而促进异构化反应
作者:小柯机器人 发布时间:2021/1/15 16:40:43

马克斯普朗克研究所的生物物理化学Alec M. Wodtke研究组近日取得一项新成果。经过不懈努力,他们的最新研究实现了振动能的运输和集中,并以此促进了异构化反应。 该研究于2021年1月11日发表于国际一流学术期刊《自然》。

据悉,可见光的吸收和由此产生的电子激发通过荧光共振能量转移(FRET)传输到反应中心对于生物光合系统的运行至关重要,并且用于多种由合成染料、聚合物或纳米点组成的人工系统。

用于描述FRET的基本方程和描述振动态-振动态(V-V)能量转移的方程相似,意味着振动能量的传输和局域化在理论上应该是可能的。尽管振动激发能够促进反应进行是已知的,传输和集中振动能量还未被报道过。

课题组研究人员最近展示了通过在NaCl(100)表面上的CO吸附物层中的振动能量池实现的定向异构化。基于这项工作,该团队展示了当有一个厚的12C16O覆盖层时,更多中红外光子被吸收并通过V-V能量转移到13C18O-NaCl界面,使得反应更有效地进行。界面上可达到的共振能量密度比通过直接激发界面间的CO要高30倍。

研究人员预期,通过细致的系统设计,这些概念能够用于驱动其他化学转化,为凝聚态化学提供新的方法。

附:英文原文

Title: Transporting and concentrating vibrational energy to promote isomerization

Author: Jascha A. Lau, Li Chen, Arnab Choudhury, Dirk Schwarzer, Varun B. Verma, Alec M. Wodtke

Issue&Volume: 2021-01-11

Abstract: Visible-light absorption and transport of the resultant electronic excitations to a reaction centre through Forster resonance energy transfer1,2,3 (FRET) are critical to the operation of biological light-harvesting systems4, and are used in various artificial systems made of synthetic dyes5, polymers6 or nanodots7,8. The fundamental equations describing FRET are similar to those describing vibration-to-vibration (V–V) energy transfer9, and suggest that transport and localization of vibrational energy should, in principle, also be possible. Although it is known that vibrational excitation can promote reactions10,11,12,13,14,15,16, transporting and concentrating vibrational energy has not yet been reported. We have recently demonstrated orientational isomerization enabled by vibrational energy pooling in a CO adsorbate layer on a NaCl(100) surface17. Here we build on that work to show that the isomerization reaction proceeds more efficiently with a thick 12C16O overlayer that absorbs more mid-infrared photons and transports the resultant vibrational excitations by V–V energy transfer to a 13C18O–NaCl interface. The vibrational energy density achieved at the interface is 30 times higher than that obtained with direct excitation of the interfacial CO. We anticipate that with careful system design, these concepts could be used to drive other chemical transformations, providing new approaches to condensed phase chemistry.

DOI: 10.1038/s41586-020-03081-y

Source: https://www.nature.com/articles/s41586-020-03081-y

期刊信息

Nature:《自然》,创刊于1869年。隶属于施普林格·自然出版集团,最新IF:42.778
官方网址:http://www.nature.com/