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钴铁普鲁士蓝类化合物中超快自旋跃迁驱动的电荷转移
作者:小柯机器人 发布时间:2020/12/10 15:12:48

法国雷恩大学Eric Collet课题组在钴铁普鲁士蓝类化合物中发现了超快自旋跃迁驱动的电荷转移。这一研究成果于2020年12月7日发表在国际顶尖学术期刊《自然·化学》上。

在这篇文章中,研究人员通过飞秒X射线和光学吸收波谱研究了氰基桥联的钴铁模型系统中的光诱导电荷转移过程,并探明了其中的超快电子和结构动力学。研究结果表明,在最初的约50fs中是钴位点上首先发生自旋跃迁,然后才驱动接下来约200fs中发生的由铁至钴的电荷转移。这项研究代表着理解和控制光致电荷转移相关功能的重要一步。

据了解,光诱导的电荷转移是自然界和技术领域中的一个重要过程,也负责实现许多新奇功能,如氰基桥联的双金属配位网络中的磁有序性。虽然其在化学和材料科学领域有着广泛的意义和许多进展,但几十年来人们对初始光诱导步骤——即金属间电荷转移和自旋跃迁的偶合过程——在原子层面上的描述仍存在争论,这是因为该过程非常快以至于超出了一般方法的检测极限。

附:英文原文

Title: Charge transfer driven by ultrafast spin transition in a CoFe Prussian blue analogue

Author: Marco Cammarata, Serhane Zerdane, Lodovico Balducci, Giovanni Azzolina, Sandra Mazerat, Cecile Exertier, Matilde Trabuco, Matteo Levantino, Roberto Alonso-Mori, James M. Glownia, Sanghoon Song, Laure Catala, Talal Mallah, Samir F. Matar, Eric Collet

Issue&Volume: 2020-12-07

Abstract: Photoinduced charge-transfer is an important process in nature and technology and is responsible for the emergence of exotic functionalities, such as magnetic order for cyanide-bridged bimetallic coordination networks. Despite its broad interest and intensive developments in chemistry and material sciences, the atomic-scale description of the initial photoinduced process, which couples intermetallic charge-transfer and spin transition, has been debated for decades; it has been beyond reach due to its extreme speed. Here we study this process in a prototype cyanide-bridged CoFe system by femtosecond X-ray and optical absorption spectroscopies, enabling the disentanglement of ultrafast electronic and structural dynamics. Our results demonstrate that it is the spin transition that occurs first on the Co site within ~50fs, and it is this that drives the subsequent Fe-to-Co charge-transfer within ~200fs. This study represents a step towards understanding and controlling charge-transfer-based functions using light.

DOI: 10.1038/s41557-020-00597-8

Source: https://www.nature.com/articles/s41557-020-00597-8

 

期刊信息

Nature Chemistry:《自然—化学》,创刊于2009年。隶属于施普林格·自然出版集团,最新IF:21.687
官方网址:https://www.nature.com/nchem/
投稿链接:https://mts-nchem.nature.com/cgi-bin/main.plex