Plasmon-mediated photodecomposition of NH3 via intramolecular charge transfer  

作　　者：Yimin Zhang Weite Meng Daqiang Chen Lili Zhang Shunfang Li Sheng Meng 

机构地区：[1]Beijing National Laboratory for Condensed Matter Physics and Institute of Physics,Chinese Academy of Sciences,Beijing 100190,China [2]Key Laboratory of Material Physics,Ministry of Education,School of Physics and Microelectronics,Zhengzhou University,Zhengzhou 450001,China [3]School of Chemical Engineering,Anhui University of Science and Technology,Huainan 232000,China [4]School of Physical Sciences,University of Chinese Academy of Sciences,Beijing 100190,China

出　　处：《Nano Research》2022年第5期3894-3900,共7页纳米研究（英文版）

基　　金：We acknowledge financial support from MOST,the National Key Research and Development Project(No.2021YFA1400200);the National Natural Science Foundation of China(NSFC)(Nos.12025407,11774396,91850120,11934003,and 11674289);CAS(XDB330301).

摘　　要：As an excellent clean medium for hydrogen storage and fuel cell applications,the photolysis of ammonia via localized surface plasmon could be invoked as a promising route towards significantly reducing the temperature for conventional thermolysis.Here,we explore the underlying microscopic mechanism of ultrafast carrier dynamics in plasmon-mediated NH3 photodecomposition at the single-molecular level using real-time time-dependent density functional theory.The NH_(3)molecule adsorbed on the tip of archetypal magic metal clusters represented by tetrahedral Ag_(2)0 and icosahedral Ag147,splits within a hundred femtoseconds upon laser pulse illumination.We found that the splitting of the first N-H bond is dominated by the intramolecular charge transfer driven by localized surface plasmon.Surprisingly,the phase of laser pulse could modulate the dynamics of charge transfer and thus affect the plasmon-induced bond breaking.These findings offer a new avenue for NH3 decomposition and provide in-depth insights in designing highly efficient plasmon-mediated photocatalysts.

关 键 词：ammonia photodecomposition localized surface plasmon intramolecular charge transfer time-dependent density functional theory 

分 类 号：O64[理学—物理化学]