文献检索文档翻译深度研究
Suppr Zotero 插件Zotero 插件
邀请有礼套餐&价格历史记录

新学期,新优惠

限时优惠:9月1日-9月22日

30天高级会员仅需29元

1天体验卡首发特惠仅需5.99元

了解详情
不再提醒
插件&应用
Suppr Zotero 插件Zotero 插件浏览器插件Mac 客户端Windows 客户端微信小程序
高级版
套餐订阅购买积分包
AI 工具
文献检索文档翻译深度研究
关于我们
关于 Suppr公司介绍联系我们用户协议隐私条款
关注我们

Suppr 超能文献

核心技术专利:CN118964589B侵权必究
粤ICP备2023148730 号-1Suppr @ 2025

[AuAg(SH)](n = 1、12、25)硫醇盐保护的纳米团簇中的非辐射弛豫动力学

Nonradiative relaxation dynamics in the [AuAg(SH)] (n = 1, 12, 25) thiolate-protected nanoclusters.

作者信息

Pandeya Pratima, Senanayake Ravithree D, Aikens Christine M

机构信息

Department of Chemistry, Kansas State University, Manhattan, Kansas 66506, USA.

出版信息

J Chem Phys. 2021 May 14;154(18):184303. doi: 10.1063/5.0045590.


DOI:10.1063/5.0045590
PMID:34241036
Abstract

Evaluation of the electron-nuclear dynamics and relaxation mechanisms of gold and silver nanoclusters and their alloys is important for future photocatalytic, light harvesting, and photoluminescence applications of these systems. In this work, the effect of silver doping on the nonradiative excited state relaxation dynamics of the atomically precise thiolate-protected gold nanocluster [AuAg(SH)] (n = 1, 12, 25) is studied theoretically. Time-dependent density functional theory is used to study excited states lying in the energy range 0.0-2.5 eV. The fewest switches surface hopping method with decoherence correction was used to investigate the dynamics of these states. The HOMO-LUMO gap increases significantly upon doping of 12 silver atoms but decreases for the pure silver nanocluster. Doped clusters show a different response for ground state population increase lifetimes and excited state population decay times in comparison to the undoped system. The ground state recovery times of the S-S states in the first excited peak were found to be longer for [AuAg(SH)] than the corresponding recovery times of other studied nanoclusters, suggesting that this partially doped nanocluster is best for preserving electrons in an excited state. The decay time constants were in the range of 2.0-20 ps for the six lowest energy excited states. Among the higher excited states, S has the slowest decay time constant although it occurs more quickly than S decay. Overall, these clusters follow common decay time constant trends and relaxation mechanisms due to the similarities in their electronic structures.

摘要

评估金和银纳米团簇及其合金的电子-核动力学和弛豫机制对于这些体系未来的光催化、光捕获和光致发光应用至关重要。在这项工作中,从理论上研究了银掺杂对原子精确的硫醇盐保护的金纳米团簇[AuAg(SH)](n = 1, 12, 25)的非辐射激发态弛豫动力学的影响。采用含时密度泛函理论研究能量范围在0.0 - 2.5 eV的激发态。使用具有退相干校正的最少开关表面跳跃方法来研究这些态的动力学。掺杂12个银原子后,最高占据分子轨道-最低未占据分子轨道能隙显著增加,但对于纯银纳米团簇则减小。与未掺杂体系相比,掺杂团簇在基态布居增加寿命和激发态布居衰减时间方面表现出不同的响应。发现[AuAg(SH)]在第一激发峰中S - S态的基态恢复时间比其他研究的纳米团簇的相应恢复时间更长,这表明这种部分掺杂的纳米团簇最有利于将电子保持在激发态。六个最低能量激发态的衰减时间常数在2.0 - 20 ps范围内。在较高激发态中,S的衰减时间常数最慢,尽管它比S衰减发生得更快。总体而言,由于这些团簇电子结构的相似性,它们遵循共同的衰减时间常数趋势和弛豫机制。

相似文献

[1]
Nonradiative relaxation dynamics in the [AuAg(SH)] (n = 1, 12, 25) thiolate-protected nanoclusters.

J Chem Phys. 2021-5-14

[2]
Electronic relaxation dynamics in [Au(SR)] (R = CH, CH, CH, MPA, PET) thiolate-protected nanoclusters.

Phys Chem Chem Phys. 2020-3-7

[3]
Theoretical investigation of relaxation dynamics in the Au(SH) thiolate-protected gold nanocluster.

J Chem Phys. 2019-9-7

[4]
Electronic and Geometric Structure, Optical Properties, and Excited State Behavior in Atomically Precise Thiolate-Stabilized Noble Metal Nanoclusters.

Acc Chem Res. 2018-12-18

[5]
Luminescence and Electron Dynamics in Atomically Precise Nanoclusters with Eight Superatomic Electrons.

J Am Chem Soc. 2019-11-27

[6]
Effect of single electrons on the excited state dynamics of rod-shaped Au nanoclusters.

Nanoscale. 2021-12-2

[7]
Isomerism effects in relaxation dynamics of Au(SR)thiolate-protected gold nanoclusters.

Nanotechnology. 2022-12-19

[8]
Electrochemistry of Atomically Precise Metal Nanoclusters.

Acc Chem Res. 2019-1-15

[9]
Relaxation dynamics of Au25L18 nanoclusters studied by femtosecond time-resolved near infrared transient absorption spectroscopy.

Nanoscale. 2012-6-18

[10]
Theoretical Insights into the Origin of Photoluminescence of Au25(SR)18(-) Nanoparticles.

J Am Chem Soc. 2016-8-26

文献AI研究员

20分钟写一篇综述,助力文献阅读效率提升50倍

立即体验

用中文搜PubMed

大模型驱动的PubMed中文搜索引擎

马上搜索

推荐工具

医学文档翻译智能文献检索