当前位置：
X-MOL 学术
›
J. Phys. Chem. C
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Ultrafast Nonlinear Plasmon Decay Processes in Silver Nanoclusters
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-08-17 , DOI: 10.1021/acs.jpcc.0c03160 Gowri U. Kuda-Singappulige 1 , David B. Lingerfelt 2, 3 , Xiaosong Li 2 , Christine M. Aikens 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-08-17 , DOI: 10.1021/acs.jpcc.0c03160 Gowri U. Kuda-Singappulige 1 , David B. Lingerfelt 2, 3 , Xiaosong Li 2 , Christine M. Aikens 1
Affiliation
|
Tunable plasmonic properties of metallic nanostructures play a significant role in enhancing various photo-optical phenomena including solar energy conversion, nonlinear optics, photoluminescence and photocatalysis. Understanding the fast plasmon decay mechanisms is essential for developing practical applications utilizing these light-matter interaction processes, but has been a challenge both experimentally and computationally. Among theoretical simulation methods, real-time density functional theory (RT-TDDFT) is a valuable tool to monitor the electron dynamics of molecules subjected to an electric field. Herein, we use the RT-TDDFT method to identify the possible plasmon decay mechanisms of the bare tetrahedral Ag8 nanocluster. We excite the strong linear plasmonic states and examine dipole response and the electron dynamics in the system. Variation of density matrix elements related to occupied and virtual orbital pairs reveals that the one-photon allowed transitions, which have been excited due to the incident electric field, experience ultrafast decay into high energy transitions, specifically to two-photon allowed transitions. The tetrahedral symmetry representations of these transitions confirm that some of these high energy transitions are only allowed via two-photon absorption whereas others can be activated via both one- and two- photon absorption. Moreover, this work suggests that the collective excitations present in the system play an important role in accumulating an enormous amount of energy to enhance nonlinear processes. Overall, this work provides insights into a possible plasmon decay mechanism of nanoclusters which is activation of nonlinear processes such as two-photon absorption.
中文翻译：
银纳米团簇中的超快非线性等离子体等离子体衰变过程
金属纳米结构的可调节等离子体特性在增强各种光-光学现象中起着重要作用，这些现象包括太阳能转换，非线性光学，光致发光和光催化。了解快速的等离子体激元衰减机制对于利用这些光-质相互作用过程开发实际应用至关重要，但是在实验和计算上都是一个挑战。在理论模拟方法中，实时密度泛函理论（RT-TDDFT）是监测电场中分子的电子动力学的有价值的工具。在这里，我们使用RT-TDDFT方法来识别裸四面体Ag 8的可能的等离激元衰变机理纳米簇。我们激发强线性等离子体状态，并检查系统中的偶极响应和电子动力学。与占据轨道和虚拟轨道对有关的密度矩阵元素的变化表明，由于入射电场而激发的单光子允许跃迁经历了超快衰减到高能量跃迁，特别是到两个光子允许跃迁。这些跃迁的四面体对称表示证实，这些高能跃迁中的某些仅通过双光子吸收才被允许，而另一些可以通过单光子和双光子吸收而被激活。此外，这项工作表明，系统中存在的集体激励在积累大量能量以增强非线性过程中起着重要作用。总体，
更新日期：2020-09-18
中文翻译：
银纳米团簇中的超快非线性等离子体等离子体衰变过程
金属纳米结构的可调节等离子体特性在增强各种光-光学现象中起着重要作用，这些现象包括太阳能转换，非线性光学，光致发光和光催化。了解快速的等离子体激元衰减机制对于利用这些光-质相互作用过程开发实际应用至关重要，但是在实验和计算上都是一个挑战。在理论模拟方法中，实时密度泛函理论（RT-TDDFT）是监测电场中分子的电子动力学的有价值的工具。在这里，我们使用RT-TDDFT方法来识别裸四面体Ag 8的可能的等离激元衰变机理纳米簇。我们激发强线性等离子体状态，并检查系统中的偶极响应和电子动力学。与占据轨道和虚拟轨道对有关的密度矩阵元素的变化表明，由于入射电场而激发的单光子允许跃迁经历了超快衰减到高能量跃迁，特别是到两个光子允许跃迁。这些跃迁的四面体对称表示证实，这些高能跃迁中的某些仅通过双光子吸收才被允许，而另一些可以通过单光子和双光子吸收而被激活。此外，这项工作表明，系统中存在的集体激励在积累大量能量以增强非线性过程中起着重要作用。总体，
京公网安备 11010802027423号