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六方钯纳米片和 Ag/Pd/Ag 三明治纳米盘中的电子和声子动力学。

Electron and Phonon Dynamics in Hexagonal Pd Nanosheets and Ag/Pd/Ag Sandwich Nanoplates.

机构信息

Department of Chemistry, School of Science and Technology, Kwansei Gakuin University , Sanda 669-1337, Japan.

出版信息

ACS Nano. 2017 Feb 28;11(2):1180-1188. doi: 10.1021/acsnano.6b07082. Epub 2017 Jan 9.

Abstract

Pd and its hybrid nanostructures have attracted considerable attention over the past decade, with both catalytic and plasmonic properties. The electron and phonon properties directly govern conversion efficiencies in applications such as energy collectors and photocatalysts. We report the dynamic processes of electron-phonon coupling and coherent acoustic phonon vibration in hexagonal Pd nanosheets and Ag/Pd/Ag sandwich nanoplates using transient absorption spectroscopy. The electron-phonon coupling constant of Pd nanosheets, G (8.7 × 10 W/(m·K)) is larger than that of the bulk G (5.0 × 10 W/(m·K)). The effective coupling constant G of Ag/Pd/Ag nanoplates decreases with increasing Ag shell thickness, finally approaching the bulk G. The variation of G is explained in terms of reduced density of states near Fermi level of Pd nanosheets with 1.8 nm ultrathin thickness. Coherent acoustic phonon vibration in Pd nanosheets is assigned to a fundamental breathing mode, similar to the vibration of benzene. The period increases with increasing Ag shell thickness. For Ag/Pd/Ag nanoplates with 20 nm thick Ag shells, the vibrational mode is ascribed to a quasi-extensional mode. The results show that the modes of the coherent acoustic phonon vibration transform with the geometric variation of Pd nanosheets and Ag/Pd/Ag nanoplates. Our results represent an understanding of quantum-confinement related electron dynamics and bulk-like phonon kinetics in the ultrathin Pd nanosheets and their hybrid nanostructures.

摘要

在过去的十年中,钯及其杂化纳米结构因其具有催化和等离子体特性而引起了相当大的关注。电子和声子性质直接决定了在能源收集器和光催化剂等应用中的能量转换效率。我们使用瞬态吸收光谱报告了六方钯纳米片和 Ag/Pd/Ag 三明治纳米板中电子-声子耦合和相干声子振动的动态过程。钯纳米片的电子-声子耦合常数 G(8.7×10 W/(m·K))大于体相 G(5.0×10 W/(m·K))。Ag/Pd/Ag 纳米板的有效耦合常数 G 随着 Ag 壳层厚度的增加而减小,最终接近体相 G。G 的变化可以用 1.8nm 超薄厚度的钯纳米片费米能级附近的态密度降低来解释。钯纳米片中的相干声子振动归因于基本的呼吸模式,类似于苯的振动。周期随 Ag 壳层厚度的增加而增加。对于具有 20nm 厚 Ag 壳层的 Ag/Pd/Ag 纳米板,振动模式归因于准伸张模式。结果表明,随着钯纳米片和 Ag/Pd/Ag 纳米板的几何变化,相干声子振动的模式发生了转变。我们的研究结果代表了对超薄钯纳米片及其杂化纳米结构中量子限制相关电子动力学和类似体相的声子动力学的理解。

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