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State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies
Accounts of Chemical Research ( IF 16.4 ) Pub Date : 2018-05-08 00:00:00 , DOI: 10.1021/acs.accounts.8b00096 Tian Zhao 1 , Patrick J. Herbert 1 , Hongjun Zheng 1 , Kenneth L. Knappenberger 1
Accounts of Chemical Research ( IF 16.4 ) Pub Date : 2018-05-08 00:00:00 , DOI: 10.1021/acs.accounts.8b00096 Tian Zhao 1 , Patrick J. Herbert 1 , Hongjun Zheng 1 , Kenneth L. Knappenberger 1
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Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain.
中文翻译：
通过超快和磁光光谱学的组合透镜观察状态分辨的金属纳米粒子动力学
电子载流子动力学在纳米材料的功能特性中起着至关重要的作用。对于胶体金属，这些动力学的机理和影响取决于结构。纳米粒子（约2 nm及更大）的集体等离激元模式的相干载流子动力学决定了光学放大因子，这对于应用光谱技术至关重要。在纳米簇域（低于2 nm）中，载流子耦合至振动模式会影响光致发光产量。具有纳米颗粒和纳米团簇的光催化材料的性能还取决于非平衡电荷载体的弛豫动力学。开发涵盖这两个领域的载波动力学的全面描述所面临的挑战是多重的。等离子体相干性是短暂的，仅持续数十飞秒。纳米团簇表现出离散的载流子动力学，在某些情况下可以持续几微秒。在此时间尺度上，许多依赖状态的过程（包括振动弛豫，电荷转移和自旋转换）以不可缩放但特定于结构的方式影响载流子动力学。因此，需要状态解析光谱法来了解纳米簇域中的载流子动力学。
更新日期：2018-05-08
中文翻译：
通过超快和磁光光谱学的组合透镜观察状态分辨的金属纳米粒子动力学
电子载流子动力学在纳米材料的功能特性中起着至关重要的作用。对于胶体金属，这些动力学的机理和影响取决于结构。纳米粒子（约2 nm及更大）的集体等离激元模式的相干载流子动力学决定了光学放大因子，这对于应用光谱技术至关重要。在纳米簇域（低于2 nm）中，载流子耦合至振动模式会影响光致发光产量。具有纳米颗粒和纳米团簇的光催化材料的性能还取决于非平衡电荷载体的弛豫动力学。开发涵盖这两个领域的载波动力学的全面描述所面临的挑战是多重的。等离子体相干性是短暂的，仅持续数十飞秒。纳米团簇表现出离散的载流子动力学，在某些情况下可以持续几微秒。在此时间尺度上，许多依赖状态的过程（包括振动弛豫，电荷转移和自旋转换）以不可缩放但特定于结构的方式影响载流子动力学。因此，需要状态解析光谱法来了解纳米簇域中的载流子动力学。
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