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具有周期性伸长的原子精确金量子棒中相干振动的演化

Evolution of coherent vibrations in atomically precise gold quantum rods with periodic elongation.

作者信息

Zhang Wei, Luo Lianshun, Liu Zhongyu, Zhao Fangming, Kong Jie, Jin Rongchao, Luo Yi, Zhou Meng

机构信息

Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Anhui 230026, P. R. China.

Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213, USA.

出版信息

Sci Adv. 2025 Jun 13;11(24):eadx2781. doi: 10.1126/sciadv.adx2781. Epub 2025 Jun 11.


DOI:10.1126/sciadv.adx2781
PMID:40498827
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12154193/
Abstract

The coherent vibrational dynamics of gold nanorods with varying aspect ratios have been extensively studied by time-resolved spectroscopy to reveal their mechanical properties, but quantum-sized rods (transverse diameter < 2 nanometers) remain unexplored. Here, we present a comprehensive study on the coherent vibrations of atomically precise gold quantum rods with distinct energy gaps (0.6 to 1.3 electron volts), all sharing the same radial dimension but with increasing aspect ratios. Time-resolved spectroscopy reveals ultrafast internal conversion and intersystem crossing, along with oscillatory features superimposed on transient signals that unveil coherent vibrational dynamics. Two dominant modes are identified: a longitudinal mode scaling with rod length and a transverse mode independent of aspect ratio. Theoretical simulations support these findings and clarify the structural origins of the observed vibrational behavior. Our study provides a framework for designing atomically precise gold quantum rods with tailored optical and vibrational properties, advancing the understanding and application of anisotropic quantum materials.

摘要

通过时间分辨光谱对不同纵横比的金纳米棒的相干振动动力学进行了广泛研究,以揭示其力学性质,但量子尺寸的棒(横向直径<2纳米)仍未被探索。在此,我们对具有不同能隙(0.6至1.3电子伏特)的原子精确金量子棒的相干振动进行了全面研究,这些量子棒都具有相同的径向尺寸,但纵横比不断增加。时间分辨光谱揭示了超快的内转换和系间窜越,以及叠加在瞬态信号上的振荡特征,这些特征揭示了相干振动动力学。确定了两种主导模式:一种与棒长度成比例的纵向模式和一种与纵横比无关的横向模式。理论模拟支持了这些发现,并阐明了观察到的振动行为的结构起源。我们的研究为设计具有定制光学和振动性质的原子精确金量子棒提供了一个框架,推动了对各向异性量子材料的理解和应用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5fb/12154193/7004ccc1fb2b/sciadv.adx2781-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5fb/12154193/0c4d80b0bc0a/sciadv.adx2781-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5fb/12154193/22580d364e96/sciadv.adx2781-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5fb/12154193/7004ccc1fb2b/sciadv.adx2781-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5fb/12154193/0c4d80b0bc0a/sciadv.adx2781-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5fb/12154193/22580d364e96/sciadv.adx2781-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b5fb/12154193/7004ccc1fb2b/sciadv.adx2781-f5.jpg

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Evolution of coherent vibrations in atomically precise gold quantum rods with periodic elongation.

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本文引用的文献

[1]
Thermally Activated Delayed Fluorescence-Based Near-Infrared-II Luminescence and Controlled Size Growth of Silver Nanoclusters.

ACS Nano. 2025-2-25

[2]
Lattice Modulation on Singlet-Triplet Splitting of Silver Cluster Boosting Near-Unity Photoluminescence Quantum Yield.

Angew Chem Int Ed Engl. 2025-3-10

[3]
Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy: Toward High Sensitivity and Broad Applicability.

ACS Nano. 2024-11-26

[4]
Crystal plane orientation-dependent surface atom diffusion in sub-10-nm Au nanocrystals.

Sci Adv. 2024-5-24

[5]
Structure Effects of Ligands in Gold-Ligand Complexes for Controlled Formation of Gold Nanoclusters.

ACS Nano. 2024-6-4

[6]
Chiroptical Activity Amplification of Chiral Metal Nanoclusters via Surface/Interface Solidification.

ACS Nano. 2024-5-28

[7]
Robust vibrational coherence protected by a core-shell structure in silver nanoclusters.

Chem Sci. 2024-4-1

[8]
Stepwise structural evolution toward robust carboranealkynyl-protected copper nanocluster catalysts for nitrate electroreduction.

Sci Adv. 2024-5-3

[9]
Site-Recognition-Induced Structural and Photoluminescent Evolution of the Gold-Pincer Nanocluster.

J Am Chem Soc. 2024-4-10

[10]
Bottom-Up Construction of Metal-Organic Framework Loricae on Metal Nanoclusters with Consecutive Single Nonmetal Atom Tuning for Tailored Catalysis.

J Am Chem Soc. 2024-4-3

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