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Recent advances in the determination of crystal structures and studies of optical properties of gold nanoclusters in the size range from tens to hundreds of gold atoms have started to reveal the grand evolution from gold complexes to nanoclusters and further to plasmonic nanoparticles. However, a detailed comparison of their photophysical properties is still lacking. Here, we compared the excited state behaviors of gold complexes, nanolcusters, and plasmonic nanoparticles, as well as small organic molecules by choosing four typical examples including the Au10 complex, Au25 nanocluster (1 nm metal core), 13 diameter Au nanoparticles, and Rhodamine B. To compare their photophysical behaviors, we performed steady-state absorption, photoluminescence, and femtosecond transient absorption spectroscopic measurements. It was found that gold nanoclusters behave somewhat like small molecules, showing both rapid internal conversion (<1 ps) and long-lived excited state lifetime (about 100 ns). Unlike the nanocluster form in which metal–metal transitions dominate, gold complexes showed significant charge transfer between metal atoms and surface ligands. Plasmonic gold nanoparticles, on the other hand, had electrons being heated and cooled (~100 ps time scale) after photo-excitation, and the relaxation was dominated by electron–electron scattering, electron–phonon coupling, and energy dissipation. In both nanoclusters and plasmonic nanoparticles, one can observe coherent oscillations of the metal core, but with different fundamental origins. Overall, this work provides some benchmarking features for organic dye molecules, organometallic complexes, metal nanoclusters, and plasmonic nanoparticles.
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Plasmon-assisted random lasing from a single-mode fiber tip
Random lasing occurs as the result of a coherent optical feedback from multiple scattering centers. Here, we demonstrate that plasmonic gold nanostars are efficient light scattering centers, exhibiting strong field enhancement at their nanotips, which assists a very narrow bandwidth and highly amplified coherent random lasing with a low lasing threshold. First, by embedding plasmonic gold nanostars in a rhodamine 6G dye gain medium, we observe a series of very narrow random lasing peaks with full-width at half-maximum ∼ 0.8 nm. In contrast, free rhodamine 6G dye molecules exhibit only a single amplified spontaneous emission peak with a broader linewidth of 6 nm. The lasing threshold for the dye with gold nanostars is two times lower than that for a free dye. Furthermore, by coating the tip of a single-mode optical fiber with gold nanostars, we demonstrate a collection of random lasing signal through the fiber that can be easily guided and analyzed. Time-resolved measurements show a significant increase in the emission rate above the lasing threshold, indicating a stimulated emission process. Our study provides a method for generating random lasing in the nanoscale with low threshold values that can be easily collected and guided, which promise a range of potential applications in remote sensing, information processing, and on-chip coherent light sources.
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- Award ID(s):
- 1709612
- PAR ID:
- 10151851
- Publisher / Repository:
- Optical Society of America
- Date Published:
- Journal Name:
- Optics Express
- Volume:
- 28
- Issue:
- 11
- ISSN:
- 1094-4087; OPEXFF
- Format(s):
- Medium: X Size: Article No. 16417
- Size(s):
- Article No. 16417
- Sponsoring Org:
- National Science Foundation
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