Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays

Claire Deeb; Zhi Guo; Ankun Yang; Libai Huang; Teri W. Odom

doi:10.1021/acs.nanolett.7b05223

Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays

Claire Deeb, Zhi Guo, Ankun Yang, Libai Huang, Teri W. Odom^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

30 Scopus citations

Abstract

Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.

Original language	English (US)
Pages (from-to)	1454-1459
Number of pages	6
Journal	Nano letters
Volume	18
Issue number	2
DOIs	https://doi.org/10.1021/acs.nanolett.7b05223
State	Published - Feb 14 2018

Funding

This work was supported by the National Science Foundation (NSF) under DMR-1608258 (T.W.O.) and DMR-1306514 (C.D. and T.W.O). This work made use of the NUANCE Center facilities, which are supported by NSF-MRSEC, NSF-NSC, and the Keck Foundation. L.H. and Z.G. acknowledge the support from the U.S. Department of Energy Office of Basic Energy Sciences through award no. DE-SC0016356. We thank Yi Hua and Alexander J. Hryn for helping with FDTD simulations and providing photoresist post samples.

Keywords

Localized surface plasmons
lattice plasmons
metal nanoparticle arrays
plasmon lasing
transient absorption microscopy

ASJC Scopus subject areas

Condensed Matter Physics
Mechanical Engineering
Bioengineering
General Chemistry
General Materials Science

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10.1021/acs.nanolett.7b05223

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title = "Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays",

abstract = "Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.",

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AU - Guo, Zhi

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AU - Huang, Libai

AU - Odom, Teri W.

PY - 2018/2/14

Y1 - 2018/2/14

N2 - Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.

AB - Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.

KW - Localized surface plasmons

KW - lattice plasmons

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KW - plasmon lasing

KW - transient absorption microscopy

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Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays

Abstract

Funding

Keywords

ASJC Scopus subject areas

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