Cryogenic Correlative Single-Particle Photoluminescence Spectroscopy and Electron Tomography for Investigation of Nanomaterials
Abstract
Cryogenic single-particle photoluminescence (PL) spectroscopy has been used with great success to directly observe the heterogeneous photophysical states present in a population of luminescent particles. Cryogenic electron tomography provides complementary nanometer scale structural information to PL spectroscopy, but the two techniques have not been correlated due to technical challenges. Here, we present a method for correlating single-particle information from these two powerful microscopy modalities. We simultaneously observe PL brightness, emission spectrum, and in-plane excitation dipole orientation of CdSSe/ZnS quantum dots suspended in vitreous ice. Stable and fluctuating emitters were observed, as well as a surprising splitting of the PL spectrum into two bands with an average energy separation of 80 meV. In some cases, the onset of the splitting corresponded to changes in the in-plane excitation dipole orientation. These dynamics were assigned to structures of individual quantum dots and the excitation dipoles were visualized in the context of structural features.
- Authors:
-
[1]
- Stanford Univ., CA (United States). Dept. of Chemistry
- Stanford Univ., CA (United States). Dept. of Bioengineering
- Stanford Univ., CA (United States). Dept. of Bioengineering; SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1632147
- Alternate Identifier(s):
- OSTI ID: 1617981
- Grant/Contract Number:
- AC02-76SF00515; FG02-07ER15892; P41GM103832
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 36; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; correlative light electron microscopy (CLEM); cryogenic electron tomography; fluorescence spectroscopy; nanoparticles; single-molecule studies
Citation Formats
Dahlberg, Peter D., Perez, Davis, Su, Zhaoming, Chiu, Wah, and Moerner, W. E. Cryogenic Correlative Single-Particle Photoluminescence Spectroscopy and Electron Tomography for Investigation of Nanomaterials. United States: N. p., 2020.
Web. doi:10.1002/anie.202002856.
Dahlberg, Peter D., Perez, Davis, Su, Zhaoming, Chiu, Wah, & Moerner, W. E. Cryogenic Correlative Single-Particle Photoluminescence Spectroscopy and Electron Tomography for Investigation of Nanomaterials. United States. https://doi.org/10.1002/anie.202002856
Dahlberg, Peter D., Perez, Davis, Su, Zhaoming, Chiu, Wah, and Moerner, W. E. Mon .
"Cryogenic Correlative Single-Particle Photoluminescence Spectroscopy and Electron Tomography for Investigation of Nanomaterials". United States. https://doi.org/10.1002/anie.202002856. https://www.osti.gov/servlets/purl/1632147.
@article{osti_1632147,
title = {Cryogenic Correlative Single-Particle Photoluminescence Spectroscopy and Electron Tomography for Investigation of Nanomaterials},
author = {Dahlberg, Peter D. and Perez, Davis and Su, Zhaoming and Chiu, Wah and Moerner, W. E.},
abstractNote = {Cryogenic single-particle photoluminescence (PL) spectroscopy has been used with great success to directly observe the heterogeneous photophysical states present in a population of luminescent particles. Cryogenic electron tomography provides complementary nanometer scale structural information to PL spectroscopy, but the two techniques have not been correlated due to technical challenges. Here, we present a method for correlating single-particle information from these two powerful microscopy modalities. We simultaneously observe PL brightness, emission spectrum, and in-plane excitation dipole orientation of CdSSe/ZnS quantum dots suspended in vitreous ice. Stable and fluctuating emitters were observed, as well as a surprising splitting of the PL spectrum into two bands with an average energy separation of 80 meV. In some cases, the onset of the splitting corresponded to changes in the in-plane excitation dipole orientation. These dynamics were assigned to structures of individual quantum dots and the excitation dipoles were visualized in the context of structural features.},
doi = {10.1002/anie.202002856},
journal = {Angewandte Chemie (International Edition)},
number = 36,
volume = 59,
place = {United States},
year = {Mon May 11 00:00:00 EDT 2020},
month = {Mon May 11 00:00:00 EDT 2020}
}
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