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Title: Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy

Abstract

Understanding and rationally controlling the properties of nanomaterial surfaces is a rapidly expanding field of research due to the dramatic role they play on the optical and electronic properties vital to light harvesting, emitting and detection technologies. This information is essential to the continued development of synthetic approaches designed to tailor interfaces for optimal nanomaterial based device performance. In this work, closely spaced electronic excited states in model CdSe quantum dots (QDs) are resolved using second harmonic generation (SHG) spectroscopy, and the corresponding contributions from surface species to these states are assessed. Two distinct spectral features are observed in the SHG spectra, which are not readily identified in linear absorption and photoluminescence excitation spectra. These features include a weak band at 395 6 nm, which coincides with transitions to the 2S1/2 1Se state, and a much more pronounced band at 423 4 nm arising from electronic transitions to the 1P3/2 1Pe state. Chemical modification of the QD surfaces through oxidation resulted in disappearance of the SHG band corresponding to the 1P3/2 1Pe state, indicating prominent surface contributions. Signatures of deep trap states localized on the surfaces of the QDs are also observed. We further find that the SHG signal intensitiesmore » depend strongly on the electronic states being probed and their relative surface contributions, thereby offering additional insight into the surface specificity of SHG signals from QDs.« less

Authors:
 [1];  [1];  [1]
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  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1185673
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal Issue: 5; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nonlinear spectroscopy; surface; nanoparticle; electronic structure; trap state; semiconductor

Citation Formats

Doughty, Benjamin L., Ma, Yingzhong, and Shaw, Robert W. Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy. United States: N. p., 2015. Web. doi:10.1021/jp510357p.
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Doughty, Benjamin L., Ma, Yingzhong, & Shaw, Robert W. Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy. United States. https://doi.org/10.1021/jp510357p
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Doughty, Benjamin L., Ma, Yingzhong, and Shaw, Robert W. Wed . "Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy". United States. https://doi.org/10.1021/jp510357p. https://www.osti.gov/servlets/purl/1185673.
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@article{osti_1185673,
title = {Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy},
author = {Doughty, Benjamin L. and Ma, Yingzhong and Shaw, Robert W},
abstractNote = {Understanding and rationally controlling the properties of nanomaterial surfaces is a rapidly expanding field of research due to the dramatic role they play on the optical and electronic properties vital to light harvesting, emitting and detection technologies. This information is essential to the continued development of synthetic approaches designed to tailor interfaces for optimal nanomaterial based device performance. In this work, closely spaced electronic excited states in model CdSe quantum dots (QDs) are resolved using second harmonic generation (SHG) spectroscopy, and the corresponding contributions from surface species to these states are assessed. Two distinct spectral features are observed in the SHG spectra, which are not readily identified in linear absorption and photoluminescence excitation spectra. These features include a weak band at 395 6 nm, which coincides with transitions to the 2S1/2 1Se state, and a much more pronounced band at 423 4 nm arising from electronic transitions to the 1P3/2 1Pe state. Chemical modification of the QD surfaces through oxidation resulted in disappearance of the SHG band corresponding to the 1P3/2 1Pe state, indicating prominent surface contributions. Signatures of deep trap states localized on the surfaces of the QDs are also observed. We further find that the SHG signal intensities depend strongly on the electronic states being probed and their relative surface contributions, thereby offering additional insight into the surface specificity of SHG signals from QDs.},
doi = {10.1021/jp510357p},
journal = {Journal of Physical Chemistry. C},
number = 5,
volume = 119,
place = {United States},
year = {Wed Jan 07 00:00:00 EST 2015},
month = {Wed Jan 07 00:00:00 EST 2015}
}
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