Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/CdxZn1–xSe Quantum Dots
Abstract
Colloidal CdSe quantum dots (QDs) designed with a high degree of asymmetric internal strain have recently been shown to host a number of desirable optical properties including subthermal room-temperature line widths, suppressed spectral diffusion, and high photoluminescence (PL) quantum yields. It remains an open question, however, whether they are well-suited for applications requiring emission of identical single photons. Here we measure the low-temperature PL dynamics and the polarization-resolved fluorescence line narrowing spectra from ensembles of these strained QDs. Our spectroscopy reveals the radiative recombination rates of bright and dark excitons, the relaxation rate between the two, and the energy spectra of the quantized acoustic phonons in the QDs that can contribute to relaxation processes. In comparison to conventional colloidal CdSe/ZnS core/shell QDs, we find that in asymmetrically strained CdSe QDs over six times more light is emitted directly by the bright exciton. Furthermore, these results are therefore encouraging for the prospects of chemically synthesized colloidal QDs as emitters of single indistinguishable photons.
- Authors:
-
[2];
[2];
[2];
[2]
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Alabama, Tuscaloosa, AL (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1822763
- Report Number(s):
- LA-UR-21-23484
Journal ID: ISSN 1936-0851
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 9; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; High Magnetic Field Science; nanocrystal; colloidal quantum dot; single-photon emitter; exciton fine structure; acoustic phonon; bright exciton; exciton; phonons; quantum dots; energy; cadmium selenide
Citation Formats
Fedin, Igor, Goryca, Mateusz, Liu, Dan, Tretiak, Sergei, Klimov, Victor I., and Crooker, Scott A. Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/CdxZn1–xSe Quantum Dots. United States: N. p., 2021.
Web. doi:10.1021/acsnano.1c03864.
Fedin, Igor, Goryca, Mateusz, Liu, Dan, Tretiak, Sergei, Klimov, Victor I., & Crooker, Scott A. Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/CdxZn1–xSe Quantum Dots. United States. https://doi.org/10.1021/acsnano.1c03864
Fedin, Igor, Goryca, Mateusz, Liu, Dan, Tretiak, Sergei, Klimov, Victor I., and Crooker, Scott A. Thu .
"Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/CdxZn1–xSe Quantum Dots". United States. https://doi.org/10.1021/acsnano.1c03864. https://www.osti.gov/servlets/purl/1822763.
@article{osti_1822763,
title = {Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/CdxZn1–xSe Quantum Dots},
author = {Fedin, Igor and Goryca, Mateusz and Liu, Dan and Tretiak, Sergei and Klimov, Victor I. and Crooker, Scott A.},
abstractNote = {Colloidal CdSe quantum dots (QDs) designed with a high degree of asymmetric internal strain have recently been shown to host a number of desirable optical properties including subthermal room-temperature line widths, suppressed spectral diffusion, and high photoluminescence (PL) quantum yields. It remains an open question, however, whether they are well-suited for applications requiring emission of identical single photons. Here we measure the low-temperature PL dynamics and the polarization-resolved fluorescence line narrowing spectra from ensembles of these strained QDs. Our spectroscopy reveals the radiative recombination rates of bright and dark excitons, the relaxation rate between the two, and the energy spectra of the quantized acoustic phonons in the QDs that can contribute to relaxation processes. In comparison to conventional colloidal CdSe/ZnS core/shell QDs, we find that in asymmetrically strained CdSe QDs over six times more light is emitted directly by the bright exciton. Furthermore, these results are therefore encouraging for the prospects of chemically synthesized colloidal QDs as emitters of single indistinguishable photons.},
doi = {10.1021/acsnano.1c03864},
journal = {ACS Nano},
number = 9,
volume = 15,
place = {United States},
year = {Thu Sep 02 00:00:00 EDT 2021},
month = {Thu Sep 02 00:00:00 EDT 2021}
}
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