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Title: Single Nanocrystal Spectroscopy of Shortwave Infrared Emitters

Abstract

Short-wave infrared (SWIR) emitters are at the center of ground-breaking applications in biomedical imaging, next-generation optoelectronic devices, and optical communications. Colloidal nanocrystals based on indium arsenide are some of the most promising SWIR emitters to date. However, the lack of single-particle spectroscopic methods accessible in the SWIR has prevented advances in both nanocrystal synthesis and fundamental characterization of emitters. In this paper, we demonstrate an implementation of a solution photon correlation Fourier spectroscopy (s-PCFS) experiment utilizing the SWIR sensitivity and time resolution of superconducting nanowire single-photon detectors to extract single-particle emission linewidths from colloidal indium arsenide/cadmium selenide (InAs/CdSe) core/shell nanocrystals emissive from 1.2 to 1.6 μm. We show that the average single InAs/CdSe nanocrystal fluorescence linewidth is, remarkably, as narrow as 52 meV, similar to what has been observed in some of the most narrowband nanostructured emitters in the visible region. Additionally, the single nanocrystal fluorescence linewidth increases with increasing shell thickness, suggesting exciton–phonon coupling as the dominant emission line-broadening mechanism in this system. The development of the SWIR s-PCFS technique has enabled measurements of spectral linewidths of colloidal SWIR-emissive NCs in solution and provides a platform to study the single NC spectral characteristics of SWIR emitters.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1];  [3];  [3]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
  2. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry
  3. MIT Lincoln Lab., Lexington, MA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1566578
Grant/Contract Number:  
FG02-07ER46454; SC0001088
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 2; 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; solar (photovoltaic); solid state lighting; photosynthesis (natural and artificial); charge transport; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); nanocrystals; single-molecule spectroscopy; short-wave infrared; indium arsenide; core/shell

Citation Formats

Bertram, Sophie N., Spokoyny, Boris, Franke, Daniel, Caram, Justin R., Yoo, Jason J., Murphy, Ryan P., Grein, Matthew E., and Bawendi, Moungi G. Single Nanocrystal Spectroscopy of Shortwave Infrared Emitters. United States: N. p., 2018. Web. doi:10.1021/acsnano.8b07578.
Bertram, Sophie N., Spokoyny, Boris, Franke, Daniel, Caram, Justin R., Yoo, Jason J., Murphy, Ryan P., Grein, Matthew E., & Bawendi, Moungi G. Single Nanocrystal Spectroscopy of Shortwave Infrared Emitters. United States. doi:10.1021/acsnano.8b07578.
Bertram, Sophie N., Spokoyny, Boris, Franke, Daniel, Caram, Justin R., Yoo, Jason J., Murphy, Ryan P., Grein, Matthew E., and Bawendi, Moungi G. Fri . "Single Nanocrystal Spectroscopy of Shortwave Infrared Emitters". United States. doi:10.1021/acsnano.8b07578. https://www.osti.gov/servlets/purl/1566578.
@article{osti_1566578,
title = {Single Nanocrystal Spectroscopy of Shortwave Infrared Emitters},
author = {Bertram, Sophie N. and Spokoyny, Boris and Franke, Daniel and Caram, Justin R. and Yoo, Jason J. and Murphy, Ryan P. and Grein, Matthew E. and Bawendi, Moungi G.},
abstractNote = {Short-wave infrared (SWIR) emitters are at the center of ground-breaking applications in biomedical imaging, next-generation optoelectronic devices, and optical communications. Colloidal nanocrystals based on indium arsenide are some of the most promising SWIR emitters to date. However, the lack of single-particle spectroscopic methods accessible in the SWIR has prevented advances in both nanocrystal synthesis and fundamental characterization of emitters. In this paper, we demonstrate an implementation of a solution photon correlation Fourier spectroscopy (s-PCFS) experiment utilizing the SWIR sensitivity and time resolution of superconducting nanowire single-photon detectors to extract single-particle emission linewidths from colloidal indium arsenide/cadmium selenide (InAs/CdSe) core/shell nanocrystals emissive from 1.2 to 1.6 μm. We show that the average single InAs/CdSe nanocrystal fluorescence linewidth is, remarkably, as narrow as 52 meV, similar to what has been observed in some of the most narrowband nanostructured emitters in the visible region. Additionally, the single nanocrystal fluorescence linewidth increases with increasing shell thickness, suggesting exciton–phonon coupling as the dominant emission line-broadening mechanism in this system. The development of the SWIR s-PCFS technique has enabled measurements of spectral linewidths of colloidal SWIR-emissive NCs in solution and provides a platform to study the single NC spectral characteristics of SWIR emitters.},
doi = {10.1021/acsnano.8b07578},
journal = {ACS Nano},
issn = {1936-0851},
number = 2,
volume = 13,
place = {United States},
year = {2018},
month = {11}
}

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