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Title: Spectrally Resolved Photodynamics of Individual Emitters in Large-Area Monolayers of Hexagonal Boron Nitride

Abstract

Hexagonal boron nitride (h-BN) is a 2D, wide band gap semiconductor that has recently been shown to display bright room-temperature emission in the visible region, sparking immense interest in the material for use in quantum applications. In this work, we study highly crystalline, single atomic layers of chemical vapor deposition grown h-BN and find predominantly one type of emissive state. Using a multidimensional super-resolution fluorescence microscopy technique we simultaneously measure spatial position, intensity, and spectral properties of the emitters, as they are exposed to continuous wave illumination over minutes. As well as low emitter heterogeneity, we observe inhomogeneous broadening of emitter line-widths and power law dependency in fluorescence intermittency; this is strikingly similar to previous work on quantum dots. Lastly, these results show that high control over h-BN growth and treatment can produce a narrow distribution of emitter type and that surface interactions heavily influence the photodynamics. Furthermore, we highlight the utility of spectrally resolved wide-field microscopy in the study of optically active excitations in atomically thin two-dimensional materials.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [2]; ORCiD logo [3];  [1]; ORCiD logo [1];  [1]
  1. Univ. of Cambridge, Cambridge (United Kingdom)
  2. Univ. of California, Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoSciences Inst., Berkeley, CA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Photonics at Thermodynamic Limits (PTL); Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1566580
Grant/Contract Number:  
SC0019140
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 4; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; optics; phonons; thermal conductivity; charge transport; materials and chemistry by design; mesostructured materials; synthesis (novel materials)

Citation Formats

Stern, Hannah L., Wang, Ruizhi, Fan, Ye, Mizuta, Ryo, Stewart, James C., Needham, Lisa -Maria, Roberts, Trevor D., Wai, Rebecca, Ginsberg, Naomi S., Klenerman, David, Hofmann, Stephan, and Lee, Steven F. Spectrally Resolved Photodynamics of Individual Emitters in Large-Area Monolayers of Hexagonal Boron Nitride. United States: N. p., 2019. Web. doi:10.1021/acsnano.9b00274.
Stern, Hannah L., Wang, Ruizhi, Fan, Ye, Mizuta, Ryo, Stewart, James C., Needham, Lisa -Maria, Roberts, Trevor D., Wai, Rebecca, Ginsberg, Naomi S., Klenerman, David, Hofmann, Stephan, & Lee, Steven F. Spectrally Resolved Photodynamics of Individual Emitters in Large-Area Monolayers of Hexagonal Boron Nitride. United States. https://doi.org/10.1021/acsnano.9b00274
Stern, Hannah L., Wang, Ruizhi, Fan, Ye, Mizuta, Ryo, Stewart, James C., Needham, Lisa -Maria, Roberts, Trevor D., Wai, Rebecca, Ginsberg, Naomi S., Klenerman, David, Hofmann, Stephan, and Lee, Steven F. Wed . "Spectrally Resolved Photodynamics of Individual Emitters in Large-Area Monolayers of Hexagonal Boron Nitride". United States. https://doi.org/10.1021/acsnano.9b00274. https://www.osti.gov/servlets/purl/1566580.
@article{osti_1566580,
title = {Spectrally Resolved Photodynamics of Individual Emitters in Large-Area Monolayers of Hexagonal Boron Nitride},
author = {Stern, Hannah L. and Wang, Ruizhi and Fan, Ye and Mizuta, Ryo and Stewart, James C. and Needham, Lisa -Maria and Roberts, Trevor D. and Wai, Rebecca and Ginsberg, Naomi S. and Klenerman, David and Hofmann, Stephan and Lee, Steven F.},
abstractNote = {Hexagonal boron nitride (h-BN) is a 2D, wide band gap semiconductor that has recently been shown to display bright room-temperature emission in the visible region, sparking immense interest in the material for use in quantum applications. In this work, we study highly crystalline, single atomic layers of chemical vapor deposition grown h-BN and find predominantly one type of emissive state. Using a multidimensional super-resolution fluorescence microscopy technique we simultaneously measure spatial position, intensity, and spectral properties of the emitters, as they are exposed to continuous wave illumination over minutes. As well as low emitter heterogeneity, we observe inhomogeneous broadening of emitter line-widths and power law dependency in fluorescence intermittency; this is strikingly similar to previous work on quantum dots. Lastly, these results show that high control over h-BN growth and treatment can produce a narrow distribution of emitter type and that surface interactions heavily influence the photodynamics. Furthermore, we highlight the utility of spectrally resolved wide-field microscopy in the study of optically active excitations in atomically thin two-dimensional materials.},
doi = {10.1021/acsnano.9b00274},
journal = {ACS Nano},
number = 4,
volume = 13,
place = {United States},
year = {Wed Mar 13 00:00:00 EDT 2019},
month = {Wed Mar 13 00:00:00 EDT 2019}
}

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Cited by: 35 works
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Works referencing / citing this record:

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