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Title: Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

Abstract

Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron–hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton–exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈250meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. As a result, these observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.

Authors:
 [1];  [2];  [2];  [3];  [4];  [4];  [4];  [5];  [6];  [7];  [4];  [8]
+ Show Author Affiliations
  1. Politecnico di Milano, Milano (Italy); Univ. of Cambridge, Cambridge (United Kingdom)
  2. Istituto di Fotonica e Nanotecnologie, Milano (Italy)
  3. Politecnico di Milano, Milano (Italy)
  4. Max Planck Institute for Polymer Research, Mainz (Germany)
  5. Univ. of Graz, Graz (Austria)
  6. Univ. di Modena e Reggio Emilia, Modena (Italy); Istituto Nanoscience, Modena (Italy)
  7. Istituto Nanoscience, Modena (Italy)
  8. Politecnico di Milano, Milano (Italy); Istituto di Fotonica e Nanotecnologie, Milano (Italy)
Publication Date:
Research Org.:
Brookhaven Science Associates, LLC, Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1255251
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Soavi, Giancarlo, Dal Conte, Stefano, Manzoni, Cristian, Viola, Daniele, Narita, Akimitsu, Hu, Yunbin, Feng, Xinliang, Hohenester, Ulrich, Molinari, Elisa, Prezzi, Deborah, Mullen, Klaus, and Cerullo, Giulio. Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons. United States: N. p., 2016. Web. doi:10.1038/ncomms11010.
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Soavi, Giancarlo, Dal Conte, Stefano, Manzoni, Cristian, Viola, Daniele, Narita, Akimitsu, Hu, Yunbin, Feng, Xinliang, Hohenester, Ulrich, Molinari, Elisa, Prezzi, Deborah, Mullen, Klaus, & Cerullo, Giulio. Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons. United States. https://doi.org/10.1038/ncomms11010
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Soavi, Giancarlo, Dal Conte, Stefano, Manzoni, Cristian, Viola, Daniele, Narita, Akimitsu, Hu, Yunbin, Feng, Xinliang, Hohenester, Ulrich, Molinari, Elisa, Prezzi, Deborah, Mullen, Klaus, and Cerullo, Giulio. Thu . "Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons". United States. https://doi.org/10.1038/ncomms11010. https://www.osti.gov/servlets/purl/1255251.
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@article{osti_1255251,
title = {Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons},
author = {Soavi, Giancarlo and Dal Conte, Stefano and Manzoni, Cristian and Viola, Daniele and Narita, Akimitsu and Hu, Yunbin and Feng, Xinliang and Hohenester, Ulrich and Molinari, Elisa and Prezzi, Deborah and Mullen, Klaus and Cerullo, Giulio},
abstractNote = {Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron–hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton–exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈250meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. As a result, these observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.},
doi = {10.1038/ncomms11010},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Thu Mar 17 00:00:00 EDT 2016},
month = {Thu Mar 17 00:00:00 EDT 2016}
}
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https://doi.org/10.1038/ncomms11010
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Room temperature magnetic order on zigzag edges of narrow graphene nanoribbons
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Optical spectrum of bottom-up graphene nanoribbons: towards efficient atom-thick excitonic solar cells
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Half-Metallic Graphene Nanoribbons
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Excitonic Effects in the Optical Spectra of Graphene Nanoribbons
text, January 2007

Biexciton stability in carbon nanotubes
text, January 2007

Room temperature magnetic order on zigzag edges of narrow graphene nanoribbons
text, January 2014

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Atomically controlled substitutional boron-doping of graphene nanoribbons
text, January 2015

Exciton-dominated optical response of ultra-narrow graphene nanoribbons
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  • DOI: 10.7892/boris.58130
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