Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

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

doi:10.1038/ncomms11010

Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

Journal Article · Thu Mar 17 00:00:00 EDT 2016 · Nature Communications

DOI:https://doi.org/10.1038/ncomms11010· OSTI ID:1255251

Soavi, Giancarlo ^[1]; Dal Conte, Stefano ^[2]; Manzoni, Cristian ^[2]; Viola, Daniele ^[3]; Narita, Akimitsu ^[4]; Hu, Yunbin ^[4]; Feng, Xinliang ^[4]; Hohenester, Ulrich ^[5]; Molinari, Elisa ^[6]; Prezzi, Deborah ^[7]; Mullen, Klaus ^[4]; Cerullo, Giulio ^[8]

Politecnico di Milano, Milano (Italy); Univ. of Cambridge, Cambridge (United Kingdom); University of Cambridge, UK
Istituto di Fotonica e Nanotecnologie, Milano (Italy)
Politecnico di Milano, Milano (Italy)
Max Planck Institute for Polymer Research, Mainz (Germany)
Univ. of Graz, Graz (Austria)
Univ. di Modena e Reggio Emilia, Modena (Italy); Istituto Nanoscience, Modena (Italy)
Istituto Nanoscience, Modena (Italy)
Politecnico di Milano, Milano (Italy); Istituto di Fotonica e Nanotecnologie, Milano (Italy)

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven Science Associates, LLC, Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1255251

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Screening of long-range Coulomb interaction in graphene nanoribbons: Armchair versus zigzag edges Hadipour, H.; Şaşıoğlu, E.; Bagherpour, F. Physical Review B, Vol. 98, Issue 20 https://doi.org/10.1103/physrevb.98.205123	journal	November 2018
Exciton absorption spectra in narrow armchair graphene nanoribbons in an electric field Monozon, B. S.; Schmelcher, P. Physical Review B, Vol. 99, Issue 16 https://doi.org/10.1103/physrevb.99.165415	journal	April 2019
Termini effects on the optical properties of graphene nanoribbons Cardoso, Claudia; Ferretti, Andrea; Prezzi, Deborah The European Physical Journal B, Vol. 91, Issue 11 https://doi.org/10.1140/epjb/e2018-90179-4	journal	November 2018
Multiple Exciton Generation in Nanostructures for Advanced Photovoltaic Cells Siemons, Nicholas; Serafini, Alessio Journal of Nanotechnology, Vol. 2018 https://doi.org/10.1155/2018/7285483	journal	January 2018
Onset of exciton-exciton annihilation in single layer black phosphorus Surrente, A.; Mitioglu, A. A.; Galkowski, K. arXiv https://doi.org/10.48550/arxiv.1605.06998	text	January 2016
Exciton absorption spectra in narrow armchair graphene nanoribbons in electric fields Monozon, B. S.; Schmelcher, P. arXiv https://doi.org/10.48550/arxiv.1812.06450	text	January 2018

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