Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons

Here, we demonstrate a bias-driven superluminescent point light-source based on an optically pumped molecular junction (gold substrate/self-assembled molecular monolayer/gold tip) of a scanning tunneling microscope, operating at ambient conditions and providing almost three orders of magnitude highe...

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Main Authors: Kai Braun, Xiao Wang, Andreas M. Kern, Hilmar Adler, Heiko Peisert, Thomas Chassé, Dai Zhang, Alfred J. Meixner
Format: Article
Language:English
Published: Beilstein-Institut 2015-05-01
Series:Beilstein Journal of Nanotechnology
Subjects:
Online Access:https://doi.org/10.3762/bjnano.6.111
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author Kai Braun
Xiao Wang
Andreas M. Kern
Hilmar Adler
Heiko Peisert
Thomas Chassé
Dai Zhang
Alfred J. Meixner
author_facet Kai Braun
Xiao Wang
Andreas M. Kern
Hilmar Adler
Heiko Peisert
Thomas Chassé
Dai Zhang
Alfred J. Meixner
author_sort Kai Braun
collection DOAJ
description Here, we demonstrate a bias-driven superluminescent point light-source based on an optically pumped molecular junction (gold substrate/self-assembled molecular monolayer/gold tip) of a scanning tunneling microscope, operating at ambient conditions and providing almost three orders of magnitude higher electron-to-photon conversion efficiency than electroluminescence induced by inelastic tunneling without optical pumping. A positive, steadily increasing bias voltage induces a step-like rise of the Stokes shifted optical signal emitted from the junction. This emission is strongly attenuated by reversing the applied bias voltage. At high bias voltage, the emission intensity depends non-linearly on the optical pump power. The enhanced emission can be modelled by rate equations taking into account hole injection from the tip (anode) into the highest occupied orbital of the closest substrate-bound molecule (lower level) and radiative recombination with an electron from above the Fermi level (upper level), hence feeding photons back by stimulated emission resonant with the gap mode. The system reflects many essential features of a superluminescent light emitting diode.
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spelling doaj.art-2ec6e95811a743b0ba58a9d9d9f836892022-12-22T01:38:15ZengBeilstein-InstitutBeilstein Journal of Nanotechnology2190-42862015-05-01611100110610.3762/bjnano.6.1112190-4286-6-111Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electronsKai Braun0Xiao Wang1Andreas M. Kern2Hilmar Adler3Heiko Peisert4Thomas Chassé5Dai Zhang6Alfred J. Meixner7Institute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyInstitute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyInstitute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyInstitute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyInstitute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyInstitute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyInstitute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyInstitute of Physical and Theoretical Chemistry, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, GermanyHere, we demonstrate a bias-driven superluminescent point light-source based on an optically pumped molecular junction (gold substrate/self-assembled molecular monolayer/gold tip) of a scanning tunneling microscope, operating at ambient conditions and providing almost three orders of magnitude higher electron-to-photon conversion efficiency than electroluminescence induced by inelastic tunneling without optical pumping. A positive, steadily increasing bias voltage induces a step-like rise of the Stokes shifted optical signal emitted from the junction. This emission is strongly attenuated by reversing the applied bias voltage. At high bias voltage, the emission intensity depends non-linearly on the optical pump power. The enhanced emission can be modelled by rate equations taking into account hole injection from the tip (anode) into the highest occupied orbital of the closest substrate-bound molecule (lower level) and radiative recombination with an electron from above the Fermi level (upper level), hence feeding photons back by stimulated emission resonant with the gap mode. The system reflects many essential features of a superluminescent light emitting diode.https://doi.org/10.3762/bjnano.6.111inelastic tunnelinglight emitting diodequantum plasmonicsscanning near-field optical microscopytip-enhanced Raman spectroscopy
spellingShingle Kai Braun
Xiao Wang
Andreas M. Kern
Hilmar Adler
Heiko Peisert
Thomas Chassé
Dai Zhang
Alfred J. Meixner
Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons
Beilstein Journal of Nanotechnology
inelastic tunneling
light emitting diode
quantum plasmonics
scanning near-field optical microscopy
tip-enhanced Raman spectroscopy
title Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons
title_full Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons
title_fullStr Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons
title_full_unstemmed Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons
title_short Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons
title_sort superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons
topic inelastic tunneling
light emitting diode
quantum plasmonics
scanning near-field optical microscopy
tip-enhanced Raman spectroscopy
url https://doi.org/10.3762/bjnano.6.111
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