Observation of Three-Photon Cascaded Emission from Triexcitons in Giant CsPbBr3 Quantum Dots at Room Temperature

Miri Kazes; Dekel Nakar; Ihor Cherniukh; Maryna I. Bodnarchuk; Leon G. Feld; Chenglian Zhu; Daniel Amgar; Gabriele Rainò; Maksym V. Kovalenko; Dan Oron

doi:10.1021/acs.nanolett.4c03096

Observation of Three-Photon Cascaded Emission from Triexcitons in Giant CsPbBr₃ Quantum Dots at Room Temperature

Miri Kazes, Dekel Nakar, Ihor Cherniukh, Maryna I. Bodnarchuk, Leon G. Feld, Chenglian Zhu, Daniel Amgar, Gabriele Rainò^*, Maksym V. Kovalenko^*, Dan Oron^*

^*Corresponding author for this work

Department of Physics of Complex Systems

Research output: Contribution to journal › Article › peer-review

Abstract

Colloidal semiconductor nanocrystals have long been considered a promising source of time-correlated and entangled photons via the cascaded emission of multiexcitonic states. The spectroscopy of such cascaded emission, however, is hindered by efficient nonradiative Auger-Meitner decay, rendering multiexcitonic states nonemissive. Here we present room-temperature heralded spectroscopy of three-photon cascades from triexcitons in giant CsPbBr₃ nanocrystals. We show that this system exhibits second- and third-order correlation function values, g⁽²⁾(0) and g⁽³⁾(0,0), close to unity, identifying very weak binding of both biexcitons and triexcitons. Combining fluorescence lifetime analysis, photon statistics, and spectroscopy, we can readily identify emission from higher multiexcitonic states. We use this to verify emission from a single emitter despite high emission quantum yields of multiply excited states and comparable emission lifetimes of singly and multiply excited states. Finally, we present potential pathways toward control of the photon number statistics of multiexcitonic emission cascades.

Original language	English
Pages (from-to)	13185-13191
Number of pages	7
Journal	Nano Letters
Volume	24
Issue number	42
Early online date	14 Oct 2024
DOIs	https://doi.org/10.1021/acs.nanolett.4c03096
Publication status	Published - 23 Oct 2024

Funding

The authors gratefully acknowledge funding by the Weizmann-ETH Zurich Bridge Program. I.C., M.I.B., C.Z., and G.R. acknowledge funding from the Swiss National Science Foundation (Grant No. 200021_192308, “Q-Light – Engineered Quantum Light Sources with Nanocrystal Assemblies”). M.V.K. is thankful for the funding received from the European Union through the Horizon 2020 Research and Innovation Program (Grant 819740, Project SCALE-HALO). D.O. Acknowledges support by the Israel Science Foundation (ISF) and the Directorate for Defense Research and Development (DDR&D), grant no. 3415/21. This publication was partially created as part of NCCR Catalysis (grant number 180544), a National Centre of Competence in Research funded by the Swiss National Science Foundation. D.A. gratefully acknowledges support by the VATAT Fellowship for female PhD students in Physics/Math and Computer Science. D.O. is the incumbent of the Harry Weinrebe professorial chair of laser physics. Publisher Copyright: © 2024 American Chemical Society.

All Science Journal Classification (ASJC) codes

Bioengineering
General Chemistry
General Materials Science
Condensed Matter Physics
Mechanical Engineering

Access to Document

10.1021/acs.nanolett.4c03096Licence: CC BY

Cite this

@article{fce5cbe9cc3e41d4b0d363f10cebdd6d,

title = "Observation of Three-Photon Cascaded Emission from Triexcitons in Giant CsPbBr3 Quantum Dots at Room Temperature",

abstract = "Colloidal semiconductor nanocrystals have long been considered a promising source of time-correlated and entangled photons via the cascaded emission of multiexcitonic states. The spectroscopy of such cascaded emission, however, is hindered by efficient nonradiative Auger-Meitner decay, rendering multiexcitonic states nonemissive. Here we present room-temperature heralded spectroscopy of three-photon cascades from triexcitons in giant CsPbBr3 nanocrystals. We show that this system exhibits second- and third-order correlation function values, g(2)(0) and g(3)(0,0), close to unity, identifying very weak binding of both biexcitons and triexcitons. Combining fluorescence lifetime analysis, photon statistics, and spectroscopy, we can readily identify emission from higher multiexcitonic states. We use this to verify emission from a single emitter despite high emission quantum yields of multiply excited states and comparable emission lifetimes of singly and multiply excited states. Finally, we present potential pathways toward control of the photon number statistics of multiexcitonic emission cascades.",

author = "Miri Kazes and Dekel Nakar and Ihor Cherniukh and Bodnarchuk, {Maryna I.} and Feld, {Leon G.} and Chenglian Zhu and Daniel Amgar and Gabriele Rain{\`o} and Kovalenko, {Maksym V.} and Dan Oron",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

year = "2024",

month = oct,

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doi = "10.1021/acs.nanolett.4c03096",

language = "English",

volume = "24",

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T1 - Observation of Three-Photon Cascaded Emission from Triexcitons in Giant CsPbBr3 Quantum Dots at Room Temperature

AU - Kazes, Miri

AU - Nakar, Dekel

AU - Cherniukh, Ihor

AU - Bodnarchuk, Maryna I.

AU - Feld, Leon G.

AU - Zhu, Chenglian

AU - Amgar, Daniel

AU - Rainò, Gabriele

AU - Kovalenko, Maksym V.

AU - Oron, Dan

PY - 2024/10/23

Y1 - 2024/10/23

N2 - Colloidal semiconductor nanocrystals have long been considered a promising source of time-correlated and entangled photons via the cascaded emission of multiexcitonic states. The spectroscopy of such cascaded emission, however, is hindered by efficient nonradiative Auger-Meitner decay, rendering multiexcitonic states nonemissive. Here we present room-temperature heralded spectroscopy of three-photon cascades from triexcitons in giant CsPbBr3 nanocrystals. We show that this system exhibits second- and third-order correlation function values, g(2)(0) and g(3)(0,0), close to unity, identifying very weak binding of both biexcitons and triexcitons. Combining fluorescence lifetime analysis, photon statistics, and spectroscopy, we can readily identify emission from higher multiexcitonic states. We use this to verify emission from a single emitter despite high emission quantum yields of multiply excited states and comparable emission lifetimes of singly and multiply excited states. Finally, we present potential pathways toward control of the photon number statistics of multiexcitonic emission cascades.

AB - Colloidal semiconductor nanocrystals have long been considered a promising source of time-correlated and entangled photons via the cascaded emission of multiexcitonic states. The spectroscopy of such cascaded emission, however, is hindered by efficient nonradiative Auger-Meitner decay, rendering multiexcitonic states nonemissive. Here we present room-temperature heralded spectroscopy of three-photon cascades from triexcitons in giant CsPbBr3 nanocrystals. We show that this system exhibits second- and third-order correlation function values, g(2)(0) and g(3)(0,0), close to unity, identifying very weak binding of both biexcitons and triexcitons. Combining fluorescence lifetime analysis, photon statistics, and spectroscopy, we can readily identify emission from higher multiexcitonic states. We use this to verify emission from a single emitter despite high emission quantum yields of multiply excited states and comparable emission lifetimes of singly and multiply excited states. Finally, we present potential pathways toward control of the photon number statistics of multiexcitonic emission cascades.

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