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Direct Visualization of Confinement and Many-Body Correlation Effects in 2D Spectroscopy of Quantum Dots

Amarotti, Edoardo LU ; Wang, Zhengjun LU ; Hedse, Albin LU ; Lenngren, Nils LU ; Žídek, Karel LU ; Zheng, Kaibo LU ; Zigmantas, Donatas LU orcid and Pullerits, Tõnu LU (2024) In Advanced Optical Materials
Abstract

The size tunable color of colloidal semiconductor quantum dots (QDs) is probably the most elegant illustration of the quantum confinement effect. As explained by the simple “particle-in-a-box” model, the transition energies between the levels increase when the “box” becomes smaller. To investigate quantum confinement effects, typically a well-defined narrow size distribution of the nanoparticles is needed. In this contribution, how coherent electronic two-dimensional spectroscopy (2DES) can directly visualize the quantum size effect in a sample with broad size distribution of QDs is demonstrated. The method is based on two features of the 2DES – the ability to resolve inhomogeneous broadening and the capability to reveal correlations... (More)

The size tunable color of colloidal semiconductor quantum dots (QDs) is probably the most elegant illustration of the quantum confinement effect. As explained by the simple “particle-in-a-box” model, the transition energies between the levels increase when the “box” becomes smaller. To investigate quantum confinement effects, typically a well-defined narrow size distribution of the nanoparticles is needed. In this contribution, how coherent electronic two-dimensional spectroscopy (2DES) can directly visualize the quantum size effect in a sample with broad size distribution of QDs is demonstrated. The method is based on two features of the 2DES – the ability to resolve inhomogeneous broadening and the capability to reveal correlations between the states. In QD samples, inhomogeneous spectral broadening is mainly caused by the size distribution and leads to elongated diagonal peaks of the spectra. Since the cross peaks correlate the energies of two states, they allow drawing conclusions about the size dependence of the corresponding states. It is also found that the biexciton binding energy changes between 3 and 8 meV with the QD size. Remarkably, the size dependence is non-monotonic with a clear minimum.

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author
; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
epub
subject
keywords
2D electronic spectroscopy, biexciton, binding energy, quantum dots, size dependence, ultrafast spectroscopy
in
Advanced Optical Materials
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:85185452876
ISSN
2195-1071
DOI
10.1002/adom.202302968
language
English
LU publication?
yes
id
d7130e56-2006-47e3-94dc-21048d13b9be
date added to LUP
2024-03-20 13:50:15
date last changed
2024-03-25 11:11:01
@article{d7130e56-2006-47e3-94dc-21048d13b9be,
  abstract     = {{<p>The size tunable color of colloidal semiconductor quantum dots (QDs) is probably the most elegant illustration of the quantum confinement effect. As explained by the simple “particle-in-a-box” model, the transition energies between the levels increase when the “box” becomes smaller. To investigate quantum confinement effects, typically a well-defined narrow size distribution of the nanoparticles is needed. In this contribution, how coherent electronic two-dimensional spectroscopy (2DES) can directly visualize the quantum size effect in a sample with broad size distribution of QDs is demonstrated. The method is based on two features of the 2DES – the ability to resolve inhomogeneous broadening and the capability to reveal correlations between the states. In QD samples, inhomogeneous spectral broadening is mainly caused by the size distribution and leads to elongated diagonal peaks of the spectra. Since the cross peaks correlate the energies of two states, they allow drawing conclusions about the size dependence of the corresponding states. It is also found that the biexciton binding energy changes between 3 and 8 meV with the QD size. Remarkably, the size dependence is non-monotonic with a clear minimum.</p>}},
  author       = {{Amarotti, Edoardo and Wang, Zhengjun and Hedse, Albin and Lenngren, Nils and Žídek, Karel and Zheng, Kaibo and Zigmantas, Donatas and Pullerits, Tõnu}},
  issn         = {{2195-1071}},
  keywords     = {{2D electronic spectroscopy; biexciton; binding energy; quantum dots; size dependence; ultrafast spectroscopy}},
  language     = {{eng}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Advanced Optical Materials}},
  title        = {{Direct Visualization of Confinement and Many-Body Correlation Effects in 2D Spectroscopy of Quantum Dots}},
  url          = {{http://dx.doi.org/10.1002/adom.202302968}},
  doi          = {{10.1002/adom.202302968}},
  year         = {{2024}},
}