Biexciton Binding Energy and Line width of Single Quantum Dots at Room Temperature

Sander J.W. Vonk; Bart A.J. Heemskerk; Robert C. Keitel; Stijn O.M. Hinterding; Jaco J. Geuchies; Arjan J. Houtepen; Freddy T. Rabouw

doi:10.1021/acs.nanolett.1c01556

Biexciton Binding Energy and Line width of Single Quantum Dots at Room Temperature

Sander J.W. Vonk, Bart A.J. Heemskerk, Robert C. Keitel, Stijn O.M. Hinterding, Jaco J. Geuchies, Arjan J. Houtepen, Freddy T. Rabouw^*

^*Corresponding author for this work

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

Abstract

Broadening of multiexciton emission from colloidal quantum dots (QDs) at room temperature is important for their use in high-power applications, but an in-depth characterization has not been possible until now. We present and apply a novel spectroscopic method to quantify the biexciton line width and biexciton binding energy of single CdSe/CdS/ZnS colloidal QDs at room temperature. In our method, which we term “cascade spectroscopy”, we select emission events from the biexciton cascade and reconstruct their spectrum. The biexciton has an average emission line width of 86 meV on the single-QD scale, similar to that of the exciton. Variations in the biexciton repulsion (E_b= 4.0 ± 3.1 meV; mean ± standard deviation of 15 QDs) are correlated with but are more narrowly distributed than variations in the exciton energy (10.0 meV standard deviation). Using a simple quantum-mechanical model, we conclude that inhomogeneous broadening in our sample is primarily due to variations in the CdS shell thickness.

Original language	English
Pages (from-to)	5760-5766
Number of pages	7
Journal	Nano Letters
Volume	21
Issue number	13
DOIs	https://doi.org/10.1021/acs.nanolett.1c01556
Publication status	Published - 14 Jul 2021

Bibliographical note

Funding Information:
This work was supported by the Dutch Research Council NWO (OCENW.KLEIN.008). F.T.R. acknowledges financial support from The Netherlands Organisation for Scientific Research NWO (VENI grant number 722.017.002) and The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). J.J.G. and A.J.H. acknowledge support from European Research Council Horizon 2020 ERC Grant Agreement 678004 (Doping on Demand). R.C.K. acknowledges support from the European Research Council (ERC; FP/2007-2013), ERC Grant Agreement No. 339905 (QuaDoPS Advanced Grant). Peter Helfferich is thanked for technical support setting up the galvo-APD setup.

Publisher Copyright:
© 2021 The Authors. Published by American Chemical Society

Funding

This work was supported by the Dutch Research Council NWO (OCENW.KLEIN.008). F.T.R. acknowledges financial support from The Netherlands Organisation for Scientific Research NWO (VENI grant number 722.017.002) and The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). J.J.G. and A.J.H. acknowledge support from European Research Council Horizon 2020 ERC Grant Agreement 678004 (Doping on Demand). R.C.K. acknowledges support from the European Research Council (ERC; FP/2007-2013), ERC Grant Agreement No. 339905 (QuaDoPS Advanced Grant). Peter Helfferich is thanked for technical support setting up the galvo-APD setup.

Keywords

biexciton line width
multiexciton emission
quantum dots
single-quantum-dot spectroscopy

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title = "Biexciton Binding Energy and Line width of Single Quantum Dots at Room Temperature",

abstract = "Broadening of multiexciton emission from colloidal quantum dots (QDs) at room temperature is important for their use in high-power applications, but an in-depth characterization has not been possible until now. We present and apply a novel spectroscopic method to quantify the biexciton line width and biexciton binding energy of single CdSe/CdS/ZnS colloidal QDs at room temperature. In our method, which we term “cascade spectroscopy”, we select emission events from the biexciton cascade and reconstruct their spectrum. The biexciton has an average emission line width of 86 meV on the single-QD scale, similar to that of the exciton. Variations in the biexciton repulsion (Eb= 4.0 ± 3.1 meV; mean ± standard deviation of 15 QDs) are correlated with but are more narrowly distributed than variations in the exciton energy (10.0 meV standard deviation). Using a simple quantum-mechanical model, we conclude that inhomogeneous broadening in our sample is primarily due to variations in the CdS shell thickness.",

keywords = "biexciton line width, multiexciton emission, quantum dots, single-quantum-dot spectroscopy",

author = "Vonk, {Sander J.W.} and Heemskerk, {Bart A.J.} and Keitel, {Robert C.} and Hinterding, {Stijn O.M.} and Geuchies, {Jaco J.} and Houtepen, {Arjan J.} and Rabouw, {Freddy T.}",

note = "Funding Information: This work was supported by the Dutch Research Council NWO (OCENW.KLEIN.008). F.T.R. acknowledges financial support from The Netherlands Organisation for Scientific Research NWO (VENI grant number 722.017.002) and The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). J.J.G. and A.J.H. acknowledge support from European Research Council Horizon 2020 ERC Grant Agreement 678004 (Doping on Demand). R.C.K. acknowledges support from the European Research Council (ERC; FP/2007-2013), ERC Grant Agreement No. 339905 (QuaDoPS Advanced Grant). Peter Helfferich is thanked for technical support setting up the galvo-APD setup. Publisher Copyright: {\textcopyright} 2021 The Authors. Published by American Chemical Society",

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AU - Vonk, Sander J.W.

AU - Heemskerk, Bart A.J.

AU - Keitel, Robert C.

AU - Hinterding, Stijn O.M.

AU - Geuchies, Jaco J.

AU - Houtepen, Arjan J.

AU - Rabouw, Freddy T.

N1 - Funding Information: This work was supported by the Dutch Research Council NWO (OCENW.KLEIN.008). F.T.R. acknowledges financial support from The Netherlands Organisation for Scientific Research NWO (VENI grant number 722.017.002) and The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). J.J.G. and A.J.H. acknowledge support from European Research Council Horizon 2020 ERC Grant Agreement 678004 (Doping on Demand). R.C.K. acknowledges support from the European Research Council (ERC; FP/2007-2013), ERC Grant Agreement No. 339905 (QuaDoPS Advanced Grant). Peter Helfferich is thanked for technical support setting up the galvo-APD setup. Publisher Copyright: © 2021 The Authors. Published by American Chemical Society

PY - 2021/7/14

Y1 - 2021/7/14

N2 - Broadening of multiexciton emission from colloidal quantum dots (QDs) at room temperature is important for their use in high-power applications, but an in-depth characterization has not been possible until now. We present and apply a novel spectroscopic method to quantify the biexciton line width and biexciton binding energy of single CdSe/CdS/ZnS colloidal QDs at room temperature. In our method, which we term “cascade spectroscopy”, we select emission events from the biexciton cascade and reconstruct their spectrum. The biexciton has an average emission line width of 86 meV on the single-QD scale, similar to that of the exciton. Variations in the biexciton repulsion (Eb= 4.0 ± 3.1 meV; mean ± standard deviation of 15 QDs) are correlated with but are more narrowly distributed than variations in the exciton energy (10.0 meV standard deviation). Using a simple quantum-mechanical model, we conclude that inhomogeneous broadening in our sample is primarily due to variations in the CdS shell thickness.

AB - Broadening of multiexciton emission from colloidal quantum dots (QDs) at room temperature is important for their use in high-power applications, but an in-depth characterization has not been possible until now. We present and apply a novel spectroscopic method to quantify the biexciton line width and biexciton binding energy of single CdSe/CdS/ZnS colloidal QDs at room temperature. In our method, which we term “cascade spectroscopy”, we select emission events from the biexciton cascade and reconstruct their spectrum. The biexciton has an average emission line width of 86 meV on the single-QD scale, similar to that of the exciton. Variations in the biexciton repulsion (Eb= 4.0 ± 3.1 meV; mean ± standard deviation of 15 QDs) are correlated with but are more narrowly distributed than variations in the exciton energy (10.0 meV standard deviation). Using a simple quantum-mechanical model, we conclude that inhomogeneous broadening in our sample is primarily due to variations in the CdS shell thickness.

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KW - single-quantum-dot spectroscopy

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JF - Nano Letters

IS - 13

ER -

Biexciton Binding Energy and Line width of Single Quantum Dots at Room Temperature

Abstract

Bibliographical note

Funding

Keywords

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