Photon correlations in colloidal quantum dot molecules controlled by the neck barrier

Somnath Koley; Jiabin Cui; Yossef E. Panfil; Yonatan Ossia; Adar Levi; Einav Scharf; Lior Verbitsky; Uri Banin

doi:10.1016/j.matt.2022.07.032

Photon correlations in colloidal quantum dot molecules controlled by the neck barrier

Somnath Koley, Jiabin Cui, Yossef E. Panfil, Yonatan Ossia, Adar Levi, Einav Scharf, Lior Verbitsky, Uri Banin^*

^*Corresponding author for this work

Institute of Chemistry

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

4 Scopus citations

Abstract

The charge redistribution upon optical excitation of various necked homodimer colloidal quantum dot molecules (CQDMs) is investigated using single-particle emission spectroscopy. By tuning the hybridization of the electron wavefunctions at a fixed center-to-center distance through controlling the neck girth, we reveal two coupling limits: on one hand, a “connected-but-confined” situation where neighboring CQDs are weakly fused to each other, manifesting a weak-coupling regime, and on the other hand, a “connected-and-delocalized” situation where the neck is filled beyond the facet size, leading to a rod-like architecture manifesting strong coupling. The interplay between the radiative and non-radiative Auger decays of these states turns emitted photons from the CQDMs in the weak-coupling regime highly bunched unlike CQD monomers, while the antibunching is regained at the strong-coupling regime. This work sets an analogy for the artificial molecule CQDMs with regular molecules, where the two distinct regimes of weak and strong coupling correspond to ionic- or covalent-type bonding, respectively.

Original language	American English
Pages (from-to)	3997-4014
Number of pages	18
Journal	Matter
Volume	5
Issue number	11
DOIs	https://doi.org/10.1016/j.matt.2022.07.032
State	Published - 2 Nov 2022

Bibliographical note

Funding Information:
The research leading to these results has received financial support from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. 741767, advanced investigator grant CoupledNC). S.K. and J.C. acknowledge support from the Planning and Budgeting Committee of the Council of Higher Education in Israel through a fellowship. Y.E.P. acknowledges support by the Ministry of Science and Technology and the National Foundation for Applied and Engineering Sciences, Israel. U.B. thanks the Alfred & Erica Larisch memorial chair. We thank Professor Eran Rabani for stimulating discussions. We thank Dr. Sergei Remmenik at the HUJI Nanocenter for assistance in structural characterization of the CQDMs. S.K. and U.B. conceived the idea. S.K. performed the optical experiment and analyzed and represented data with input from Y.O. and E.S. J.C. and A.L. synthesized and purified the CQDs and CQDMs, and S.K. took part in size-selective separation of dimers. S.K. U.B. and Y.E.P. interpreted the results to declutter the processes with input from all other authors. S.K. and U.B. co-wrote the manuscript with contribution from all authors. U.B. supervised the work. The authors declare no competing interests.

Funding Information:
The research leading to these results has received financial support from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. 741767 , advanced investigator grant CoupledNC). S.K. and J.C. acknowledge support from the Planning and Budgeting Committee of the Council of Higher Education in Israel through a fellowship. Y.E.P. acknowledges support by the Ministry of Science and Technology and the National Foundation for Applied and Engineering Sciences , Israel. U.B. thanks the Alfred & Erica Larisch memorial chair. We thank Professor Eran Rabani for stimulating discussions. We thank Dr. Sergei Remmenik at the HUJI Nanocenter for assistance in structural characterization of the CQDMs.

Publisher Copyright:
© 2022 Elsevier Inc.

Keywords

Auger process
MAP2: Benchmark
colloidal quantum dots
electronic coupling
photon antibunching
single-particle spectroscopy

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10.1016/j.matt.2022.07.032

Cite this

@article{e1d98c6be3164df69b3b954dca5e4aa6,

title = "Photon correlations in colloidal quantum dot molecules controlled by the neck barrier",

abstract = "The charge redistribution upon optical excitation of various necked homodimer colloidal quantum dot molecules (CQDMs) is investigated using single-particle emission spectroscopy. By tuning the hybridization of the electron wavefunctions at a fixed center-to-center distance through controlling the neck girth, we reveal two coupling limits: on one hand, a “connected-but-confined” situation where neighboring CQDs are weakly fused to each other, manifesting a weak-coupling regime, and on the other hand, a “connected-and-delocalized” situation where the neck is filled beyond the facet size, leading to a rod-like architecture manifesting strong coupling. The interplay between the radiative and non-radiative Auger decays of these states turns emitted photons from the CQDMs in the weak-coupling regime highly bunched unlike CQD monomers, while the antibunching is regained at the strong-coupling regime. This work sets an analogy for the artificial molecule CQDMs with regular molecules, where the two distinct regimes of weak and strong coupling correspond to ionic- or covalent-type bonding, respectively.",

keywords = "Auger process, MAP2: Benchmark, colloidal quantum dots, electronic coupling, photon antibunching, single-particle spectroscopy",

author = "Somnath Koley and Jiabin Cui and Panfil, {Yossef E.} and Yonatan Ossia and Adar Levi and Einav Scharf and Lior Verbitsky and Uri Banin",

note = "Funding Information: The research leading to these results has received financial support from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. 741767, advanced investigator grant CoupledNC). S.K. and J.C. acknowledge support from the Planning and Budgeting Committee of the Council of Higher Education in Israel through a fellowship. Y.E.P. acknowledges support by the Ministry of Science and Technology and the National Foundation for Applied and Engineering Sciences, Israel. U.B. thanks the Alfred & Erica Larisch memorial chair. We thank Professor Eran Rabani for stimulating discussions. We thank Dr. Sergei Remmenik at the HUJI Nanocenter for assistance in structural characterization of the CQDMs. S.K. and U.B. conceived the idea. S.K. performed the optical experiment and analyzed and represented data with input from Y.O. and E.S. J.C. and A.L. synthesized and purified the CQDs and CQDMs, and S.K. took part in size-selective separation of dimers. S.K. U.B. and Y.E.P. interpreted the results to declutter the processes with input from all other authors. S.K. and U.B. co-wrote the manuscript with contribution from all authors. U.B. supervised the work. The authors declare no competing interests. Funding Information: The research leading to these results has received financial support from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. 741767 , advanced investigator grant CoupledNC). S.K. and J.C. acknowledge support from the Planning and Budgeting Committee of the Council of Higher Education in Israel through a fellowship. Y.E.P. acknowledges support by the Ministry of Science and Technology and the National Foundation for Applied and Engineering Sciences , Israel. U.B. thanks the Alfred & Erica Larisch memorial chair. We thank Professor Eran Rabani for stimulating discussions. We thank Dr. Sergei Remmenik at the HUJI Nanocenter for assistance in structural characterization of the CQDMs. Publisher Copyright: {\textcopyright} 2022 Elsevier Inc.",

year = "2022",

month = nov,

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doi = "10.1016/j.matt.2022.07.032",

language = "American English",

volume = "5",

pages = "3997--4014",

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T1 - Photon correlations in colloidal quantum dot molecules controlled by the neck barrier

AU - Koley, Somnath

AU - Cui, Jiabin

AU - Panfil, Yossef E.

AU - Ossia, Yonatan

AU - Levi, Adar

AU - Scharf, Einav

AU - Verbitsky, Lior

AU - Banin, Uri

N1 - Funding Information: The research leading to these results has received financial support from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. 741767, advanced investigator grant CoupledNC). S.K. and J.C. acknowledge support from the Planning and Budgeting Committee of the Council of Higher Education in Israel through a fellowship. Y.E.P. acknowledges support by the Ministry of Science and Technology and the National Foundation for Applied and Engineering Sciences, Israel. U.B. thanks the Alfred & Erica Larisch memorial chair. We thank Professor Eran Rabani for stimulating discussions. We thank Dr. Sergei Remmenik at the HUJI Nanocenter for assistance in structural characterization of the CQDMs. S.K. and U.B. conceived the idea. S.K. performed the optical experiment and analyzed and represented data with input from Y.O. and E.S. J.C. and A.L. synthesized and purified the CQDs and CQDMs, and S.K. took part in size-selective separation of dimers. S.K. U.B. and Y.E.P. interpreted the results to declutter the processes with input from all other authors. S.K. and U.B. co-wrote the manuscript with contribution from all authors. U.B. supervised the work. The authors declare no competing interests. Funding Information: The research leading to these results has received financial support from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. 741767 , advanced investigator grant CoupledNC). S.K. and J.C. acknowledge support from the Planning and Budgeting Committee of the Council of Higher Education in Israel through a fellowship. Y.E.P. acknowledges support by the Ministry of Science and Technology and the National Foundation for Applied and Engineering Sciences , Israel. U.B. thanks the Alfred & Erica Larisch memorial chair. We thank Professor Eran Rabani for stimulating discussions. We thank Dr. Sergei Remmenik at the HUJI Nanocenter for assistance in structural characterization of the CQDMs. Publisher Copyright: © 2022 Elsevier Inc.

PY - 2022/11/2

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N2 - The charge redistribution upon optical excitation of various necked homodimer colloidal quantum dot molecules (CQDMs) is investigated using single-particle emission spectroscopy. By tuning the hybridization of the electron wavefunctions at a fixed center-to-center distance through controlling the neck girth, we reveal two coupling limits: on one hand, a “connected-but-confined” situation where neighboring CQDs are weakly fused to each other, manifesting a weak-coupling regime, and on the other hand, a “connected-and-delocalized” situation where the neck is filled beyond the facet size, leading to a rod-like architecture manifesting strong coupling. The interplay between the radiative and non-radiative Auger decays of these states turns emitted photons from the CQDMs in the weak-coupling regime highly bunched unlike CQD monomers, while the antibunching is regained at the strong-coupling regime. This work sets an analogy for the artificial molecule CQDMs with regular molecules, where the two distinct regimes of weak and strong coupling correspond to ionic- or covalent-type bonding, respectively.

AB - The charge redistribution upon optical excitation of various necked homodimer colloidal quantum dot molecules (CQDMs) is investigated using single-particle emission spectroscopy. By tuning the hybridization of the electron wavefunctions at a fixed center-to-center distance through controlling the neck girth, we reveal two coupling limits: on one hand, a “connected-but-confined” situation where neighboring CQDs are weakly fused to each other, manifesting a weak-coupling regime, and on the other hand, a “connected-and-delocalized” situation where the neck is filled beyond the facet size, leading to a rod-like architecture manifesting strong coupling. The interplay between the radiative and non-radiative Auger decays of these states turns emitted photons from the CQDMs in the weak-coupling regime highly bunched unlike CQD monomers, while the antibunching is regained at the strong-coupling regime. This work sets an analogy for the artificial molecule CQDMs with regular molecules, where the two distinct regimes of weak and strong coupling correspond to ionic- or covalent-type bonding, respectively.

KW - Auger process

KW - MAP2: Benchmark

KW - colloidal quantum dots

KW - electronic coupling

KW - photon antibunching

KW - single-particle spectroscopy

UR - http://www.scopus.com/inward/record.url?scp=85140921250&partnerID=8YFLogxK

U2 - 10.1016/j.matt.2022.07.032

DO - 10.1016/j.matt.2022.07.032

M3 - Article

AN - SCOPUS:85140921250

SN - 2590-2393

VL - 5

SP - 3997

EP - 4014

JO - Matter

JF - Matter

IS - 11

ER -

Photon correlations in colloidal quantum dot molecules controlled by the neck barrier

Abstract

Bibliographical note

Keywords

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