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  Investigating the electronic structure of confined multiexcitons with nonlinear spectroscopies

Palato, S., Seiler, H., Baker, H., Sonnichsen, C., Brosseau, P., & Kambhampati, P. (2020). Investigating the electronic structure of confined multiexcitons with nonlinear spectroscopies. The Journal of Chemical Physics, 152(10): 104710. doi:10.1063/1.5142180.

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 Creators:
Palato, Samuel1, 2, Author           
Seiler, Helene1, 2, Author           
Baker, H.2, Author
Sonnichsen, C.2, Author
Brosseau, P.2, Author
Kambhampati, P.2, Author
Affiliations:
1Physical Chemistry, Fritz Haber Institute, Max Planck Society, ou_634546              
2Department of Chemistry, McGill University, 801 Sherbrooke Street W, Montréal, Québec H3A 0B8, Canada, ou_persistent22              

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 Abstract: Strong confinement in semiconductor quantum dots enables them to host multiple electron–hole pairs or excitons. The excitons in these materials are forced to interact, resulting in quantum-confined multiexcitons (MXs). The MXs are integral to the physics of the electronic properties of these materials and impact their key properties for applications such as gain and light emission. Despite their importance, the electronic structure of MX has yet to be fully characterized. MXs have a complex electronic structure arising from quantum many-body effects, which is challenging for both experiments and theory. Here, we report on the investigation of the electronic structure of MX in colloidal CdSe QDs using time-resolved photoluminescence, state-resolved pump–probe, and two-dimensional spectroscopies. The use of varying excitation energy and intensities enables the observation of many signals from biexcitons and triexcitons. The experiments enable the study of MX structures and dynamics on time scales spanning 6 orders of magnitude and directly reveal dynamics in the biexciton manifold. These results outline the limits of the simple concept of binding energy. The methods of investigations should be applicable to reveal complex many-body physics in other nanomaterials and low-dimensional materials of interest.

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Language(s): eng - English
 Dates: 2019-12-102020-02-202020-03-112020-03-14
 Publication Status: Published in print
 Pages: 21
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1063/1.5142180
 Degree: -

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Title: The Journal of Chemical Physics
  Other : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: 21 Volume / Issue: 152 (10) Sequence Number: 104710 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226