Harvesting a Wide Spectral Range of Electronic Coherences with Disordered Quasi-Homo Dimeric Assemblies at Room Temperature
(2022) In Advanced Quantum Technologies 5(11).- Abstract
A wide variety of photoinduced electronic coherences are shown to be robust with respect to dephasing in ensembles of quasi-homodimers assembled with sub-nm ligands from colloidal 3 nm CdSe quantum dots (QDs) with controlled 9% size dispersion, both in solution and in solid-state. Coherence periods ranging from 40 to 300 fs are consistently characterized by multidimensional electronic spectroscopy in the Vis range in solution and solid-state samples. A theoretical model that includes size dispersion, spin orbit coupling, and crystal field splitting supports the assignment of electronic coherences. Further, this model provides a guide for optimizing the coherences by tuning the interplay between dimer electronic delocalization, optical... (More)
A wide variety of photoinduced electronic coherences are shown to be robust with respect to dephasing in ensembles of quasi-homodimers assembled with sub-nm ligands from colloidal 3 nm CdSe quantum dots (QDs) with controlled 9% size dispersion, both in solution and in solid-state. Coherence periods ranging from 40 to 300 fs are consistently characterized by multidimensional electronic spectroscopy in the Vis range in solution and solid-state samples. A theoretical model that includes size dispersion, spin orbit coupling, and crystal field splitting supports the assignment of electronic coherences. Further, this model provides a guide for optimizing the coherences by tuning the interplay between dimer electronic delocalization, optical activity, and size dispersion. The experimental persistence of many QD electronic coherences at the level of the size dispersed ensemble in the solid-state and in solution opens the way for building versatile bottom-up materials well suited to quantum technology applications.
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- author
- Hamilton, James R. ; Amarotti, Edoardo LU ; Dibenedetto, Carlo Nazareno ; Striccoli, Marinella ; Levine, R. D. ; Collini, Elisabetta and Remacle, F.
- publishing date
- 2022-11
- type
- Contribution to journal
- publication status
- published
- keywords
- 2D electronic spectroscopy, coherent coupling, multidimensional electronic spectroscopy, multilayered assemblies of CdSe quantum dots, quantum dot quasi-dimers, quantum dots for quantum information processing, size dispersion
- in
- Advanced Quantum Technologies
- volume
- 5
- issue
- 11
- article number
- 2200060
- publisher
- Wiley
- external identifiers
-
- scopus:85139237575
- ISSN
- 2511-9044
- DOI
- 10.1002/qute.202200060
- language
- English
- LU publication?
- no
- additional info
- Publisher Copyright: © 2022 Wiley-VCH GmbH.
- id
- 6cd33f38-b373-4713-b531-e4b39071c730
- date added to LUP
- 2023-03-29 10:14:06
- date last changed
- 2023-04-04 09:00:04
@article{6cd33f38-b373-4713-b531-e4b39071c730,
abstract = {{<p>A wide variety of photoinduced electronic coherences are shown to be robust with respect to dephasing in ensembles of quasi-homodimers assembled with sub-nm ligands from colloidal 3 nm CdSe quantum dots (QDs) with controlled 9% size dispersion, both in solution and in solid-state. Coherence periods ranging from 40 to 300 fs are consistently characterized by multidimensional electronic spectroscopy in the Vis range in solution and solid-state samples. A theoretical model that includes size dispersion, spin orbit coupling, and crystal field splitting supports the assignment of electronic coherences. Further, this model provides a guide for optimizing the coherences by tuning the interplay between dimer electronic delocalization, optical activity, and size dispersion. The experimental persistence of many QD electronic coherences at the level of the size dispersed ensemble in the solid-state and in solution opens the way for building versatile bottom-up materials well suited to quantum technology applications.</p>}},
author = {{Hamilton, James R. and Amarotti, Edoardo and Dibenedetto, Carlo Nazareno and Striccoli, Marinella and Levine, R. D. and Collini, Elisabetta and Remacle, F.}},
issn = {{2511-9044}},
keywords = {{2D electronic spectroscopy; coherent coupling; multidimensional electronic spectroscopy; multilayered assemblies of CdSe quantum dots; quantum dot quasi-dimers; quantum dots for quantum information processing; size dispersion}},
language = {{eng}},
number = {{11}},
publisher = {{Wiley}},
series = {{Advanced Quantum Technologies}},
title = {{Harvesting a Wide Spectral Range of Electronic Coherences with Disordered Quasi-Homo Dimeric Assemblies at Room Temperature}},
url = {{http://dx.doi.org/10.1002/qute.202200060}},
doi = {{10.1002/qute.202200060}},
volume = {{5}},
year = {{2022}},
}