Fate of Optical Excitons in FAPbI3 Nanocube Superlattices
Milloch, Alessandra ; Filippi, Umberto ; Franceschini, Paolo ; Mor, Selene ; Pagliara, Stefania ; Ferrini, Gabriele ; Camargo, Franco V. A. ; Cerullo, Giulio ; Baranov, Dmitry LU
and Manna, Liberato
, et al.
(2024)
In ACS Photonics
11(9).
p.3511-3520
- Abstract
Understanding the nature of the photoexcitation and ultrafast charge dynamics pathways in organic halide perovskite nanocubes and their aggregation into superlattices is key for potential applications as tunable light emitters, photon-harvesting materials, and light-amplification systems. In this work, we apply two-dimensional coherent electronic spectroscopy (2DES) to track in real time the formation of near-infrared optical excitons and their ultrafast relaxation in CH(NH2)2PbI3 nanocube superlattices. Our results unveil that the coherent ultrafast dynamics is limited by the combination of the inherent short exciton decay time (≃40 fs) and the dephasing due to the coupling with selective optical phonon... (More)
Understanding the nature of the photoexcitation and ultrafast charge dynamics pathways in organic halide perovskite nanocubes and their aggregation into superlattices is key for potential applications as tunable light emitters, photon-harvesting materials, and light-amplification systems. In this work, we apply two-dimensional coherent electronic spectroscopy (2DES) to track in real time the formation of near-infrared optical excitons and their ultrafast relaxation in CH(NH2)2PbI3 nanocube superlattices. Our results unveil that the coherent ultrafast dynamics is limited by the combination of the inherent short exciton decay time (≃40 fs) and the dephasing due to the coupling with selective optical phonon modes at higher temperatures. On the picosecond time scale, we observe the progressive formation of long-lived localized trap states. The analysis of the temperature dependence of the excitonic intrinsic line width, as extracted by the antidiagonal components of the 2D spectra, unveils a dramatic change of the excitonic coherence time across the cubic to tetragonal structural transition. Our results offer a new way to control and enhance the ultrafast coherent dynamics of photocarrier generation in hybrid halide perovskite synthetic solids.
(Less)
- author
- Milloch, Alessandra
; Filippi, Umberto
; Franceschini, Paolo
; Mor, Selene
; Pagliara, Stefania
; Ferrini, Gabriele
; Camargo, Franco V. A.
; Cerullo, Giulio
; Baranov, Dmitry
LU
and Manna, Liberato
, et al. (More)
- Milloch, Alessandra
; Filippi, Umberto
; Franceschini, Paolo
; Mor, Selene
; Pagliara, Stefania
; Ferrini, Gabriele
; Camargo, Franco V. A.
; Cerullo, Giulio
; Baranov, Dmitry
LU
; Manna, Liberato
and Giannetti, Claudio
(Less)
- organization
- publishing date
- 2024-09-18
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- 2D spectroscopy, hybrid halide perovskites, multiexciton dynamics, nanocube superlattices, trap states
- in
- ACS Photonics
- volume
- 11
- issue
- 9
- pages
- 10 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- scopus:85203170767
- pmid:39310294
- ISSN
- 2330-4022
- DOI
- 10.1021/acsphotonics.4c00105
- language
- English
- LU publication?
- yes
- additional info
- Publisher Copyright: © 2024 The Authors. Published by American Chemical Society.
- id
- 17e9628d-75e2-4e9f-be76-8e90bbc33cc3
- date added to LUP
- 2024-11-17 10:40:38
- date last changed
- 2025-07-14 06:06:33
@article{17e9628d-75e2-4e9f-be76-8e90bbc33cc3,
abstract = {{<p>Understanding the nature of the photoexcitation and ultrafast charge dynamics pathways in organic halide perovskite nanocubes and their aggregation into superlattices is key for potential applications as tunable light emitters, photon-harvesting materials, and light-amplification systems. In this work, we apply two-dimensional coherent electronic spectroscopy (2DES) to track in real time the formation of near-infrared optical excitons and their ultrafast relaxation in CH(NH<sub>2</sub>)<sub>2</sub>PbI<sub>3</sub> nanocube superlattices. Our results unveil that the coherent ultrafast dynamics is limited by the combination of the inherent short exciton decay time (≃40 fs) and the dephasing due to the coupling with selective optical phonon modes at higher temperatures. On the picosecond time scale, we observe the progressive formation of long-lived localized trap states. The analysis of the temperature dependence of the excitonic intrinsic line width, as extracted by the antidiagonal components of the 2D spectra, unveils a dramatic change of the excitonic coherence time across the cubic to tetragonal structural transition. Our results offer a new way to control and enhance the ultrafast coherent dynamics of photocarrier generation in hybrid halide perovskite synthetic solids.</p>}},
author = {{Milloch, Alessandra and Filippi, Umberto and Franceschini, Paolo and Mor, Selene and Pagliara, Stefania and Ferrini, Gabriele and Camargo, Franco V. A. and Cerullo, Giulio and Baranov, Dmitry and Manna, Liberato and Giannetti, Claudio}},
issn = {{2330-4022}},
keywords = {{2D spectroscopy; hybrid halide perovskites; multiexciton dynamics; nanocube superlattices; trap states}},
language = {{eng}},
month = {{09}},
number = {{9}},
pages = {{3511--3520}},
publisher = {{The American Chemical Society (ACS)}},
series = {{ACS Photonics}},
title = {{Fate of Optical Excitons in FAPbI<sub>3</sub> Nanocube Superlattices}},
url = {{http://dx.doi.org/10.1021/acsphotonics.4c00105}},
doi = {{10.1021/acsphotonics.4c00105}},
volume = {{11}},
year = {{2024}},
}