Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy

We measure the ultrafast spectral diffusion, vibronic dynamics, and energy relaxation of a CdSe colloidal quantum wells (CQWs) system at room temperature using two-dimensional electronic spectroscopy (2DES). The energy relaxation of light-hole (LH) excitons and hot carriers to heavy-hole (HH) excito...

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Main Authors: Nguyen, Hoang Long, Do, Thanh Nhut, Durmusoglu, Emek Goksu, Izmir, Merve, Sarkar, Ritabrata, Pal, Sougata, Prezhdo, Oleg V., Demir, Hilmi Volkan, Tan, Howe-Siang
Other Authors: School of Electrical and Electronic Engineering
Format: Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/165260
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Institution: Nanyang Technological University
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spelling sg-ntu-dr.10356-1652602023-06-21T08:01:54Z Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy Nguyen, Hoang Long Do, Thanh Nhut Durmusoglu, Emek Goksu Izmir, Merve Sarkar, Ritabrata Pal, Sougata Prezhdo, Oleg V. Demir, Hilmi Volkan Tan, Howe-Siang School of Electrical and Electronic Engineering School of Physical and Mathematical Sciences School of Materials Science and Engineering School of Chemistry, Chemical Engineering and Biotechnology LUMINOUS! Centre of Excellence for Semiconductor Lighting & Displays The Photonics Institute Engineering::Materials::Nanostructured materials Spectral Diffusion Colloidal Quantum Well We measure the ultrafast spectral diffusion, vibronic dynamics, and energy relaxation of a CdSe colloidal quantum wells (CQWs) system at room temperature using two-dimensional electronic spectroscopy (2DES). The energy relaxation of light-hole (LH) excitons and hot carriers to heavy-hole (HH) excitons is resolved with a time scale of ∼210 fs. We observe the equilibration dynamics between the spectroscopically accessible HH excitonic state and a dark state with a time scale of ∼160 fs. We use the center line slope analysis to quantify the spectral diffusion dynamics in HH excitons, which contains an apparent sub-200 fs decay together with oscillatory features resolved at 4 and 25 meV. These observations can be explained by the coupling to various lattice phonon modes. We further perform quantum calculations that can replicate and explain the observed dynamics. The 4 meV mode is observed to be in the near-critically damped regime and may be mediating the transition between the bright and dark HH excitons. These findings show that 2DES can provide a comprehensive and detailed characterization of the ultrafast spectral properties in CQWs and similar nanomaterials. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) Submitted/Accepted version H.V.D. gratefully acknowledges the financial support in part from the Singapore Agency for Science, Technology and Research (A*STAR) SERC under Grant No. M21J9b0085, and the Singapore Ministry of Education Tier 1 grant (MOERG62/20). H.V.D. also gratefully acknowledges the support from TUBA. H.-S.T. gratefully acknowledges the financial support in part from the Singapore Ministry of Education Tier 1 grant (MOE-RG2/19 and MOE-RG14/20). O.V.P. acknowledges the financial support from the United States National Science Foundation under Grant No. CHE-2154367. 2023-03-27T03:10:47Z 2023-03-27T03:10:47Z 2023 Journal Article Nguyen, H. L., Do, T. N., Durmusoglu, E. G., Izmir, M., Sarkar, R., Pal, S., Prezhdo, O. V., Demir, H. V. & Tan, H. (2023). Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy. ACS Nano, 17(3), 2411-2420. https://dx.doi.org/10.1021/acsnano.2c09606 1936-0851 https://hdl.handle.net/10356/165260 10.1021/acsnano.2c09606 17 2-s2.0-85148114293 3 17 2411 2420 en M21J9b0085 MOE-RG62/20 MOE-RG2/19 MOE-RG14/20 ACS Nano This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, copyright © 2023 American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsnano.2c09606. application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Materials::Nanostructured materials
Spectral Diffusion
Colloidal Quantum Well
spellingShingle Engineering::Materials::Nanostructured materials
Spectral Diffusion
Colloidal Quantum Well
Nguyen, Hoang Long
Do, Thanh Nhut
Durmusoglu, Emek Goksu
Izmir, Merve
Sarkar, Ritabrata
Pal, Sougata
Prezhdo, Oleg V.
Demir, Hilmi Volkan
Tan, Howe-Siang
Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy
description We measure the ultrafast spectral diffusion, vibronic dynamics, and energy relaxation of a CdSe colloidal quantum wells (CQWs) system at room temperature using two-dimensional electronic spectroscopy (2DES). The energy relaxation of light-hole (LH) excitons and hot carriers to heavy-hole (HH) excitons is resolved with a time scale of ∼210 fs. We observe the equilibration dynamics between the spectroscopically accessible HH excitonic state and a dark state with a time scale of ∼160 fs. We use the center line slope analysis to quantify the spectral diffusion dynamics in HH excitons, which contains an apparent sub-200 fs decay together with oscillatory features resolved at 4 and 25 meV. These observations can be explained by the coupling to various lattice phonon modes. We further perform quantum calculations that can replicate and explain the observed dynamics. The 4 meV mode is observed to be in the near-critically damped regime and may be mediating the transition between the bright and dark HH excitons. These findings show that 2DES can provide a comprehensive and detailed characterization of the ultrafast spectral properties in CQWs and similar nanomaterials.
author2 School of Electrical and Electronic Engineering
author_facet School of Electrical and Electronic Engineering
Nguyen, Hoang Long
Do, Thanh Nhut
Durmusoglu, Emek Goksu
Izmir, Merve
Sarkar, Ritabrata
Pal, Sougata
Prezhdo, Oleg V.
Demir, Hilmi Volkan
Tan, Howe-Siang
format Article
author Nguyen, Hoang Long
Do, Thanh Nhut
Durmusoglu, Emek Goksu
Izmir, Merve
Sarkar, Ritabrata
Pal, Sougata
Prezhdo, Oleg V.
Demir, Hilmi Volkan
Tan, Howe-Siang
author_sort Nguyen, Hoang Long
title Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy
title_short Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy
title_full Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy
title_fullStr Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy
title_full_unstemmed Measuring the ultrafast spectral diffusion and vibronic coupling dynamics in CdSe colloidal quantum wells using two-dimensional electronic spectroscopy
title_sort measuring the ultrafast spectral diffusion and vibronic coupling dynamics in cdse colloidal quantum wells using two-dimensional electronic spectroscopy
publishDate 2023
url https://hdl.handle.net/10356/165260
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