Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties

Characterized by their strong 1D confinement and long-lifetime red-shifted emission spectra, colloidal nanoplatelets (NPLs) with type-II electronic structure provide an exciting ground to design complex heterostructures with remarkable properties. This work demonstrates the synthesis and optical cha...

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Main Authors: Shabani, Farzan, Martinez, Pedro Ludwig Hernandez, Shermet, Nina, Korkut, Hilal, Sarpkaya, Ibrahim, Baruj, Hamed Dehghanpour, Delikanli, Savas, Isik, Furkan, Durmusoglu, Emek Goksu, Demir, Hilmi Volkan
Other Authors: School of Electrical and Electronic Engineering
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Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/165211
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Institution: Nanyang Technological University
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spelling sg-ntu-dr.10356-1652112023-03-27T15:34:36Z Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties Shabani, Farzan Martinez, Pedro Ludwig Hernandez Shermet, Nina Korkut, Hilal Sarpkaya, Ibrahim Baruj, Hamed Dehghanpour Delikanli, Savas Isik, Furkan Durmusoglu, Emek Goksu Demir, Hilmi Volkan School of Electrical and Electronic Engineering School of Physical and Mathematical Sciences School of Materials Science and Engineering LUMINOUS! Centre of Excellence for Semiconductor Lighting & Displays Engineering::Materials::Nanostructured materials Colloidal Quantum Wells Semiconductor Nanoplatelets Characterized by their strong 1D confinement and long-lifetime red-shifted emission spectra, colloidal nanoplatelets (NPLs) with type-II electronic structure provide an exciting ground to design complex heterostructures with remarkable properties. This work demonstrates the synthesis and optical characterization of CdSe/CdSeTe/CdTe core/crown/crown NPLs having a step-wise gradient electronic structure and disproportional wavefunction distribution, in which the excitonic properties of the electron and hole can be finely tuned through adjusting the geometry of the intermediate crown. The first crown with staggered configuration gives rise to a series of direct and indirect transition channels that activation/deactivation of each channel is possible through wavefunction engineering. Moreover, these NPLs allow for switching between active channels with temperature, where lattice contraction directly affects the electron–hole (e–h) overlap. Dominated by the indirect transition channels over direct transitions, the lifetime of the NPLs starts to increase at 9 K, indicative of low dark-bright exciton splitting energy. The charge transfer states from the two type-II interfaces promote a large number of indirect transitions, which effectively increase the absorption of low-energy photons critical for nonlinear properties. As a result, these NPLs demonstrate exceptionally high two-photon absorption cross-sections with the highest value of 12.9 × 106 GM and superlinear behavior. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) Submitted/Accepted version The authors gratefully acknowledge the financial support from Agency for Science, Technology and Research (A*STAR) MTC program, Grant No. M21J9b0085 (Singapore), Ministry of Education Tier 1 grant MOE-RG62/20 (Singapore) and TUBITAK 115F297, 117E713, 119N343, 121N395, and 20AG001. H.V.D. also acknowledges the support from TUBA. 2023-03-27T02:07:35Z 2023-03-27T02:07:35Z 2023 Journal Article Shabani, F., Martinez, P. L. H., Shermet, N., Korkut, H., Sarpkaya, I., Baruj, H. D., Delikanli, S., Isik, F., Durmusoglu, E. G. & Demir, H. V. (2023). Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties. Small, 19(11), 2205729-. https://dx.doi.org/10.1002/smll.202205729 1613-6810 https://hdl.handle.net/10356/165211 10.1002/smll.202205729 2-s2.0-85146473706 11 19 2205729 en M21J9b0085 RG62/20 Small © 2023 Wiley-VCH GmbH. All rights reserved. This is the peer reviewed version of the following article: Shabani, F., Martinez, P. L. H., Shermet, N., Korkut, H., Sarpkaya, I., Baruj, H. D., Delikanli, S., Isik, F., Durmusoglu, E. G. & Demir, H. V. (2023). Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties. Small, 19(11), 2205729-, which has been published in final form at https://doi.org/10.1002/smll.202205729. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. 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
Colloidal Quantum Wells
Semiconductor Nanoplatelets
spellingShingle Engineering::Materials::Nanostructured materials
Colloidal Quantum Wells
Semiconductor Nanoplatelets
Shabani, Farzan
Martinez, Pedro Ludwig Hernandez
Shermet, Nina
Korkut, Hilal
Sarpkaya, Ibrahim
Baruj, Hamed Dehghanpour
Delikanli, Savas
Isik, Furkan
Durmusoglu, Emek Goksu
Demir, Hilmi Volkan
Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties
description Characterized by their strong 1D confinement and long-lifetime red-shifted emission spectra, colloidal nanoplatelets (NPLs) with type-II electronic structure provide an exciting ground to design complex heterostructures with remarkable properties. This work demonstrates the synthesis and optical characterization of CdSe/CdSeTe/CdTe core/crown/crown NPLs having a step-wise gradient electronic structure and disproportional wavefunction distribution, in which the excitonic properties of the electron and hole can be finely tuned through adjusting the geometry of the intermediate crown. The first crown with staggered configuration gives rise to a series of direct and indirect transition channels that activation/deactivation of each channel is possible through wavefunction engineering. Moreover, these NPLs allow for switching between active channels with temperature, where lattice contraction directly affects the electron–hole (e–h) overlap. Dominated by the indirect transition channels over direct transitions, the lifetime of the NPLs starts to increase at 9 K, indicative of low dark-bright exciton splitting energy. The charge transfer states from the two type-II interfaces promote a large number of indirect transitions, which effectively increase the absorption of low-energy photons critical for nonlinear properties. As a result, these NPLs demonstrate exceptionally high two-photon absorption cross-sections with the highest value of 12.9 × 106 GM and superlinear behavior.
author2 School of Electrical and Electronic Engineering
author_facet School of Electrical and Electronic Engineering
Shabani, Farzan
Martinez, Pedro Ludwig Hernandez
Shermet, Nina
Korkut, Hilal
Sarpkaya, Ibrahim
Baruj, Hamed Dehghanpour
Delikanli, Savas
Isik, Furkan
Durmusoglu, Emek Goksu
Demir, Hilmi Volkan
format Article
author Shabani, Farzan
Martinez, Pedro Ludwig Hernandez
Shermet, Nina
Korkut, Hilal
Sarpkaya, Ibrahim
Baruj, Hamed Dehghanpour
Delikanli, Savas
Isik, Furkan
Durmusoglu, Emek Goksu
Demir, Hilmi Volkan
author_sort Shabani, Farzan
title Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties
title_short Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties
title_full Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties
title_fullStr Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties
title_full_unstemmed Gradient type‐II CdSe/CdSeTe/CdTe core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties
title_sort gradient type‐ii cdse/cdsete/cdte core/crown/crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties
publishDate 2023
url https://hdl.handle.net/10356/165211
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