TY - JOUR
T1 - Efficient generation of emissive many-body correlations in copper-doped colloidal quantum wells
AU - Yu, Junhong
AU - Sharma, Manoj
AU - Li, Mingjie
AU - Liu, Baiquan
AU - Hernández-Martínez, Pedro Ludwig
AU - Delikanli, Savas
AU - Sharma, Ashma
AU - Altintas, Yemliha
AU - Hettiarachchi, Chathuranga
AU - Sum, Tze Chien
AU - Demir, Hilmi Volkan
AU - Dang, Cuong
N1 - Funding Information:
C.D. is grateful for the financial support from the Ministry of Education, Singapore, under its AcRF Tier 2 grant (MOE-T2EP50121-0012). H.V.D. acknowledges the financial support in part from the Singapore Agency for Science, Technology and Research (A∗STAR) MTC program under grant no. M21J9b0085, the Ministry of Education, Singapore, under its Academic Research Fund Tier 1 (MOE-RG62/20), and in part from TUBITAK 119N343, 20AG001, 121N395, and 121C266. H.V.D. also acknowledges support from TUBA and TUBITAK 2247-A National Leader Researchers Program (121C266). M.S. also acknowledges the funding through the Australian Research Council Center of Excellence in Exciton Science (grant no. CE170100026). We would like to thank Muhammad Taimoor and Thomas Kusserow at the University of Kassel (Kassel, Germany) for carefully reading our manuscript. C.D. and H.V.D. supervised and contributed to all aspects of the research. J.Y. M.S. H.V.D. and C.D. wrote the manuscript. J.Y. conducted the spectroscopy measurements and initiated the study. M.S. performed the material syntheses and designed them to achieve the best performance. S.D. and A.S. helped in material synthesis and characterizations. M.L. performed trPL and transient absorption measurements. M.L. and T.C.S. supervised the ultrafast dynamic analysis. P.L.H.-M. helped to explain the experimental observations. Y.A. conducted the ICP-MS and XPS measurements. B.L. provided fruitful discussions about many-body physics. All authors analyzed the data, discussed the results, commented on the manuscript, and participated in manuscript revision. The authors declare no competing interests.
Funding Information:
C.D. is grateful for the financial support from the Ministry of Education, Singapore , under its AcRF Tier 2 grant ( MOE-T2EP50121-0012 ). H.V.D. acknowledges the financial support in part from the Singapore Agency for Science, Technology and Research (A∗STAR) MTC program under grant no. M21J9b0085 , the Ministry of Education, Singapore, under its Academic Research Fund Tier 1 ( MOE-RG62/20 ), and in part from TUBITAK 119N343 , 20AG001 , 121N395 , and 121C266 . H.V.D. also acknowledges support from TUBA and TUBITAK 2247-A National Leader Researchers Program ( 121C266 ). M.S. also acknowledges the funding through the Australian Research Council Center of Excellence in Exciton Science (grant no. CE170100026 ). We would like to thank Muhammad Taimoor and Thomas Kusserow at the University of Kassel (Kassel, Germany) for carefully reading our manuscript.
Publisher Copyright:
© 2022 The Authors
PY - 2022/9/21
Y1 - 2022/9/21
N2 - Colloidal quantum wells (CQWs) provide an appealing platform to achieve emissive many-body correlations for novel optoelectronic devices, given that they act as hosts for strong carrier Coulomb interactions and present suppressed Auger recombination. However, the demonstrated high-order excitonic emission in CQWs requires ultrafast pumping with high excitation levels and can only be spectrally resolved at the single-particle level under cryogenic conditions. Here, through systematic investigation using static power-dependent emission spectroscopy and transient carrier dynamics, we show that Cu-doped CdSe CQWs exhibit continuous-wave-pumped high-order excitonic emission at room temperature with a large binding energy of ∼64 meV. We attribute this unique behavior to dopant excitons in which the ultralong lifetime and the highly localized wavefunction facilitate the formation of many-body correlations. The spectrally resolved high-order excitonic emission generated at power levels compatible with solar irradiation and electrical injection might pave the way for novel solution-processed solid-state devices.
AB - Colloidal quantum wells (CQWs) provide an appealing platform to achieve emissive many-body correlations for novel optoelectronic devices, given that they act as hosts for strong carrier Coulomb interactions and present suppressed Auger recombination. However, the demonstrated high-order excitonic emission in CQWs requires ultrafast pumping with high excitation levels and can only be spectrally resolved at the single-particle level under cryogenic conditions. Here, through systematic investigation using static power-dependent emission spectroscopy and transient carrier dynamics, we show that Cu-doped CdSe CQWs exhibit continuous-wave-pumped high-order excitonic emission at room temperature with a large binding energy of ∼64 meV. We attribute this unique behavior to dopant excitons in which the ultralong lifetime and the highly localized wavefunction facilitate the formation of many-body correlations. The spectrally resolved high-order excitonic emission generated at power levels compatible with solar irradiation and electrical injection might pave the way for novel solution-processed solid-state devices.
KW - colloidal nanocrystals
KW - colloidal quantum wells
KW - copper doping
KW - high-order excitonic states
KW - ultrafast spectroscopy
UR - https://www.scopus.com/pages/publications/85138207712
U2 - 10.1016/j.xcrp.2022.101049
DO - 10.1016/j.xcrp.2022.101049
M3 - Journal article
AN - SCOPUS:85138207712
SN - 2666-3864
VL - 3
JO - Cell Reports Physical Science
JF - Cell Reports Physical Science
IS - 9
M1 - 101049
ER -