TY - JOUR

T1 - Non-Resonant Barrier Excitation in Conjugated Aromatic Ligand-Modified Perovskite Quantum Dots Enables a High Quantum Efficiency

AU - Yin, Hang

AU - Yang, Qing

AU - Bai, Tianxin

AU - Wang, Honglei

AU - Yang, Bin

AU - Wei, Qinhua

AU - Wu, Yingnan

AU - Zhang, Ruiling

AU - Qin, Laishun

AU - Chen, Junsheng

AU - Liu, Feng

AU - Liu, Jianyong

AU - Han, Keli

N1 - Funding Information: H.Y. and Q.Y. contributed equally to this work. This work was financially supported by the National Key R&D Program of China (No. 2022YFB3503600), National Natural Science Foundation of China (NSFC) (No. 12275262, 51972291), Natural Science Foundationof Zhejiang Province (No. LQ23A050004) and the China Association for Science and Technology Youth Talent Promotion Project (2022QNRC001‐No. YESS20220358), the Fundamental Research Funds for the Provincial Universities of Zhejiang (2023YW31). J.C. acknowledges support from the Novo Nordisk Foundation (NNF22OC0073582). The authors gratefully acknowledge HZWTECH for providing computation facilities. This paper is dedicated to Prof. Han on the first anniversary of his death. Publisher Copyright: © 2023 Wiley-VCH GmbH.

PY - 2024

Y1 - 2024

N2 - CsPbI3 quantum dots (QDs) hold tremendous promise for quantum emitters, but they undergo a considerable energy loss when excited above their optical bandgap, which impedes the utilization of high-energy photons. Different surface modification strategies have been proposed to improve the phase stability of CsPbI3 QDs, however, little progress has been made to realize high photoluminescence quantum yield (PLQY) with high-energy photon excitation. Here, a non-resonant barrier excitation (NRBE) mechanism in conjugated aromatic tetraphenylporphyrin (H2TPP)-modified CsPbI3 QDs is presented, which enables a high PLQY in the high-energy excitation regime as well as enhanced phase stability. Particularly, the proposed H2TPP ligand possesses adequate energy depth needed to realize NRBE in CsPbI3 QDs, which allows efficient charge injection from organic ligands to the inorganic core. As a result, the H2TPP-modified CsPbI3 QDs exhibit enhanced light absorption, large Stokes shift, and near-unity red emission when excited above the optical bandgap. The findings provide new insights into the ligand design strategies for improving optoelectronic properties.

AB - CsPbI3 quantum dots (QDs) hold tremendous promise for quantum emitters, but they undergo a considerable energy loss when excited above their optical bandgap, which impedes the utilization of high-energy photons. Different surface modification strategies have been proposed to improve the phase stability of CsPbI3 QDs, however, little progress has been made to realize high photoluminescence quantum yield (PLQY) with high-energy photon excitation. Here, a non-resonant barrier excitation (NRBE) mechanism in conjugated aromatic tetraphenylporphyrin (H2TPP)-modified CsPbI3 QDs is presented, which enables a high PLQY in the high-energy excitation regime as well as enhanced phase stability. Particularly, the proposed H2TPP ligand possesses adequate energy depth needed to realize NRBE in CsPbI3 QDs, which allows efficient charge injection from organic ligands to the inorganic core. As a result, the H2TPP-modified CsPbI3 QDs exhibit enhanced light absorption, large Stokes shift, and near-unity red emission when excited above the optical bandgap. The findings provide new insights into the ligand design strategies for improving optoelectronic properties.

KW - carrier dynamics

KW - conjugated aromatic ligand

KW - non-resonant barrier excitation

KW - perovskite quantum dots

KW - photoluminescence

U2 - 10.1002/lpor.202301051

DO - 10.1002/lpor.202301051

M3 - Journal article

AN - SCOPUS:85179667510

VL - 18

JO - Laser and Photonics Reviews

JF - Laser and Photonics Reviews

SN - 1863-8880

IS - 3

M1 - 2301051

ER -