Enhancing Charge Carrier Delocalization in Perovskite Quantum Dot Solids with Energetically Aligned Conjugated Capping Ligands

Evan T. Vickers; Emily E. Enlow; William G. Delmas; Albert C. Dibenedetto; Ashraful H. Chowdhury; Behzad Bahrami; Benjamin W. Dreskin; Thomas A. Graham; Isaak N. Hernandez; Sue A. Carter; Sayantani Ghosh; Qiquan Qiao; Jin Z. Zhang

doi:10.1021/acsenergylett.0c00093

Enhancing Charge Carrier Delocalization in Perovskite Quantum Dot Solids with Energetically Aligned Conjugated Capping Ligands

Evan T. Vickers, Emily E. Enlow, William G. Delmas, Albert C. Dibenedetto, Ashraful H. Chowdhury, Behzad Bahrami, Benjamin W. Dreskin, Thomas A. Graham, Isaak N. Hernandez, Sue A. Carter, Sayantani Ghosh, Qiquan Qiao, Jin Z. Zhang

Research output: Contribution to journal › Article › peer-review

65 Scopus citations

Abstract

Compared to bulk perovskites, charge transport in perovskite quantum dot (PQD) solids is limited. To address this issue, energetically aligned capping ligands were used to prepare methylammonium lead bromide (MAPbBr₃) PQDs toward enhancing surface charge carrier density in PQD solids. Trans-cinnamic acid (TCA) and its derivates, functionalized with electron-donating or electron-withdrawing groups to modulate energy levels, are used as passivating exciton-delocalizing ligands (EDLs) to decrease the energy gap with respect to the PQD core. 3,3-Diphenylpropylamine (DPPA) ligand is shown to stabilize EDLs on the PQD surface through π-πstacking intermolecular interaction, mitigating charge trapping and nonradiative decay. Passivation using EDLs in combination with DPPA increases the photoluminescence (PL) quantum yield (QY) (90%), photoconductivity, extraction, mobility, transport time, and lifetime of charge carriers in PQD solids. Prototype PQD-based light-emitting diodes (LEDs) were demonstrated with a low turn-on voltage of 2.5 V.

Original language	English (US)
Pages (from-to)	817-825
Number of pages	9
Journal	ACS Energy Letters
Volume	5
Issue number	3
DOIs	https://doi.org/10.1021/acsenergylett.0c00093
State	Published - Mar 13 2020
Externally published	Yes

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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10.1021/acsenergylett.0c00093

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Vickers, E. T., Enlow, E. E., Delmas, W. G., Dibenedetto, A. C., Chowdhury, A. H., Bahrami, B., Dreskin, B. W., Graham, T. A., Hernandez, I. N., Carter, S. A., Ghosh, S., Qiao, Q., & Zhang, J. Z. (2020). Enhancing Charge Carrier Delocalization in Perovskite Quantum Dot Solids with Energetically Aligned Conjugated Capping Ligands. ACS Energy Letters, 5(3), 817-825. https://doi.org/10.1021/acsenergylett.0c00093

Vickers, ET, Enlow, EE, Delmas, WG, Dibenedetto, AC, Chowdhury, AH, Bahrami, B, Dreskin, BW, Graham, TA, Hernandez, IN, Carter, SA, Ghosh, S, Qiao, Q & Zhang, JZ 2020, 'Enhancing Charge Carrier Delocalization in Perovskite Quantum Dot Solids with Energetically Aligned Conjugated Capping Ligands', ACS Energy Letters, vol. 5, no. 3, pp. 817-825. https://doi.org/10.1021/acsenergylett.0c00093

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abstract = "Compared to bulk perovskites, charge transport in perovskite quantum dot (PQD) solids is limited. To address this issue, energetically aligned capping ligands were used to prepare methylammonium lead bromide (MAPbBr3) PQDs toward enhancing surface charge carrier density in PQD solids. Trans-cinnamic acid (TCA) and its derivates, functionalized with electron-donating or electron-withdrawing groups to modulate energy levels, are used as passivating exciton-delocalizing ligands (EDLs) to decrease the energy gap with respect to the PQD core. 3,3-Diphenylpropylamine (DPPA) ligand is shown to stabilize EDLs on the PQD surface through π-πstacking intermolecular interaction, mitigating charge trapping and nonradiative decay. Passivation using EDLs in combination with DPPA increases the photoluminescence (PL) quantum yield (QY) (90%), photoconductivity, extraction, mobility, transport time, and lifetime of charge carriers in PQD solids. Prototype PQD-based light-emitting diodes (LEDs) were demonstrated with a low turn-on voltage of 2.5 V.",

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N2 - Compared to bulk perovskites, charge transport in perovskite quantum dot (PQD) solids is limited. To address this issue, energetically aligned capping ligands were used to prepare methylammonium lead bromide (MAPbBr3) PQDs toward enhancing surface charge carrier density in PQD solids. Trans-cinnamic acid (TCA) and its derivates, functionalized with electron-donating or electron-withdrawing groups to modulate energy levels, are used as passivating exciton-delocalizing ligands (EDLs) to decrease the energy gap with respect to the PQD core. 3,3-Diphenylpropylamine (DPPA) ligand is shown to stabilize EDLs on the PQD surface through π-πstacking intermolecular interaction, mitigating charge trapping and nonradiative decay. Passivation using EDLs in combination with DPPA increases the photoluminescence (PL) quantum yield (QY) (90%), photoconductivity, extraction, mobility, transport time, and lifetime of charge carriers in PQD solids. Prototype PQD-based light-emitting diodes (LEDs) were demonstrated with a low turn-on voltage of 2.5 V.

AB - Compared to bulk perovskites, charge transport in perovskite quantum dot (PQD) solids is limited. To address this issue, energetically aligned capping ligands were used to prepare methylammonium lead bromide (MAPbBr3) PQDs toward enhancing surface charge carrier density in PQD solids. Trans-cinnamic acid (TCA) and its derivates, functionalized with electron-donating or electron-withdrawing groups to modulate energy levels, are used as passivating exciton-delocalizing ligands (EDLs) to decrease the energy gap with respect to the PQD core. 3,3-Diphenylpropylamine (DPPA) ligand is shown to stabilize EDLs on the PQD surface through π-πstacking intermolecular interaction, mitigating charge trapping and nonradiative decay. Passivation using EDLs in combination with DPPA increases the photoluminescence (PL) quantum yield (QY) (90%), photoconductivity, extraction, mobility, transport time, and lifetime of charge carriers in PQD solids. Prototype PQD-based light-emitting diodes (LEDs) were demonstrated with a low turn-on voltage of 2.5 V.

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Enhancing Charge Carrier Delocalization in Perovskite Quantum Dot Solids with Energetically Aligned Conjugated Capping Ligands

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