Holistic energy landscape management in 2D/3D heterojunction via molecular engineering for efficient perovskite solar cells

Ke Ma; Jiaonan Sun; Harindi R. Atapattu; Bryon W. Larson; Hanjun Yang; Dewei Sun; Ke Chen; Kang Wang; Yoonho Lee; Yuanhao Tang; Anika Bhoopalam; Libai Huang; Kenneth R. Graham; Jianguo Mei; Letian Dou

doi:10.1126/sciadv.adg0032

Holistic energy landscape management in 2D/3D heterojunction via molecular engineering for efficient perovskite solar cells

Ke Ma, Jiaonan Sun, Harindi R. Atapattu, Bryon W. Larson, Hanjun Yang, Dewei Sun, Ke Chen, Kang Wang, Yoonho Lee, Yuanhao Tang, Anika Bhoopalam, Libai Huang, Kenneth R. Graham, Jianguo Mei, Letian Dou

Chemistry

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

Abstract

Constructing two-dimensional (2D) perovskite atop of 3D with energy landscape management is still a challenge in perovskite photovoltaics. Here, we report a strategy through designing a series of π-conjugated organic cations to construct stable 2D perovskites and to realize delicate energy level tunability at 2D/3D heterojunctions. As a result, the hole transfer energy barriers can be reduced both at heterojunctions and within 2D structures, and the preferable work function shift reduces charge accumulation at interface. Leveraging these insights and also benefitted from the superior interface contact between conjugated cations and poly(triarylamine) (PTAA) hole transporting layer, a solar cell with power conversion efficiency of 24.6% has been achieved, which is the highest among PTAA-based n-i-p devices to the best of our knowledge. The devices exhibit greatly enhanced stability and reproducibility. This approach is generic to several hole transporting materials, offering opportunities to realize high efficiency without using the unstable Spiro-OMeTAD.

Original language	English
Article number	eadg0032
Journal	Science advances
Volume	9
Issue number	23
DOIs	https://doi.org/10.1126/sciadv.adg0032
State	Published - Jun 2023

Bibliographical note

Funding Information:
Acknowledgments:W ethankK.ZhuforexperimentalhelpandM.Zellerforsingle-crystal analysis.W ealsothankT .T erlier forTOF-SIMScharacterization.Funding:Thismaterialisbased on work supported by the U.S. Department of Energy’s Office of Energy Efficiency and RenewableEnergy(EERE)underSolarEnergyT echnologies OfficeA wardDE-EE0009519.K.M. acknowledgesthefinancialsupportfromLillianGilbrethPostdoctoralFellowships.H.R.A.and K.R.G.acknowledgefundingfromtheOfficeofScienceoftheU.S.DepartmentofEnergyfor supportingtheUPSandXPSmeasurementsunderawardnumberDE-SC0018208.D.S.andL.H. acknowledgefundingfromtheOfficeofScienceoftheU.S.DepartmentofEnergyfor supportingthetime-resolvedT AandPLmeasurementsunderawardnumberDE-SC0022082. TheworkwaspartiallysupportedbytheU.S.DepartmentofEnergyundercontractnumberDE-A C36-08GO28308 withAllianceforSustainableEnergy,LimitedLiabilityCompany(LLC),the ManagerandOperatoroftheNationalRenewableEnergyLaboratory.TRMCmeasurementsand opticalcharacterizationsweresupportedbytheDe-RiskingHalidePero vskite SolarCells programoftheNationalCenterforPhotovoltaicsfromDE-FO A-0002064 andDE-EE0008790, fundedbytheU.S.DepartmentofEnergy,OfficeofEnergyEfficiencyandRenewableEnergy, SolarEnergyT echnologies Office.Theviewsexpressedinthearticledonotnecessarily represent the views of the DOE or the U.S. government. Author contributions: Conceptualization:L.D.,K.M.,andJ.S.Organicchemicalsynthesis:J.S.Devicefabricationand generalchara cteriza tion:K.M.,J.S.,Y .T ., andA.B.UPS/XPSmeasurementandanalysis:H.R.A.and K.R.G.TRMCmeasurement:B.W .L. TRPLmeasurementandanalysis:D.S.andH.Y .Cyclic voltammetry:K.C.LEDmeasurement:K.W .Contactanglemeasurement:Y .L. Supervision:L.D., J.M.,andL.H.Writing—originaldraft:K.M.,J.S.,andL.D.Writing—reviewandediting:allauthors Competinginterests:Anapplicationhasbeenmadeforaprovisionalpatent(U.S.patent application number 70055-01) related to the subject matter of this manuscript, and the authorshipincludeL.D.,K.M.,andJ.S.Theauthorsdeclarethattheyhav enoothercompeting interests.Dataandmaterialsavailability:Alldataneededtoevaluatetheconclusionsinthe paperarepresentinthepaperand/ortheSupplementaryMaterials.

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© 2023 The Authors.

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Ma, K., Sun, J., Atapattu, H. R., Larson, B. W., Yang, H., Sun, D., Chen, K., Wang, K., Lee, Y., Tang, Y., Bhoopalam, A., Huang, L., Graham, K. R., Mei, J., & Dou, L. (2023). Holistic energy landscape management in 2D/3D heterojunction via molecular engineering for efficient perovskite solar cells. Science advances, 9(23), Article eadg0032. https://doi.org/10.1126/sciadv.adg0032

@article{7bf0566c70814f289df461164f5845a5,

title = "Holistic energy landscape management in 2D/3D heterojunction via molecular engineering for efficient perovskite solar cells",

abstract = "Constructing two-dimensional (2D) perovskite atop of 3D with energy landscape management is still a challenge in perovskite photovoltaics. Here, we report a strategy through designing a series of π-conjugated organic cations to construct stable 2D perovskites and to realize delicate energy level tunability at 2D/3D heterojunctions. As a result, the hole transfer energy barriers can be reduced both at heterojunctions and within 2D structures, and the preferable work function shift reduces charge accumulation at interface. Leveraging these insights and also benefitted from the superior interface contact between conjugated cations and poly(triarylamine) (PTAA) hole transporting layer, a solar cell with power conversion efficiency of 24.6% has been achieved, which is the highest among PTAA-based n-i-p devices to the best of our knowledge. The devices exhibit greatly enhanced stability and reproducibility. This approach is generic to several hole transporting materials, offering opportunities to realize high efficiency without using the unstable Spiro-OMeTAD.",

author = "Ke Ma and Jiaonan Sun and Atapattu, {Harindi R.} and Larson, {Bryon W.} and Hanjun Yang and Dewei Sun and Ke Chen and Kang Wang and Yoonho Lee and Yuanhao Tang and Anika Bhoopalam and Libai Huang and Graham, {Kenneth R.} and Jianguo Mei and Letian Dou",

note = "Funding Information: Acknowledgments:W ethankK.ZhuforexperimentalhelpandM.Zellerforsingle-crystal analysis.W ealsothankT .T erlier forTOF-SIMScharacterization.Funding:Thismaterialisbased on work supported by the U.S. Department of Energy{\textquoteright}s Office of Energy Efficiency and RenewableEnergy(EERE)underSolarEnergyT echnologies OfficeA wardDE-EE0009519.K.M. acknowledgesthefinancialsupportfromLillianGilbrethPostdoctoralFellowships.H.R.A.and K.R.G.acknowledgefundingfromtheOfficeofScienceoftheU.S.DepartmentofEnergyfor supportingtheUPSandXPSmeasurementsunderawardnumberDE-SC0018208.D.S.andL.H. acknowledgefundingfromtheOfficeofScienceoftheU.S.DepartmentofEnergyfor supportingthetime-resolvedT AandPLmeasurementsunderawardnumberDE-SC0022082. TheworkwaspartiallysupportedbytheU.S.DepartmentofEnergyundercontractnumberDE-A C36-08GO28308 withAllianceforSustainableEnergy,LimitedLiabilityCompany(LLC),the ManagerandOperatoroftheNationalRenewableEnergyLaboratory.TRMCmeasurementsand opticalcharacterizationsweresupportedbytheDe-RiskingHalidePero vskite SolarCells programoftheNationalCenterforPhotovoltaicsfromDE-FO A-0002064 andDE-EE0008790, fundedbytheU.S.DepartmentofEnergy,OfficeofEnergyEfficiencyandRenewableEnergy, SolarEnergyT echnologies Office.Theviewsexpressedinthearticledonotnecessarily represent the views of the DOE or the U.S. government. Author contributions: Conceptualization:L.D.,K.M.,andJ.S.Organicchemicalsynthesis:J.S.Devicefabricationand generalchara cteriza tion:K.M.,J.S.,Y .T ., andA.B.UPS/XPSmeasurementandanalysis:H.R.A.and K.R.G.TRMCmeasurement:B.W .L. TRPLmeasurementandanalysis:D.S.andH.Y .Cyclic voltammetry:K.C.LEDmeasurement:K.W .Contactanglemeasurement:Y .L. Supervision:L.D., J.M.,andL.H.Writing—originaldraft:K.M.,J.S.,andL.D.Writing—reviewandediting:allauthors Competinginterests:Anapplicationhasbeenmadeforaprovisionalpatent(U.S.patent application number 70055-01) related to the subject matter of this manuscript, and the authorshipincludeL.D.,K.M.,andJ.S.Theauthorsdeclarethattheyhav enoothercompeting interests.Dataandmaterialsavailability:Alldataneededtoevaluatetheconclusionsinthe paperarepresentinthepaperand/ortheSupplementaryMaterials. Publisher Copyright: {\textcopyright} 2023 The Authors.",

year = "2023",

month = jun,

doi = "10.1126/sciadv.adg0032",

language = "English",

volume = "9",

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T1 - Holistic energy landscape management in 2D/3D heterojunction via molecular engineering for efficient perovskite solar cells

AU - Ma, Ke

AU - Sun, Jiaonan

AU - Atapattu, Harindi R.

AU - Larson, Bryon W.

AU - Yang, Hanjun

AU - Sun, Dewei

AU - Chen, Ke

AU - Wang, Kang

AU - Lee, Yoonho

AU - Tang, Yuanhao

AU - Bhoopalam, Anika

AU - Huang, Libai

AU - Graham, Kenneth R.

AU - Mei, Jianguo

AU - Dou, Letian

N1 - Funding Information: Acknowledgments:W ethankK.ZhuforexperimentalhelpandM.Zellerforsingle-crystal analysis.W ealsothankT .T erlier forTOF-SIMScharacterization.Funding:Thismaterialisbased on work supported by the U.S. Department of Energy’s Office of Energy Efficiency and RenewableEnergy(EERE)underSolarEnergyT echnologies OfficeA wardDE-EE0009519.K.M. acknowledgesthefinancialsupportfromLillianGilbrethPostdoctoralFellowships.H.R.A.and K.R.G.acknowledgefundingfromtheOfficeofScienceoftheU.S.DepartmentofEnergyfor supportingtheUPSandXPSmeasurementsunderawardnumberDE-SC0018208.D.S.andL.H. acknowledgefundingfromtheOfficeofScienceoftheU.S.DepartmentofEnergyfor supportingthetime-resolvedT AandPLmeasurementsunderawardnumberDE-SC0022082. TheworkwaspartiallysupportedbytheU.S.DepartmentofEnergyundercontractnumberDE-A C36-08GO28308 withAllianceforSustainableEnergy,LimitedLiabilityCompany(LLC),the ManagerandOperatoroftheNationalRenewableEnergyLaboratory.TRMCmeasurementsand opticalcharacterizationsweresupportedbytheDe-RiskingHalidePero vskite SolarCells programoftheNationalCenterforPhotovoltaicsfromDE-FO A-0002064 andDE-EE0008790, fundedbytheU.S.DepartmentofEnergy,OfficeofEnergyEfficiencyandRenewableEnergy, SolarEnergyT echnologies Office.Theviewsexpressedinthearticledonotnecessarily represent the views of the DOE or the U.S. government. Author contributions: Conceptualization:L.D.,K.M.,andJ.S.Organicchemicalsynthesis:J.S.Devicefabricationand generalchara cteriza tion:K.M.,J.S.,Y .T ., andA.B.UPS/XPSmeasurementandanalysis:H.R.A.and K.R.G.TRMCmeasurement:B.W .L. TRPLmeasurementandanalysis:D.S.andH.Y .Cyclic voltammetry:K.C.LEDmeasurement:K.W .Contactanglemeasurement:Y .L. Supervision:L.D., J.M.,andL.H.Writing—originaldraft:K.M.,J.S.,andL.D.Writing—reviewandediting:allauthors Competinginterests:Anapplicationhasbeenmadeforaprovisionalpatent(U.S.patent application number 70055-01) related to the subject matter of this manuscript, and the authorshipincludeL.D.,K.M.,andJ.S.Theauthorsdeclarethattheyhav enoothercompeting interests.Dataandmaterialsavailability:Alldataneededtoevaluatetheconclusionsinthe paperarepresentinthepaperand/ortheSupplementaryMaterials. Publisher Copyright: © 2023 The Authors.

PY - 2023/6

Y1 - 2023/6

N2 - Constructing two-dimensional (2D) perovskite atop of 3D with energy landscape management is still a challenge in perovskite photovoltaics. Here, we report a strategy through designing a series of π-conjugated organic cations to construct stable 2D perovskites and to realize delicate energy level tunability at 2D/3D heterojunctions. As a result, the hole transfer energy barriers can be reduced both at heterojunctions and within 2D structures, and the preferable work function shift reduces charge accumulation at interface. Leveraging these insights and also benefitted from the superior interface contact between conjugated cations and poly(triarylamine) (PTAA) hole transporting layer, a solar cell with power conversion efficiency of 24.6% has been achieved, which is the highest among PTAA-based n-i-p devices to the best of our knowledge. The devices exhibit greatly enhanced stability and reproducibility. This approach is generic to several hole transporting materials, offering opportunities to realize high efficiency without using the unstable Spiro-OMeTAD.

AB - Constructing two-dimensional (2D) perovskite atop of 3D with energy landscape management is still a challenge in perovskite photovoltaics. Here, we report a strategy through designing a series of π-conjugated organic cations to construct stable 2D perovskites and to realize delicate energy level tunability at 2D/3D heterojunctions. As a result, the hole transfer energy barriers can be reduced both at heterojunctions and within 2D structures, and the preferable work function shift reduces charge accumulation at interface. Leveraging these insights and also benefitted from the superior interface contact between conjugated cations and poly(triarylamine) (PTAA) hole transporting layer, a solar cell with power conversion efficiency of 24.6% has been achieved, which is the highest among PTAA-based n-i-p devices to the best of our knowledge. The devices exhibit greatly enhanced stability and reproducibility. This approach is generic to several hole transporting materials, offering opportunities to realize high efficiency without using the unstable Spiro-OMeTAD.

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Holistic energy landscape management in 2D/3D heterojunction via molecular engineering for efficient perovskite solar cells

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