Molecular and Self-Trapped Excitonic Contributions to the Broadband Luminescence in Diamine-Based Low-Dimensional Hybrid Perovskite Systems

Shrreya Krishnamurthy; Rounak Naphade; Wasim J. Mir; Suresh Gosavi; Sudip Chakraborty; Ramanathan Vaidhyanathan; Satishchandra Ogale

doi:10.1002/adom.201800751

Molecular and Self-Trapped Excitonic Contributions to the Broadband Luminescence in Diamine-Based Low-Dimensional Hybrid Perovskite Systems

Shrreya Krishnamurthy, Rounak Naphade, Wasim J. Mir, Suresh Gosavi, Sudip Chakraborty^*, Ramanathan Vaidhyanathan, Satishchandra Ogale

^*Corresponding author for this work

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

42 Scopus citations

Abstract

The present solid state lighting (SSL) technology is based on using a combination of phosphors to give the desired white light emitting devices. The property of broadband emission from a single phosphor is not only difficult to achieve but also poses a challenge in device fabrication. Hybrid organic–inorganic perovskites especially in low dimensions (2D/1D) are being widely explored for their optoelectronic properties. Few of these materials exhibit broadband emission upon ultraviolet excitation, providing a scope for synthetic engineering in achieving commercially viable single-phosphor materials. In this work, three interesting diammonium-based low-dimensional hybrid perovskites for broadband photoluminescence (PL) are examined. The doubly protonated ethylenediamine-configured monoclinic (P2₁/n) 1D ribbon assembly (H₃NCH₂CH₂NH₃)₈(Pb₄Br₁₈) · Br₆ (1) and the orthorhombic (Pbcm) 2D-twisted octahedral (H₃NCH₂CH₂NH₃)(Pb₂Cl₆) (2) show white luminescence, while the doubly protonated piperazine-configured orthorhombic (Pnnm) 0D dual-octahedral (C₄N₂H₁₂)₄(Pb₂Br₁₁) · (Br)(H₂O)₄ (3) exhibits bluish-white luminescence. Based on the PL of the organic diammonium salt, the time-resolved PL, Raman signatures, and density functional theory (DFT) calculations, it is shown that the broadband luminescence has dual origin: one around 400 nm from diammonium-related molecular fluorescence and another around 516 nm from self-trapped excitons. The structure-specific relative contributions and interplay between the two define the overall character of the broadband luminescence.

Original language	English (US)
Article number	1800751
Journal	Advanced Optical Materials
Volume	6
Issue number	20
DOIs	https://doi.org/10.1002/adom.201800751
State	Published - Oct 18 2018

Bibliographical note

Funding Information:
SK would like to thank CSIR for funding. The authors would like to gratefully acknowledge funding support from the DST-CERI, DST Nanomission (thematic unit), UKEIRI, and SUNRISE. The authors also like to thank Angshuman Nag, Pramod Pillai (IISER Pune), S. K. Asha (CSIR-NCL), K. S. Narayan (JNCASR), and their students, as well as Ms. Archana Patil for experimental help and Dr. Aditya Sadhanala (Cambridge) for fruitful discussions. PRACE is acknowledged for computing time.

Publisher Copyright:
© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

hybrid perovskites
self-trapped excitons
single crystals
small molecules
white light emission

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Atomic and Molecular Physics, and Optics

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10.1002/adom.201800751

Cite this

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title = "Molecular and Self-Trapped Excitonic Contributions to the Broadband Luminescence in Diamine-Based Low-Dimensional Hybrid Perovskite Systems",

abstract = "The present solid state lighting (SSL) technology is based on using a combination of phosphors to give the desired white light emitting devices. The property of broadband emission from a single phosphor is not only difficult to achieve but also poses a challenge in device fabrication. Hybrid organic–inorganic perovskites especially in low dimensions (2D/1D) are being widely explored for their optoelectronic properties. Few of these materials exhibit broadband emission upon ultraviolet excitation, providing a scope for synthetic engineering in achieving commercially viable single-phosphor materials. In this work, three interesting diammonium-based low-dimensional hybrid perovskites for broadband photoluminescence (PL) are examined. The doubly protonated ethylenediamine-configured monoclinic (P21/n) 1D ribbon assembly (H3NCH2CH2NH3)8(Pb4Br18) · Br6 (1) and the orthorhombic (Pbcm) 2D-twisted octahedral (H3NCH2CH2NH3)(Pb2Cl6) (2) show white luminescence, while the doubly protonated piperazine-configured orthorhombic (Pnnm) 0D dual-octahedral (C4N2H12)4(Pb2Br11) · (Br)(H2O)4 (3) exhibits bluish-white luminescence. Based on the PL of the organic diammonium salt, the time-resolved PL, Raman signatures, and density functional theory (DFT) calculations, it is shown that the broadband luminescence has dual origin: one around 400 nm from diammonium-related molecular fluorescence and another around 516 nm from self-trapped excitons. The structure-specific relative contributions and interplay between the two define the overall character of the broadband luminescence.",

keywords = "hybrid perovskites, self-trapped excitons, single crystals, small molecules, white light emission",

author = "Shrreya Krishnamurthy and Rounak Naphade and Mir, {Wasim J.} and Suresh Gosavi and Sudip Chakraborty and Ramanathan Vaidhyanathan and Satishchandra Ogale",

note = "Funding Information: SK would like to thank CSIR for funding. The authors would like to gratefully acknowledge funding support from the DST-CERI, DST Nanomission (thematic unit), UKEIRI, and SUNRISE. The authors also like to thank Angshuman Nag, Pramod Pillai (IISER Pune), S. K. Asha (CSIR-NCL), K. S. Narayan (JNCASR), and their students, as well as Ms. Archana Patil for experimental help and Dr. Aditya Sadhanala (Cambridge) for fruitful discussions. PRACE is acknowledged for computing time. Publisher Copyright: {\textcopyright} 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

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language = "English (US)",

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AU - Krishnamurthy, Shrreya

AU - Naphade, Rounak

AU - Mir, Wasim J.

AU - Gosavi, Suresh

AU - Chakraborty, Sudip

AU - Vaidhyanathan, Ramanathan

AU - Ogale, Satishchandra

N1 - Funding Information: SK would like to thank CSIR for funding. The authors would like to gratefully acknowledge funding support from the DST-CERI, DST Nanomission (thematic unit), UKEIRI, and SUNRISE. The authors also like to thank Angshuman Nag, Pramod Pillai (IISER Pune), S. K. Asha (CSIR-NCL), K. S. Narayan (JNCASR), and their students, as well as Ms. Archana Patil for experimental help and Dr. Aditya Sadhanala (Cambridge) for fruitful discussions. PRACE is acknowledged for computing time. Publisher Copyright: © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2018/10/18

Y1 - 2018/10/18

N2 - The present solid state lighting (SSL) technology is based on using a combination of phosphors to give the desired white light emitting devices. The property of broadband emission from a single phosphor is not only difficult to achieve but also poses a challenge in device fabrication. Hybrid organic–inorganic perovskites especially in low dimensions (2D/1D) are being widely explored for their optoelectronic properties. Few of these materials exhibit broadband emission upon ultraviolet excitation, providing a scope for synthetic engineering in achieving commercially viable single-phosphor materials. In this work, three interesting diammonium-based low-dimensional hybrid perovskites for broadband photoluminescence (PL) are examined. The doubly protonated ethylenediamine-configured monoclinic (P21/n) 1D ribbon assembly (H3NCH2CH2NH3)8(Pb4Br18) · Br6 (1) and the orthorhombic (Pbcm) 2D-twisted octahedral (H3NCH2CH2NH3)(Pb2Cl6) (2) show white luminescence, while the doubly protonated piperazine-configured orthorhombic (Pnnm) 0D dual-octahedral (C4N2H12)4(Pb2Br11) · (Br)(H2O)4 (3) exhibits bluish-white luminescence. Based on the PL of the organic diammonium salt, the time-resolved PL, Raman signatures, and density functional theory (DFT) calculations, it is shown that the broadband luminescence has dual origin: one around 400 nm from diammonium-related molecular fluorescence and another around 516 nm from self-trapped excitons. The structure-specific relative contributions and interplay between the two define the overall character of the broadband luminescence.

AB - The present solid state lighting (SSL) technology is based on using a combination of phosphors to give the desired white light emitting devices. The property of broadband emission from a single phosphor is not only difficult to achieve but also poses a challenge in device fabrication. Hybrid organic–inorganic perovskites especially in low dimensions (2D/1D) are being widely explored for their optoelectronic properties. Few of these materials exhibit broadband emission upon ultraviolet excitation, providing a scope for synthetic engineering in achieving commercially viable single-phosphor materials. In this work, three interesting diammonium-based low-dimensional hybrid perovskites for broadband photoluminescence (PL) are examined. The doubly protonated ethylenediamine-configured monoclinic (P21/n) 1D ribbon assembly (H3NCH2CH2NH3)8(Pb4Br18) · Br6 (1) and the orthorhombic (Pbcm) 2D-twisted octahedral (H3NCH2CH2NH3)(Pb2Cl6) (2) show white luminescence, while the doubly protonated piperazine-configured orthorhombic (Pnnm) 0D dual-octahedral (C4N2H12)4(Pb2Br11) · (Br)(H2O)4 (3) exhibits bluish-white luminescence. Based on the PL of the organic diammonium salt, the time-resolved PL, Raman signatures, and density functional theory (DFT) calculations, it is shown that the broadband luminescence has dual origin: one around 400 nm from diammonium-related molecular fluorescence and another around 516 nm from self-trapped excitons. The structure-specific relative contributions and interplay between the two define the overall character of the broadband luminescence.

KW - hybrid perovskites

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KW - small molecules

KW - white light emission

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DO - 10.1002/adom.201800751

M3 - Article

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VL - 6

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ER -

Molecular and Self-Trapped Excitonic Contributions to the Broadband Luminescence in Diamine-Based Low-Dimensional Hybrid Perovskite Systems

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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