TY - JOUR
T1 - Molecular and Self-Trapped Excitonic Contributions to the Broadband Luminescence in Diamine-Based Low-Dimensional Hybrid Perovskite Systems
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 (H3NCH2CH2NH3)8(Pb4Br18) · Br6 (1) and the orthorhombic (Pbcm) 2D-twisted octahedral (H3NCH2CH2NH3)(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 (H3NCH2CH2NH3)8(Pb4Br18) · Br6 (1) and the orthorhombic (Pbcm) 2D-twisted octahedral (H3NCH2CH2NH3)(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
KW - self-trapped excitons
KW - single crystals
KW - small molecules
KW - white light emission
UR - http://www.scopus.com/inward/record.url?scp=85051067393&partnerID=8YFLogxK
U2 - 10.1002/adom.201800751
DO - 10.1002/adom.201800751
M3 - Article
AN - SCOPUS:85051067393
SN - 2195-1071
VL - 6
JO - Advanced Optical Materials
JF - Advanced Optical Materials
IS - 20
M1 - 1800751
ER -