Vashishtha, Parth, Griffith, Benjamin E., Fang, Yanan, Jaiswal, Ankit, Nutan, Gautam V., Bartók, Albert P., White, Tim and Hanna, John V. (2022) Data for Elucidation of the structural and optical properties of metal cation (Na+, K+, and Bi3+) incorporated Cs2AgInCl6 double perovskite nanocrystals. [Dataset]

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Abstract

This study presents series of direct band gap Pb-free double perovskite Cs2AgInxBi1−xCl6, Cs2NaxAg1−xInCl6:Bi and Cs2KxAg1−xInCl6:Bi nanocrystal systems [Cs2B′(I)B′′(III)Cl6] synthesised using a colloidal hot-injection route. The structural properties investigated using powder XRD, TEM, solid state NMR and materials modelling approaches demonstrate that the incorporation of K+ cations into the double perovskite nanocrystal structure occurs simultaneously on both the Cs (A) site and Ag (B′(I)) positions within a series of closely related cubic and monoclinic structures. As a result of defect passivation, significant improvements in the photoluminescence quantum yield (PLQY) of ∼4.7× and ∼1.8× are exhibited in comparison to the Cs2AgInxBi1−xCl6, and Cs2NaxAg1−xInCl6:Bi nanocrystal systems, respectively. Materials modelling using the Ab Initio Random Structure Search (AIRSS) method, and the GIPAW DFT calculation of the NMR parameters from the derived structural realisations, shows that K+ incorporation induces significant short-range structural disorder and multi-phase formation. This is highlighted by the large 133Cs and 39K chemical shift dispersion characterising the MAS NMR data. Density of States (DoS) calculations describing these AIRSS generated structures suggest that increasing ionic character and reduced structural rigidity are strongly correlated with A site substitution of the K+ cation into these cubic and monoclinic phases. The 39K MAS NMR data reveals that the increasing PLQY performance maps directly with the K+ incorporation into the cubic CsKyAg1−yInCl6 phase supporting B site occupancy which is observed to be maximized at a 60 ml% K+ incorporation level. However, additional evidence indicates that low level K+ substitution primarily targets A site occupancy in a surface passivation role. The improvement to the optical properties induced by K+ and Na+ incorporation is rationalised in terms of increased covalent character and structural rigidity associated with decreased Cs+, Na+ and K+ cation mobility, as evidenced by the large (∼2 orders of magnitude) variation in the 133Cs T1 data across each compositional range.

Item Type:	Dataset
Subjects:	Q Science > QC Physics Q Science > QE Geology T Technology > TA Engineering (General). Civil engineering (General)
Divisions:	Faculty of Science, Engineering and Medicine > Science > Physics
Library of Congress Subject Headings (LCSH):	Perovskite (Mineral), Nanocrystals, Cations -- Structure , Cations -- Optical properties
Publisher:	University of Warwick, Department of Physics
Official Date:	14 January 2022
Dates:	Date Event 14 January 2022 Published 1 December 2021 Available 1 December 2021 Created
Status:	Not Peer Reviewed
Publication Status:	Published
Media of Output (format):	.txt .xy .OPJU .tiff .csv .1r .magres
Access rights to Published version:	Open Access (Creative Commons)
Copyright Holders:	University of Warwick
Description:	Dataset contains XRD Data, TEM Data, UV-Vis absoption Data, Photoluminescence (PL) Data, NMR Data and DFT calculations. All text documents and the .xy XRD data can be opened using Excel, OriginPro or any text editor. OPJU files can be opened in Origin or OriginPro. .Tiff files can be opened using Photo Viewer. .Csv file can be opend using Excel. .1r files can be opened using the Bruker software Topspin. .magres files can be opened using an editor.
Date of first compliant deposit:	1 December 2021
Date of first compliant Open Access:	14 January 2022
RIOXX Funder/Project Grant:	Project/Grant ID RIOXX Funder Name Funder ID EP/M028186/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266 EP/K024418/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266 UNSPECIFIED [BBSRC] Biotechnology and Biological Sciences Research Council http://dx.doi.org/10.13039/501100000268 UNSPECIFIED University of Warwick http://dx.doi.org/10.13039/501100000741 UNSPECIFIED [ERDF] European Regional Development Fund http://dx.doi.org/10.13039/501100008530 UNSPECIFIED Advantage West Midlands http://dx.doi.org/10.13039/100014381 UNSPECIFIED University Of Birmingham http://dx.doi.org/10.13039/501100000855 04INS000581C150OOE01 Nanyang Technological University http://dx.doi.org/10.13039/501100001475 EP/P020232/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266
Related URLs:	Related item in WRAP
Contributors:	Contribution Name Contributor ID Depositor Hanna, John V. 28389

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