TY - JOUR
T1 - Optical Fingerprints of Polynuclear Complexes in Lead Halide Perovskite Precursor Solutions
AU - Valencia, Ana M.
AU - Shargaieva, Oleksandra
AU - Schier, Richard
AU - Unger, Eva
AU - Cocchi, Caterina
N1 - Funding Information:
This work was supported by the German Research Foundation (DFG), Priority Programm SPP 2196 (Project 424394788). C.C. acknowledges funding from the German Federal Ministry of Education and Research (Professorinnenprogramm III) as well as from the State of Lower Saxony (Professorinnen für Niedersachsen). Computational resources were provided by the North-German Supercomputing Alliance (HLRN) (Project bep00076).
Publisher Copyright:
©
Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.
PY - 2021
Y1 - 2021
N2 - Solvent-solute interactions in precursor solutions of lead halide perovskites (LHPs) critically impact the quality of solution-processed materials, as they lead to the formation of a variety of poly-iodoplumbates that act as building blocks for LHPs. The formation of [PbI2+n]n- complexes is often expected in diluted solutions, while coordination occurring at high concentrations is not yet well understood. In a combined ab initio and experimental work, we demonstrate that the optical spectra of the quasi-one-dimensional iodoplumbate complexes PbI2(DMSO)4, Pb2I4(DMSO)6, and Pb3I6(DMSO)8 formed in dimethyl sulfoxide solutions are compatible with the spectral fingerprints measured at high lead iodide concentrations. This finding suggests that the interpretation of optical spectra of LHP precursor solutions should account for the formation of polynuclear lead halide complexes.
AB - Solvent-solute interactions in precursor solutions of lead halide perovskites (LHPs) critically impact the quality of solution-processed materials, as they lead to the formation of a variety of poly-iodoplumbates that act as building blocks for LHPs. The formation of [PbI2+n]n- complexes is often expected in diluted solutions, while coordination occurring at high concentrations is not yet well understood. In a combined ab initio and experimental work, we demonstrate that the optical spectra of the quasi-one-dimensional iodoplumbate complexes PbI2(DMSO)4, Pb2I4(DMSO)6, and Pb3I6(DMSO)8 formed in dimethyl sulfoxide solutions are compatible with the spectral fingerprints measured at high lead iodide concentrations. This finding suggests that the interpretation of optical spectra of LHP precursor solutions should account for the formation of polynuclear lead halide complexes.
U2 - 10.1021/acs.jpclett.0c03741
DO - 10.1021/acs.jpclett.0c03741
M3 - Article
C2 - 33651616
AN - SCOPUS:85102906093
SN - 1948-7185
VL - 12
SP - 2299
EP - 2305
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 9
ER -