Elucidating the Structure and Photophysics of Layered Perovskites through Cation Fluorination
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Elucidating the Structure and Photophysics of Layered Perovskites through Cation Fluorination. / Tekelenburg, Eelco K.; Kahmann, Simon; Kamminga, Machteld E.; Blake, Graeme R.; Loi, Maria A.
I: Advanced Optical Materials, 10.02.2021.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Elucidating the Structure and Photophysics of Layered Perovskites through Cation Fluorination
AU - Tekelenburg, Eelco K.
AU - Kahmann, Simon
AU - Kamminga, Machteld E.
AU - Blake, Graeme R.
AU - Loi, Maria A.
PY - 2021/2/10
Y1 - 2021/2/10
N2 - Optoelectronic devices based on layered perovskites containing fluorinated cations display a well-documented improved stability and enhanced performance over non-fluorinated cations. The effect of fluorination on the crystal structure and photophysics, however, has received limited attention up until now. Here, 3-fluorophenethylammonium lead iodide ((3-FPEA)(2)PbI4) single crystals are investigated and their properties to the non-fluorinated ((PEA)(2)PbI4) variant are compared. The bulkier 3-FPEA cation increases the distortion of the inorganic layers, resulting in a blue-shifted absorbance and photoluminescence. Temperature-dependent photoluminescence spectroscopy reveals an intricate exciton substructure in both cases. The fluorinated variant shows hot-exciton resonances separated by 12 to 15 meV, values that are much smaller than the 40 to 46 meV found for (PEA)(2)PbI4. In addition, high-resolution spectra show that the emission at lower energies consists of a substructure, previously thought to be a single line. With the analysis on the resolved photoluminescence, a vibronic progression is excluded as the origin of the emission at lower energies. Instead, part of the excitonic substructure is proposed to originate from bound excitons. This work furthers the understanding of the photophysics of layered perovskites that has been heavily debated lately.
AB - Optoelectronic devices based on layered perovskites containing fluorinated cations display a well-documented improved stability and enhanced performance over non-fluorinated cations. The effect of fluorination on the crystal structure and photophysics, however, has received limited attention up until now. Here, 3-fluorophenethylammonium lead iodide ((3-FPEA)(2)PbI4) single crystals are investigated and their properties to the non-fluorinated ((PEA)(2)PbI4) variant are compared. The bulkier 3-FPEA cation increases the distortion of the inorganic layers, resulting in a blue-shifted absorbance and photoluminescence. Temperature-dependent photoluminescence spectroscopy reveals an intricate exciton substructure in both cases. The fluorinated variant shows hot-exciton resonances separated by 12 to 15 meV, values that are much smaller than the 40 to 46 meV found for (PEA)(2)PbI4. In addition, high-resolution spectra show that the emission at lower energies consists of a substructure, previously thought to be a single line. With the analysis on the resolved photoluminescence, a vibronic progression is excluded as the origin of the emission at lower energies. Instead, part of the excitonic substructure is proposed to originate from bound excitons. This work furthers the understanding of the photophysics of layered perovskites that has been heavily debated lately.
KW - crystal substructure
KW - fluorinated cations
KW - layered perovskites
KW - luminescence spectroscopy
KW - photophysics
KW - Ruddlesden–
KW - Popper phase
KW - single crystals
U2 - 10.1002/adom.202001647
DO - 10.1002/adom.202001647
M3 - Journal article
JO - Advanced Optical Materials
JF - Advanced Optical Materials
SN - 2195-1071
M1 - 2001647
ER -
ID: 260358218