Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale
We study the low-temperature (T = 4.7 K) emission dynamics of a thin film of methylammonium lead bromide (MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn&g...
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MDPI AG
2023-08-01
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| Series: | Nanomaterials |
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| Online Access: | https://www.mdpi.com/2079-4991/13/16/2376 |
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| author | Justine Baronnier Benoit Mahler Christophe Dujardin Julien Houel |
| author_facet | Justine Baronnier Benoit Mahler Christophe Dujardin Julien Houel |
| author_sort | Justine Baronnier |
| collection | DOAJ |
| description | We study the low-temperature (T = 4.7 K) emission dynamics of a thin film of methylammonium lead bromide (MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula>), prepared via the anti-solvent method. Using intensity-dependent (over 5 decades) hyperspectral microscopy under quasi-resonant (532 nm) continuous wave excitation, we revealed spatial inhomogeneities in the thin film emission. This was drastically different at the band-edge (∼550 nm, sharp peaks) than in the emission tail (∼568 nm, continuum of emission). We are able to observe regions of the film at the micrometer scale where emission is dominated by excitons, in between regions of trap emission. Varying the density of absorbed photons by the MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> thin films, two-color fluorescence lifetime imaging microscopy unraveled the emission dynamics: a fast, resolution-limited (∼200 ps) monoexponential tangled with a stretched exponential decay. We associate the first to the relaxation of excitons and the latter to trap emission dynamics. The obtained stretching exponents can be interpreted as the result of a two-dimensional electron diffusion process: Förster resonant transfer mechanism. Furthermore, the non-vanishing fast monoexponential component even in the tail of the MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> emission indicates the subsistence of localized excitons. Finally, we estimate the density of traps in MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> thin films prepared using the anti-solvent method at <i>n</i>∼10<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mn>17</mn></msup></semantics></math></inline-formula> cm<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mrow><mo>−</mo><mn>3</mn></mrow></msup></semantics></math></inline-formula>. |
| first_indexed | 2024-03-10T23:40:15Z |
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| spelling | doaj.art-14a97ddcc72f44848924ecc71127572c2023-11-19T02:28:15ZengMDPI AGNanomaterials2079-49912023-08-011316237610.3390/nano13162376Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer ScaleJustine Baronnier0Benoit Mahler1Christophe Dujardin2Julien Houel3Université Claude Bernard Lyon 1, Institut Lumière-Matière UMR5306 CNRS, F-69622 Villeurbanne, FranceUniversité Claude Bernard Lyon 1, Institut Lumière-Matière UMR5306 CNRS, F-69622 Villeurbanne, FranceUniversité Claude Bernard Lyon 1, Institut Lumière-Matière UMR5306 CNRS, F-69622 Villeurbanne, FranceUniversité Claude Bernard Lyon 1, Institut Lumière-Matière UMR5306 CNRS, F-69622 Villeurbanne, FranceWe study the low-temperature (T = 4.7 K) emission dynamics of a thin film of methylammonium lead bromide (MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula>), prepared via the anti-solvent method. Using intensity-dependent (over 5 decades) hyperspectral microscopy under quasi-resonant (532 nm) continuous wave excitation, we revealed spatial inhomogeneities in the thin film emission. This was drastically different at the band-edge (∼550 nm, sharp peaks) than in the emission tail (∼568 nm, continuum of emission). We are able to observe regions of the film at the micrometer scale where emission is dominated by excitons, in between regions of trap emission. Varying the density of absorbed photons by the MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> thin films, two-color fluorescence lifetime imaging microscopy unraveled the emission dynamics: a fast, resolution-limited (∼200 ps) monoexponential tangled with a stretched exponential decay. We associate the first to the relaxation of excitons and the latter to trap emission dynamics. The obtained stretching exponents can be interpreted as the result of a two-dimensional electron diffusion process: Förster resonant transfer mechanism. Furthermore, the non-vanishing fast monoexponential component even in the tail of the MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> emission indicates the subsistence of localized excitons. Finally, we estimate the density of traps in MAPbBr<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> thin films prepared using the anti-solvent method at <i>n</i>∼10<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mn>17</mn></msup></semantics></math></inline-formula> cm<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mrow><mo>−</mo><mn>3</mn></mrow></msup></semantics></math></inline-formula>.https://www.mdpi.com/2079-4991/13/16/2376hybrid perovskitetrapthin filmsphotoluminescencemicroscopyhyperspectral |
| spellingShingle | Justine Baronnier Benoit Mahler Christophe Dujardin Julien Houel Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale Nanomaterials hybrid perovskite trap thin films photoluminescence microscopy hyperspectral |
| title | Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale |
| title_full | Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale |
| title_fullStr | Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale |
| title_full_unstemmed | Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale |
| title_short | Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale |
| title_sort | low temperature emission dynamics of methylammonium lead bromide hybrid perovskite thin films at the sub micrometer scale |
| topic | hybrid perovskite trap thin films photoluminescence microscopy hyperspectral |
| url | https://www.mdpi.com/2079-4991/13/16/2376 |
| work_keys_str_mv | AT justinebaronnier lowtemperatureemissiondynamicsofmethylammoniumleadbromidehybridperovskitethinfilmsatthesubmicrometerscale AT benoitmahler lowtemperatureemissiondynamicsofmethylammoniumleadbromidehybridperovskitethinfilmsatthesubmicrometerscale AT christophedujardin lowtemperatureemissiondynamicsofmethylammoniumleadbromidehybridperovskitethinfilmsatthesubmicrometerscale AT julienhouel lowtemperatureemissiondynamicsofmethylammoniumleadbromidehybridperovskitethinfilmsatthesubmicrometerscale |