Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy
<jats:p> Transient microscopy has emerged as a powerful tool for imaging the diffusion of excitons and free charge carriers in optoelectronic materials. In many excitonic materials, extraction of diffusion coefficients can be simplified because of the linear relationship between signal intensi...
| Main Authors: | , , , , , |
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| Format: | Article |
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AIP Publishing
2022
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| Online Access: | https://hdl.handle.net/1721.1/145519 |
| _version_ | 1826195103799050240 |
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| author | Nagaya Wong, Narumi Ha, Seung Kyun Williams, Kristopher Shcherbakov-Wu, Wenbi Swan, James W. Tisdale, William A. |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Nagaya Wong, Narumi Ha, Seung Kyun Williams, Kristopher Shcherbakov-Wu, Wenbi Swan, James W. Tisdale, William A. |
| author_sort | Nagaya Wong, Narumi |
| collection | MIT |
| description | <jats:p> Transient microscopy has emerged as a powerful tool for imaging the diffusion of excitons and free charge carriers in optoelectronic materials. In many excitonic materials, extraction of diffusion coefficients can be simplified because of the linear relationship between signal intensity and local excited state population. However, in materials where transport is dominated by free charge carriers, extracting diffusivities accurately from multidimensional data is complicated by the nonlinear dependence of the measured signal on the local charge carrier density. To obtain accurate estimates of charge carrier diffusivity from transient microscopy data, statistically robust fitting algorithms coupled to efficient 3D numerical solvers that faithfully relate local carrier dynamics to raw experimental measurables are sometimes needed. Here, we provide a detailed numerical framework for modeling the spatiotemporal dynamics of free charge carriers in bulk semiconductors with significant solving speed reduction and for simulating the corresponding transient photoluminescence microscopy data. To demonstrate the utility of this approach, we apply a fitting algorithm using a Markov chain Monte Carlo sampler to experimental data on bulk CdS and methylammonium lead bromide (MAPbBr<jats:sub>3</jats:sub>) crystals. Parameter analyses reveal that transient photoluminescence microscopy can be used to obtain robust estimates of charge carrier diffusivities in optoelectronic materials of interest, but that other experimental approaches should be used for obtaining carrier recombination constants. Additionally, simplifications can be made to the fitting model depending on the experimental conditions and material systems studied. Our open-source simulation code and fitting algorithm are made freely available to the scientific community. </jats:p> |
| first_indexed | 2024-09-23T10:07:04Z |
| format | Article |
| id | mit-1721.1/145519 |
| institution | Massachusetts Institute of Technology |
| last_indexed | 2024-09-23T10:07:04Z |
| publishDate | 2022 |
| publisher | AIP Publishing |
| record_format | dspace |
| spelling | mit-1721.1/1455192022-09-30T19:02:16Z Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy Nagaya Wong, Narumi Ha, Seung Kyun Williams, Kristopher Shcherbakov-Wu, Wenbi Swan, James W. Tisdale, William A. Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Chemistry <jats:p> Transient microscopy has emerged as a powerful tool for imaging the diffusion of excitons and free charge carriers in optoelectronic materials. In many excitonic materials, extraction of diffusion coefficients can be simplified because of the linear relationship between signal intensity and local excited state population. However, in materials where transport is dominated by free charge carriers, extracting diffusivities accurately from multidimensional data is complicated by the nonlinear dependence of the measured signal on the local charge carrier density. To obtain accurate estimates of charge carrier diffusivity from transient microscopy data, statistically robust fitting algorithms coupled to efficient 3D numerical solvers that faithfully relate local carrier dynamics to raw experimental measurables are sometimes needed. Here, we provide a detailed numerical framework for modeling the spatiotemporal dynamics of free charge carriers in bulk semiconductors with significant solving speed reduction and for simulating the corresponding transient photoluminescence microscopy data. To demonstrate the utility of this approach, we apply a fitting algorithm using a Markov chain Monte Carlo sampler to experimental data on bulk CdS and methylammonium lead bromide (MAPbBr<jats:sub>3</jats:sub>) crystals. Parameter analyses reveal that transient photoluminescence microscopy can be used to obtain robust estimates of charge carrier diffusivities in optoelectronic materials of interest, but that other experimental approaches should be used for obtaining carrier recombination constants. Additionally, simplifications can be made to the fitting model depending on the experimental conditions and material systems studied. Our open-source simulation code and fitting algorithm are made freely available to the scientific community. </jats:p> 2022-09-20T15:03:00Z 2022-09-20T15:03:00Z 2022-09-14 Article http://purl.org/eprint/type/JournalArticle 0021-9606 1089-7690 https://hdl.handle.net/1721.1/145519 Nagaya Wong, Narumi, Ha, Seung Kyun, Williams, Kristopher, Shcherbakov-Wu, Wenbi, Swan, James W. et al. 2022. "Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy." 157 (10). 10.1063/5.0100075 Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf AIP Publishing American Institute of Physics (AIP) |
| spellingShingle | Nagaya Wong, Narumi Ha, Seung Kyun Williams, Kristopher Shcherbakov-Wu, Wenbi Swan, James W. Tisdale, William A. Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy |
| title | Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy |
| title_full | Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy |
| title_fullStr | Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy |
| title_full_unstemmed | Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy |
| title_short | Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy |
| title_sort | robust estimation of charge carrier diffusivity using transient photoluminescence microscopy |
| url | https://hdl.handle.net/1721.1/145519 |
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