Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution
Abstract Colloidal nanocrystals (NCs) can be used to prepare high-color-purity metal halide perovskites (MHPs) for light-emitting displays. However, the NCs have a finite particle-size distribution, which broadens the linewidth of photoluminescence spectra under strong quantum confinement, and there...
| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2023-12-01
|
| Series: | Communications Physics |
| Online Access: | https://doi.org/10.1038/s42005-023-01459-8 |
| _version_ | 1797376927683575808 |
|---|---|
| author | Hyun Myung Jang Song Hee Lee Kyung Yeon Jang Jinwoo Park Tae-Woo Lee |
| author_facet | Hyun Myung Jang Song Hee Lee Kyung Yeon Jang Jinwoo Park Tae-Woo Lee |
| author_sort | Hyun Myung Jang |
| collection | DOAJ |
| description | Abstract Colloidal nanocrystals (NCs) can be used to prepare high-color-purity metal halide perovskites (MHPs) for light-emitting displays. However, the NCs have a finite particle-size distribution, which broadens the linewidth of photoluminescence spectra under strong quantum confinement, and thereby degrades the color purity of the MHPs. This paper presents a simple method to quantify this externally-introduced broadening of linewidth $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{SD}}}}}}}$$ Γ SD by combining experimental size-distribution histogram with size-dependent photoluminescence-wavelength (PL- $${{{{{\boldsymbol{\lambda }}}}}}$$ λ ) curve. We develop a semi-empirical method to estimate the other three contributions to the experimentally-measured full-width at half-maximum, $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{EXP}}}}}}}$$ Γ EXP . Namely: the intrinsic linewidth $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{LO}}}}}}}$$ Γ LO caused by exciton-longitudinal optical (LO) phonon Fröhlich coupling; the inhomogeneous linewidth $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{o}}}}}}}$$ Γ o caused by imperfections-related scattering, and the broadening $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{QC}}}}}}}$$ Γ QC due to the quantum-confinement effect. We show that $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{LO}}}}}}}$$ Γ LO of a nanocrystal decreases together with the particle size, disappearing at 1.6 nm radius. Finally, we show that $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{LO}}}}}}}$$ Γ LO is correlated with the degree of Fröhlich-polaron formation, hence proportional to the long-range LO-phonon-electron coupling. |
| first_indexed | 2024-03-08T19:46:36Z |
| format | Article |
| id | doaj.art-af3bc8d7d6a541a2ae8beec744824b0b |
| institution | Directory Open Access Journal |
| issn | 2399-3650 |
| language | English |
| last_indexed | 2024-03-08T19:46:36Z |
| publishDate | 2023-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Physics |
| spelling | doaj.art-af3bc8d7d6a541a2ae8beec744824b0b2023-12-24T12:21:10ZengNature PortfolioCommunications Physics2399-36502023-12-016111610.1038/s42005-023-01459-8Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distributionHyun Myung Jang0Song Hee Lee1Kyung Yeon Jang2Jinwoo Park3Tae-Woo Lee4Research Institute of Advanced Materials (RIAM), Seoul National UniversityResearch Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Seoul National UniversityDepartment of Materials Science and Engineering, Seoul National UniversityResearch Institute of Advanced Materials (RIAM), Seoul National UniversityAbstract Colloidal nanocrystals (NCs) can be used to prepare high-color-purity metal halide perovskites (MHPs) for light-emitting displays. However, the NCs have a finite particle-size distribution, which broadens the linewidth of photoluminescence spectra under strong quantum confinement, and thereby degrades the color purity of the MHPs. This paper presents a simple method to quantify this externally-introduced broadening of linewidth $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{SD}}}}}}}$$ Γ SD by combining experimental size-distribution histogram with size-dependent photoluminescence-wavelength (PL- $${{{{{\boldsymbol{\lambda }}}}}}$$ λ ) curve. We develop a semi-empirical method to estimate the other three contributions to the experimentally-measured full-width at half-maximum, $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{EXP}}}}}}}$$ Γ EXP . Namely: the intrinsic linewidth $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{LO}}}}}}}$$ Γ LO caused by exciton-longitudinal optical (LO) phonon Fröhlich coupling; the inhomogeneous linewidth $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{o}}}}}}}$$ Γ o caused by imperfections-related scattering, and the broadening $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{QC}}}}}}}$$ Γ QC due to the quantum-confinement effect. We show that $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{LO}}}}}}}$$ Γ LO of a nanocrystal decreases together with the particle size, disappearing at 1.6 nm radius. Finally, we show that $${{{{{{\boldsymbol{\Gamma }}}}}}}_{{{{{{\bf{LO}}}}}}}$$ Γ LO is correlated with the degree of Fröhlich-polaron formation, hence proportional to the long-range LO-phonon-electron coupling.https://doi.org/10.1038/s42005-023-01459-8 |
| spellingShingle | Hyun Myung Jang Song Hee Lee Kyung Yeon Jang Jinwoo Park Tae-Woo Lee Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution Communications Physics |
| title | Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution |
| title_full | Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution |
| title_fullStr | Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution |
| title_full_unstemmed | Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution |
| title_short | Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution |
| title_sort | semi empirical approach to assess externally induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle size distribution |
| url | https://doi.org/10.1038/s42005-023-01459-8 |
| work_keys_str_mv | AT hyunmyungjang semiempiricalapproachtoassessexternallyinducedphotoluminescencelinewidthbroadeningofhalideperovskitenanocrystalswithparticlesizedistribution AT songheelee semiempiricalapproachtoassessexternallyinducedphotoluminescencelinewidthbroadeningofhalideperovskitenanocrystalswithparticlesizedistribution AT kyungyeonjang semiempiricalapproachtoassessexternallyinducedphotoluminescencelinewidthbroadeningofhalideperovskitenanocrystalswithparticlesizedistribution AT jinwoopark semiempiricalapproachtoassessexternallyinducedphotoluminescencelinewidthbroadeningofhalideperovskitenanocrystalswithparticlesizedistribution AT taewoolee semiempiricalapproachtoassessexternallyinducedphotoluminescencelinewidthbroadeningofhalideperovskitenanocrystalswithparticlesizedistribution |