Hot-carrier cooling and photoinduced refractive index changes in organic–inorganic lead halide perovskites
Open accessAbstract
Metal-halide perovskites are at the frontier of optoelectronic research due to solution processability and excellent semiconductor properties. Here we use transient absorption spectroscopy to study hot-carrier distributions in CH 3 NH 3 PbI 3 and quantify key semiconductor parameters. Above bandgap, non-resonant excitation creates quasi-thermalized carrier distributions within 100 fs. During carrier cooling, a sub-bandgap transient absorption signal arises at ∼1.6 eV, which is explained by the interplay of bandgap renormalization and hot-carrier distributions. At higher excitation densities, a ‘phonon bottleneck’ substantially slows carrier cooling. This effect indicates a low contribution from inelastic carrier-impurity or phonon–impurity scattering in these polycrystalline materials, which supports high charge-carrier mobilities. Photoinduced reflectivity changes distort the shape of transient absorption spectra and must be included to extract physical constants. Using a simple band-filling model that accounts for these changes, we determine a small effective mass of m r =0.14 m o , which agrees with band structure calculations and high photovoltaic performance.
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The strong reduction of absorption at energies close to the bandgap induces a significant reduction of the real part of the refractive index, causing blue shifting of the resonant modes.
“the strong reduction of absorption at energies close to the bandgap where the laser is operating induces a significant reduction of the real part of the refractive index, 40 causing blue shifting of the resonant modes.”
From Monolithically Integrated Perovskite Semiconductor Lasers on Silicon Photonic Chips by Scalable Top-Down Fabrication (2018) · cites this paper as [40]
In Results, ‘Photoinduced reflection due to refractive index changes’ (page unavailable), the paper models a carrier-induced change in absorption that produces a refractive-index change through a Kramers–Kronig transformation, and reports significant photoinduced reflectivity changes. It does not establish that the real part of the index decreases at the laser energy or that this causes resonant modes to blue-shift. (LLM, conf=0.82)
Experimental — accuracy not yet measuredThe refractive index is coupled to absorption through the Kramers-Kronig relation.
“The refractive index is coupled to the absorption through the Kramers-Kronig relation:”
From Monolithically Integrated Perovskite Semiconductor Lasers on Silicon Photonic Chips by Scalable Top-Down Fabrication (2018) · cites this paper as [40]
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- Authors
- Price, M. B., Butkus, J., Jellicoe, T. C., Sadhanala, A., Briane, A., Halpert, J. E., Broch, K., Hodgkiss, J. M., Friend, R. H., & Deschler, F.
- Affiliations
- University of Cambridge (GB)
- Victoria University of Wellington (NZ)
- Corresponding author
- Deschler, Felix
- ORCID
- Venue
- Nature Communications
- Published
- 2015-09-25
- Volume
- 6
- Issue
- 1
- Pages
- 8420-8420
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC4598728
- OpenAlex
- W2233449626
- Cited by
- 704
- References
- 42
- Citations by year
- 2026: 58 · 2025: 49 · 2024: 69 · 2023: 84 · 2022: 59 · 2021: 66 · 2020: 75 · 2019: 74 · 2018: 65 · 2017: 61 · 2016: 40 · 2015: 4
- FWCI
- 27.28
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Nature Communications (publishedVersion, cc-by)
- Europe PMC (PubMed Central) (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- Rare & Special e-Zone (The Hong Kong University of Science and Technology) (submittedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- Apollo (University of Cambridge) (submittedVersion, cc-by)
- Funders
- Deutsche Forschungsgemeinschaft
- Cambridge Commonwealth Trust
- Engineering and Physical Sciences Research Council (EP/M005143/1, EP/G060738/1)
- Marsden Fund
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Perovskite Materials and Applications
- Physical Sciences › Materials Science › Materials Chemistry › 2D Materials and Applications
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Organic Electronics and Photovoltaics
- Keywords
- hot carrier cooling, organic-inorganic lead halide perovskites, methylammonium lead iodide, photoinduced refractive index change, transient absorption spectroscopy, band gap renormalization, phonon bottleneck, effective mass, carrier mobility, polycrystalline perovskite
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