Zhu, Xi and Su, Haibin and Marcus, Rudolph A. and Michel-Beyerle, Maria E. (2014) Computed and Experimental Absorption Spectra of the Perovskite CH_3NH_3PbI_3. Journal of Physical Chemistry Letters, 5 (17). pp. 3061-3065. ISSN 1948-7185. doi:10.1021/jz501174e. https://resolver.caltech.edu/CaltechAUTHORS:20141007-153655799
Full text is not posted in this repository. Consult Related URLs below.
Use this Persistent URL to link to this item: https://resolver.caltech.edu/CaltechAUTHORS:20141007-153655799
Abstract
Electronic structure and light absorption properties of the perovskite CH_3NH_3PbI_3 are investigated by relativistic density functional theory with quasiparticle GW corrections and many-body interactions. The nature of the Wannier exciton is studied by solving the Bethe–Salpeter equation augmented with the analysis of a conceptual hydrogen-like model. The computed absorption spectrum unravels a remarkable absorption “gap” between the first two absorption peaks. This discontinuity is maintained in the calculated tetragonal structure that, however, is not stable at low temperature. Most importantly, the discontinuity is also observed in the experimental absorption spectrum of the orthorhombic single crystal at low temperature (4 K). However, in contrast to the single crystal, in a polycrystalline perovskite film at 5 K the “gap” is filled by a monotonously increasing absorption throughout the visible range. This feature of thin films points to the potential significance of defect absorption for the excellent light harvesting properties of perovskite-based solar cells.
Item Type: | Article | ||||||||
---|---|---|---|---|---|---|---|---|---|
Related URLs: |
| ||||||||
ORCID: |
| ||||||||
Alternate Title: | Computed and Experimental Absorption Spectra of the Perovskite CH3NH3PbI3 | ||||||||
Additional Information: | © 2014 American Chemical Society. Received: June 9, 2014; Accepted: August 22, 2014; Published: August 22, 2014. We are deeply indebted to Professor Teruya Ishihara for helpful comments on perovskite optical properties and for the agreement to use his absorption spectrum. H.B.S. gratefully acknowledges the access to the High Performance Computing Center at NTU. R.A.M. thanks the ONR and ARO for their support. M.E.M.B. is grateful to the Nanyang Technical University for supporting the Biophysics Center. | ||||||||
Funders: |
| ||||||||
Issue or Number: | 17 | ||||||||
DOI: | 10.1021/jz501174e | ||||||||
Record Number: | CaltechAUTHORS:20141007-153655799 | ||||||||
Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20141007-153655799 | ||||||||
Official Citation: | Computed and Experimental Absorption Spectra of the Perovskite CH3NH3PbI3 Xi Zhu, Haibin Su, Rudolph A. Marcus, and Maria E. Michel-Beyerle The Journal of Physical Chemistry Letters 2014 5 (17), 3061-3065 | ||||||||
Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||
ID Code: | 50245 | ||||||||
Collection: | CaltechAUTHORS | ||||||||
Deposited By: | Tony Diaz | ||||||||
Deposited On: | 09 Oct 2014 21:46 | ||||||||
Last Modified: | 10 Nov 2021 18:53 |
Repository Staff Only: item control page