Photoinduced, reversible phase transitions in all-inorganic perovskite nanocrystals

Matthew S. Kirschner; Benjamin T. Diroll; Peijun Guo; Samantha M. Harvey; Waleed Helweh; Nathan C. Flanders; Alexandra Brumberg; Nicolas E. Watkins; Ariel A. Leonard; Austin M. Evans; Michael R. Wasielewski; William R. Dichtel; Xiaoyi Zhang; Lin X. Chen; Richard D. Schaller

doi:10.1038/s41467-019-08362-3

Photoinduced, reversible phase transitions in all-inorganic perovskite nanocrystals

Matthew S. Kirschner, Benjamin T. Diroll, Peijun Guo, Samantha M. Harvey, Waleed Helweh, Nathan C. Flanders, Alexandra Brumberg, Nicolas E. Watkins, Ariel A. Leonard, Austin M. Evans, Michael R. Wasielewski, William R. Dichtel, Xiaoyi Zhang, Lin X. Chen, Richard D. Schaller^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

131 Scopus citations

Abstract

Significant interest exists in lead trihalides that present the perovskite structure owing to their demonstrated potential in photovoltaic, lasing, and display applications. These materials are also notable for their unusual phase behavior often displaying easily accessible phase transitions. In this work, time-resolved X-ray diffraction, performed on perovskite cesium lead bromide nanocrystals, maps the lattice response to controlled excitation fluence. These nanocrystals undergo a reversible, photoinduced orthorhombic-to-cubic phase transition which is discernible at fluences greater than 0.34 mJ cm ⁻² through the loss of orthorhombic features and shifting of high-symmetry peaks. This transition recovers on the timescale of 510 ± 100 ps. A reversible crystalline-to-amorphous transition, observable through loss of Bragg diffraction intensity, occurs at higher fluences (greater than 2.5 mJ cm ⁻² ). These results demonstrate that light-driven phase transitions occur in perovskite materials, which will impact optoelectronic applications and enable the manipulation of non-equilibrium phase characteristics of the broad perovskite material class.

Original language	English (US)
Article number	504
Journal	Nature communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-08362-3
State	Published - Dec 1 2019

Funding

We acknowledge support from the Ultrafast Initiative of the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, through Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This work made use of the Jerome B. Cohen X-Ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University and the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205). Portions of this work were performed at the DuPont-Northwestern-Dow Collaborative Access Team (DND-CAT) located at Sector 5 of the Advanced Photon Source (APS). DND-CAT is supported by Northwestern University, E.I. DuPont de Nemours & Co., and The Dow Chemical Company. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. N.C.F partially supported by Basic Energy Science, CBG Division, U.S. Department of Energy and resources at the Advanced Photon Source were funded by the National Science Foundation under Award Number 0960140. This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award DE-FG02-99ER14999 (M.R.W.). This material is based upon work supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1324585 (S.M.H., A.B., A.M.E. and N.E.W.). Yingqi Wang assisted in the acquisition of TR-XRD data. Jerrold A. Carsello assisted in acquiring the temperature-dependent XRD measurements. Matthew L. Nisbet assisted with generating the crystal structure schematics.

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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10.1038/s41467-019-08362-3

Cite this

Kirschner, M. S., Diroll, B. T., Guo, P., Harvey, S. M., Helweh, W., Flanders, N. C., Brumberg, A., Watkins, N. E., Leonard, A. A., Evans, A. M., Wasielewski, M. R., Dichtel, W. R., Zhang, X., Chen, L. X., & Schaller, R. D. (2019). Photoinduced, reversible phase transitions in all-inorganic perovskite nanocrystals. Nature communications, 10(1), Article 504. https://doi.org/10.1038/s41467-019-08362-3

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N2 - Significant interest exists in lead trihalides that present the perovskite structure owing to their demonstrated potential in photovoltaic, lasing, and display applications. These materials are also notable for their unusual phase behavior often displaying easily accessible phase transitions. In this work, time-resolved X-ray diffraction, performed on perovskite cesium lead bromide nanocrystals, maps the lattice response to controlled excitation fluence. These nanocrystals undergo a reversible, photoinduced orthorhombic-to-cubic phase transition which is discernible at fluences greater than 0.34 mJ cm −2 through the loss of orthorhombic features and shifting of high-symmetry peaks. This transition recovers on the timescale of 510 ± 100 ps. A reversible crystalline-to-amorphous transition, observable through loss of Bragg diffraction intensity, occurs at higher fluences (greater than 2.5 mJ cm −2 ). These results demonstrate that light-driven phase transitions occur in perovskite materials, which will impact optoelectronic applications and enable the manipulation of non-equilibrium phase characteristics of the broad perovskite material class.

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Photoinduced, reversible phase transitions in all-inorganic perovskite nanocrystals

Abstract

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UN SDGs

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