Resolving Enhanced Mn2+ Luminescence near the Surface of CsPbCl3 with Time-Resolved Cathodoluminescence Imaging

Wai, Rebecca B.; Ramesh, Namrata; Aiello, Clarice D.; Raybin, Jonathan G.; Zeltmann, Steven E.; Bischak, Connor G.; Barnard, Edward; Aloni, Shaul; Ogletree, D. Frank; Minor, Andrew M.; Ginsberg, Naomi S.

doi:10.1021/acs.jpclett.0c00574

Resolving Enhanced Mn²⁺ Luminescence near the Surface of CsPbCl₃ with Time-Resolved Cathodoluminescence Imaging

Journal Article · Thu Mar 19 00:00:00 EDT 2020 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.0c00574· OSTI ID:1756328

Wai, Rebecca B. ^[1]; Ramesh, Namrata ^[1]; Aiello, Clarice D. ^[1]; Raybin, Jonathan G. ^[1]; Zeltmann, Steven E. ^[1]; ^[2]; Barnard, Edward ^[3]; Aloni, Shaul ^[3]; Ogletree, D. Frank ^[3]; Minor, Andrew M. ^[4]; ^[5]

Univ. of California, Berkeley, CA (United States); STROBE NSF Science & Technology Center, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; STROBE NSF Science & Technology Center, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); STROBE NSF Science & Technology Center, Berkeley, CA (United States)

Mn²⁺ doping of lead halide perovskites has garnered recent interest because it produces stable orange luminescence in tandem with perovskite emission. In this work, we observe enhanced Mn²⁺ luminescence at the edges of Mn²⁺-doped CsPbCl₃ perovskite microplates and suggest an explanation for its origin using the high spatiotemporal resolution of time-resolved cathodoluminescence (TRCL) imaging. We reveal two luminescent decay components that we attribute to two different Mn²⁺ populations. While each component appears to be present both near the surface and in the bulk, the origin of the intensity variation stems from a higher proportion of the longer lifetime component near the perovskite surface. Overall, we suggest that this higher emission is caused by an increased probability of electron-hole recombination on Mn²⁺ near the perovskite surface due to an increased trap concentration there. This observation suggests that such surface features have yet untapped potential to enhance emissive properties via control of surface-to-volume ratio.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Photonics at Thermodynamic Limits (PTL); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0019140

OSTI ID:: 1756328

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 7 Vol. 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Resolving Enhanced Mn2+ Luminescence near the Surface of CsPbCl3 with Time-Resolved Cathodoluminescence Imaging

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Resolving Enhanced Mn²⁺ Luminescence near the Surface of CsPbCl₃ with Time-Resolved Cathodoluminescence Imaging