Time-Resolved Electrical Scanning Probe Microscopy of Layered Perovskites Reveals Spatial Variations in Photoinduced Ionic and Electronic Carrier Motion

Giridharagopal, Rajiv; Precht, Jake T.; Jariwala, Sarthak; Collins, Liam F.; Jesse, Stephen; Kalinin, Sergei V.; Ginger, David S.

doi:10.1021/acsnano.8b08390

Title: Time-Resolved Electrical Scanning Probe Microscopy of Layered Perovskites Reveals Spatial Variations in Photoinduced Ionic and Electronic Carrier Motion

Journal Article · Wed Feb 06 00:00:00 EST 2019 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.8b08390· OSTI ID:1545224

^[1]; Precht, Jake T. ^[1]; Jariwala, Sarthak ^[1];

^[2];

^[1]

Univ. of Washington, Seattle, WA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

We study light-induced dynamics in thin films comprising Ruddlesden–Popper phases of the layered 2D perovskite (C4H9NH3)2PbI4. We probe ionic and electronic carrier dynamics using two complementary scanning probe methods, time-resolved G-mode Kelvin probe force microscopy and fast free time-resolved electrostatic force microscopy, as a function of position, time, and illumination. We show that the average surface photovoltage sign is dominated by the band bending at the buried perovskite–substrate interface. However, the film exhibits substantial variations in the spatial and temporal response of the photovoltage. Under illumination, the photovoltage equilibrates over hundreds of microseconds, a time scale associated with ionic motion and trapped electronic carriers. Surprisingly, we observe that the surface photovoltage of the 2D grain centers evolves more rapidly in time than at the grain boundaries. We propose that the slower evolution at grain boundaries is due to a combination of ion migration occurring between PbI4 planes, as well as electronic carriers traversing grain boundary traps, thereby changing the time-dependent band unbending at grain boundaries. These results provide a model for the photoinduced dynamics in 2D perovskites and are a useful basis for interpreting photovoltage dynamics on hybrid 2D/3D structures.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0013957

OSTI ID:: 1545224

Alternate ID(s):: OSTI ID: 1712697

Journal Information:: ACS Nano, Vol. 13, Issue 3; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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Title: Time-Resolved Electrical Scanning Probe Microscopy of Layered Perovskites Reveals Spatial Variations in Photoinduced Ionic and Electronic Carrier Motion

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