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

Abstract

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.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Washington, Seattle, WA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1545224
Alternate Identifier(s):
OSTI ID: 1712697
Grant/Contract Number:  
AC05-00OR22725; SC0013957
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 3; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 14 SOLAR ENERGY; layered perovskites; time-resolved electrostatic force microscopy; G-Mode; Kelvin probe force microscopy; big data microscopy; Ruddlesden−Popper; layered perovskites time-resolved electrostatic force microscopy G-Mode Kelvin probe force microscopy big data microscopy Ruddlesden−Popper

Citation Formats

Giridharagopal, Rajiv, Precht, Jake T., Jariwala, Sarthak, Collins, Liam F., Jesse, Stephen, Kalinin, Sergei V., and Ginger, David S. Time-Resolved Electrical Scanning Probe Microscopy of Layered Perovskites Reveals Spatial Variations in Photoinduced Ionic and Electronic Carrier Motion. United States: N. p., 2019. Web. doi:10.1021/acsnano.8b08390.
Giridharagopal, Rajiv, Precht, Jake T., Jariwala, Sarthak, Collins, Liam F., Jesse, Stephen, Kalinin, Sergei V., & Ginger, David S. Time-Resolved Electrical Scanning Probe Microscopy of Layered Perovskites Reveals Spatial Variations in Photoinduced Ionic and Electronic Carrier Motion. United States. https://doi.org/10.1021/acsnano.8b08390
Giridharagopal, Rajiv, Precht, Jake T., Jariwala, Sarthak, Collins, Liam F., Jesse, Stephen, Kalinin, Sergei V., and Ginger, David S. Wed . "Time-Resolved Electrical Scanning Probe Microscopy of Layered Perovskites Reveals Spatial Variations in Photoinduced Ionic and Electronic Carrier Motion". United States. https://doi.org/10.1021/acsnano.8b08390. https://www.osti.gov/servlets/purl/1545224.
@article{osti_1545224,
title = {Time-Resolved Electrical Scanning Probe Microscopy of Layered Perovskites Reveals Spatial Variations in Photoinduced Ionic and Electronic Carrier Motion},
author = {Giridharagopal, Rajiv and Precht, Jake T. and Jariwala, Sarthak and Collins, Liam F. and Jesse, Stephen and Kalinin, Sergei V. and Ginger, David S.},
abstractNote = {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.},
doi = {10.1021/acsnano.8b08390},
journal = {ACS Nano},
number = 3,
volume = 13,
place = {United States},
year = {Wed Feb 06 00:00:00 EST 2019},
month = {Wed Feb 06 00:00:00 EST 2019}
}

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