4.6 Article

Probing Carrier Transport in Layered Perovskites with Nonlinear Optical and Photocurrent Spectroscopies

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume 125, Issue 15, Pages 8021-8030

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c00654

Keywords

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Funding

  1. National Science Foundation [CHE-1763207]
  2. UNC Research Opportunities Initiative (ROI) through the Center of Hybrid Materials Enabled Electronic Technology
  3. Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES)

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Layered perovskite quantum wells show potential for optoelectronic devices, with gradients in quantum well concentrations promoting funneling of electronic excitations and charge carriers. However, experiments suggest that charge carrier funneling processes do not facilitate long-range transport due to trapping, with bulklike phases of films transporting carriers without involvement of the smallest quantum wells.
Interest in layered perovskite quantum wells is motivated by their potential for use in optoelectronic devices. In these systems, the smallest and largest quantum wells are most concentrated near opposing electrodes in photovoltaic cells. Coincident gradients in the energy levels and quantum well concentrations promote the funneling of electronic excitations and charge carriers through space. In this Perspective, we describe the development of several nonlinear optical techniques designed to elucidate the relaxation processes induced by light absorption in layered perovskite systems. Transient absorption microscopy provides insight into carrier diffusion and two-body recombination processes, whereas two-dimensional action spectroscopies are used to correlate elementary relaxation mechanisms to practical metrics of photovoltaic device performance. Our experiments suggest that charge carrier funneling processes do not facilitate long-range transport due to trapping. Rather, the bulklike phases of the films absorb light and transport carriers without participation of the smallest quantum wells.

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