Band Tailing and Deep Defect States in CH3NH3Pb(I1–xBrx)3 Perovskites As Revealed by Sub-Bandgap Photocurrent

Sutter-Fella, Carolin M.; Miller, D. Westley; Ngo, Quynh P.; Roe, Ellis T.; Toma, Francesca M.; Sharp, Ian D.; Lonergan, Mark C.; Javey, Ali

doi:10.1021/acsenergylett.6b00727

Title: Band Tailing and Deep Defect States in CH₃NH₃Pb(I_1–xBr_x)₃ Perovskites As Revealed by Sub-Bandgap Photocurrent

Journal Article · 15 February 2017 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.6b00727 · OSTI ID:1379750

^[1]; Miller, D. Westley ^[2]; Ngo, Quynh P. ^[1]; Roe, Ellis T. ^[2]; Toma, Francesca M. ^[3];

^[3]; Lonergan, Mark C. ^[2]; Javey, Ali ^[1]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of Oregon, Eugene, OR (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Organometal halide perovskite semiconductors have emerged as promising candidates for optoelectronic applications because of the outstanding charge carrier transport properties, achieved with low-temperature synthesis. In this paper, we present highly sensitive sub-bandgap external quantum efficiency (EQE) measurements of Au/spiro-OMeTAD/CH₃NH₃Pb(I_1–xBr_x)₃/TiO₂/FTO/glass photovoltaic devices. The room-temperature spectra show exponential band tails with a sharp onset characterized by low Urbach energies (E_u) over the full halide composition space. The Urbach energies are 15–23 meV, lower than those for most semiconductors with similar bandgaps (especially with E_g > 1.9 eV). Intentional aging of CH₃NH₃Pb(I_1–xBr_x)₃ for up to 2300 h, reveals no change in E_u, despite the appearance of the PbI₂ phase due to decomposition, and confirms a high degree of crystal ordering. Moreover, sub-bandgap EQE measurements reveal an extended band of sub-bandgap electronic states that can be fit with one or two point defects for pure CH₃NH₃PbI₃ or mixed CH₃NH₃Pb(I_1–xBr_x)₃ compositions, respectively. Finally, the study provides experimental evidence of defect states close to the midgap that could impact photocarrier recombination and energy conversion efficiency in higher bandgap CH₃NH₃Pb(I_1–xBr_x)₃ alloys.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); LBNL Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC02-05CH11231; SC0012363

OSTI ID:: 1379750

Journal Information:: ACS Energy Letters, Vol. 2, Issue 3; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Band Tailing and Deep Defect States in CH3NH3Pb(I1–xBrx)3 Perovskites As Revealed by Sub-Bandgap Photocurrent

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Title: Band Tailing and Deep Defect States in CH₃NH₃Pb(I_1–xBr_x)₃ Perovskites As Revealed by Sub-Bandgap Photocurrent