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Spatial-temporal spectroscopy characterizations and electronic structure of methylammonium perovskites

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Abstract

Using time-resolved laser-scanning confocal microscopy and ultrafast optical pump/THz probe spectroscopy, we measure photoluminescence (PL) and THz-conductivity in perovskite micro-crystals and films. PL quenching and lifetime variations occur from local heterogeneity. Ultrafast THz-spectra measure sharp quantum transitions from excitonic Rydberg states, providing weakly bound excitons with a binding energy of ~13.5 meV at low temperatures. Ab-initio electronic structure calculations give a direct band gap of 1.64 eV, a dielectric constant of ~18, heavy electrons, and light holes, resulting in weakly bound excitons, consistent with the binding energies from the experiment. The complementary spectroscopy and simulations reveal fundamental insights into perovskite light-matter interactions.

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Acknowledgment

This paper was supported in part (R.B., L.L., Z.L., D.C., J.M., J. S., J.W.) by the US DOE Office of Science, Basic Energy Sciences, Materials Science and Engineering Division. Ames Laboratory is operated for the US DOE by Iowa State University under Contract No. DE-AC02-07CH11358. The research used resources at the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the US DOE under Contract No. DE-AC02-05CH11231. KCB acknowledges DST for providing him financial support through SERB-NPDF through Letter No. PDF/2017/002876. The authors also acknowledge the computing resources provided by the Inter-University Accelerator Center, New Delhi.

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Authors and Affiliations

  1. Division of Materials Science and Engineering, Ames Laboratory, Ames, IA, 50011, USA

    Zhaoyu Liu, Liang Luo, Joong-Mok Park, Di Cheng, Rana Biswas & F. Fungara

  2. Department of Physics and Astronomy, Iowa State University, Ames, Iowa, 50011, USA

    Zhaoyu Liu, Liang Luo, Di Cheng, F. Fungara, Joseph Shinar & Jigang Wang

  3. CSIR-National Chemical Laboratory, Pune, 411008, Maharashtra, India

    K. C. Bhamu

  4. Department of Electrical and Computer Engineering and Microelectronics Research Center, Iowa State University, Ames, IA, 50011, USA

    Satvik Shah & Ruth Shinar

  5. Division of Chemical and Biological Sciences, Ames Laboratory, Ames, IA, 50011, USA

    Men Long & Javier Vela

  6. Department of Chemistry, Iowa State University, Ames, Iowa, 50011, USA

    Men Long & Javier Vela

  7. Division of Materials Science and Engineering, Ames Laboratory, Ames, IA, 50011, USA

    Joseph Shinar & Jigang Wang

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  1. Zhaoyu Liu
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Correspondence to Rana Biswas or Jigang Wang.

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These authors contributed equally to this work.

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Liu, Z., Bhamu, K.C., Luo, L. et al. Spatial-temporal spectroscopy characterizations and electronic structure of methylammonium perovskites. MRS Communications 8, 961–969 (2018). https://doi.org/10.1557/mrc.2018.114

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