Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes

Hong Chen; Jia Lin; Joohoon Kang; Qiao Kong; Dylan Lu; Jun Kang; Minliang Lai; Li Na Quan; Zhenni Lin; Jianbo Jin; Lin-Wang Wang; Michael F Toney; Peidong Yang

doi:10.1126/sciadv.aay4045

Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes

Sci Adv. 2020 Jan 24;6(4):eaay4045. doi: 10.1126/sciadv.aay4045. eCollection 2020 Jan.

Authors

Hong Chen^{1

2

3}, Jia Lin^{1

4}, Joohoon Kang^{1

5

6

7

8}, Qiao Kong¹, Dylan Lu¹, Jun Kang⁹, Minliang Lai¹, Li Na Quan^{1

9}, Zhenni Lin^{9

10}, Jianbo Jin¹, Lin-Wang Wang⁹, Michael F Toney², Peidong Yang^{1

7

9

10}

Affiliations

¹ Department of Chemistry, University of California, Berkeley, Berkeley, CA, USA.
² Stanford Synchrotron Radiation Light Source, SLAC National Accelerator Laboratory, Stanford University, Menlo Park, CA, USA.
³ School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong, China.
⁴ Department of Physics, Shanghai University of Electric Power, Shanghai, China.
⁵ Center for Nanomedicine, Institute for Basic Science (IBS), Seoul, South Korea.
⁶ Y-IBS Institute, Yonsei University, Seoul, South Korea.
⁷ Kavli Energy NanoScience Institute, Berkeley, CA, USA.
⁸ School of Advanced Materials Science and Engineering, Sungkyunkwan University (SKKU), Suwon, South Korea.
⁹ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
¹⁰ Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, CA, USA.

Abstract

Achieving perovskite-based high-color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high-color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate temperature-induced device degradation by investigating the crystal structural and spectral evolution dynamics via in situ temperature-dependent single-crystal x-ray diffraction, photoluminescence (PL) characterization, and density functional theory calculation. The PL peak becomes asymmetrically broadened with a marked intensity decay, as temperature increases owing to [PbBr₆]^4- octahedra tilting and the organic chain disordering, which results in bandgap decrease. This study indicates that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.

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