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

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 [PbBr 6] 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.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [4];  [5];  [4]; ORCiD logo [6];  [7]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [8]; ORCiD logo [9]
  1. Univ. of California, Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Southern Univ. of Science and Technology, Shenzhen, Guangdong (China)
  2. Univ. of California, Berkeley, CA (United States); Shanghai Univ. of Electric Power (China)
  3. Univ. of California, Berkeley, CA (United States); Inst. for Basic Science (IBS), Seoul (South Korea); Yonsei Univ., Seoul (South Korea); Kavli Energy NanoScience Inst., Berkeley, CA (United States); Sungkyunkwan Univ. (SKKU), Suwon (South Korea)
  4. Univ. of California, Berkeley, CA (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  9. Univ. of California, Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Science & Engineering Division; USDOE Office of Science (SC)
OSTI Identifier:
1599850
Alternate Identifier(s):
OSTI ID: 1604562
Grant/Contract Number:  
[AC02-05CH11231; AC02-76SF00515; AC36-08G028308]
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
[ Journal Volume: 6; Journal Issue: 4]; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Chen, Hong, Lin, Jia, Kang, Joohoon, Kong, Qiao, Lu, Dylan, Kang, Jun, Lai, Minliang, Quan, Li Na, Lin, Zhenni, Jin, Jianbo, Wang, Lin-wang, Toney, Michael F., and Yang, Peidong. Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes. United States: N. p., 2020. Web. doi:10.1126/sciadv.aay4045.
Chen, Hong, Lin, Jia, Kang, Joohoon, Kong, Qiao, Lu, Dylan, Kang, Jun, Lai, Minliang, Quan, Li Na, Lin, Zhenni, Jin, Jianbo, Wang, Lin-wang, Toney, Michael F., & Yang, Peidong. Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes. United States. doi:10.1126/sciadv.aay4045.
Chen, Hong, Lin, Jia, Kang, Joohoon, Kong, Qiao, Lu, Dylan, Kang, Jun, Lai, Minliang, Quan, Li Na, Lin, Zhenni, Jin, Jianbo, Wang, Lin-wang, Toney, Michael F., and Yang, Peidong. Wed . "Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes". United States. doi:10.1126/sciadv.aay4045. https://www.osti.gov/servlets/purl/1599850.
@article{osti_1599850,
title = {Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes},
author = {Chen, Hong and Lin, Jia and Kang, Joohoon and Kong, Qiao and Lu, Dylan and Kang, Jun and Lai, Minliang and Quan, Li Na and Lin, Zhenni and Jin, Jianbo and Wang, Lin-wang and Toney, Michael F. and Yang, Peidong},
abstractNote = {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.},
doi = {10.1126/sciadv.aay4045},
journal = {Science Advances},
number = [4],
volume = [6],
place = {United States},
year = {2020},
month = {1}
}

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