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Title: Enhancing ferroelectric photovoltaic effect by polar order engineering

Ferroelectric materials for photovoltaics have sparked great interest because of their switchable photoelectric responses and above-bandgap photovoltages that violate conventional photovoltaic theory. However, their relatively low photocurrent and power conversion efficiency limit their potential application in solar cells. To improve performance, conventional strategies focus mainly on narrowing the bandgap to better match the solar spectrum, leaving the fundamental connection between polar order and photovoltaic effect largely overlooked. We report large photovoltaic enhancement by A-site substitutions in a model ferroelectric photovoltaic material, BiFeO 3. As revealed by optical measurements and supported by theoretical calculations, the enhancement is accompanied by the chemically driven rotational instability of the polarization, which, in turn, affects the charge transfer at the band edges and drives a direct-to-indirect bandgap transition, highlighting the strong coupling between polarization, lattice, and orbital order parameters in ferroelectrics. In conclusion, polar order engineering thus provides an additional degree of freedom to further boost photovoltaic efficiency in ferroelectrics and related materials.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [3] ;  [1] ; ORCiD logo [4] ;  [5] ;  [5] ;  [6] ;  [7] ;  [8] ;  [1] ; ORCiD logo [4] ; ORCiD logo [1]
  1. Nanyang Technological Univ. (Singapore)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Soochow Univ., Suzhou (China)
  4. Univ. of Pennsylvania, Philadelphia, PA (United States)
  5. Shanghai Univ., Shanghai (China)
  6. National Univ. of Singapore (Singapore); GLOBALFOUNDRIES, Albany, NY (United States)
  7. National Univ. of Singapore (Singapore)
  8. Nanyang Technological Univ. (Singapore); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Grant/Contract Number:
AC05-76RL01830; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 7; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 42 ENGINEERING
OSTI Identifier:
1471238
Alternate Identifier(s):
OSTI ID: 1478347

You, Lu, Zheng, Fan, Fang, Liang, Zhou, Yang, Tan, Liang Z., Zhang, Zeyu, Ma, Guohong, Schmidt, Daniel, Rusydi, Andrivo, Wang, Le, Chang, Lei, Rappe, Andrew M., and Wang, Junling. Enhancing ferroelectric photovoltaic effect by polar order engineering. United States: N. p., Web. doi:10.1126/sciadv.aat3438.
You, Lu, Zheng, Fan, Fang, Liang, Zhou, Yang, Tan, Liang Z., Zhang, Zeyu, Ma, Guohong, Schmidt, Daniel, Rusydi, Andrivo, Wang, Le, Chang, Lei, Rappe, Andrew M., & Wang, Junling. Enhancing ferroelectric photovoltaic effect by polar order engineering. United States. doi:10.1126/sciadv.aat3438.
You, Lu, Zheng, Fan, Fang, Liang, Zhou, Yang, Tan, Liang Z., Zhang, Zeyu, Ma, Guohong, Schmidt, Daniel, Rusydi, Andrivo, Wang, Le, Chang, Lei, Rappe, Andrew M., and Wang, Junling. 2018. "Enhancing ferroelectric photovoltaic effect by polar order engineering". United States. doi:10.1126/sciadv.aat3438. https://www.osti.gov/servlets/purl/1471238.
@article{osti_1471238,
title = {Enhancing ferroelectric photovoltaic effect by polar order engineering},
author = {You, Lu and Zheng, Fan and Fang, Liang and Zhou, Yang and Tan, Liang Z. and Zhang, Zeyu and Ma, Guohong and Schmidt, Daniel and Rusydi, Andrivo and Wang, Le and Chang, Lei and Rappe, Andrew M. and Wang, Junling},
abstractNote = {Ferroelectric materials for photovoltaics have sparked great interest because of their switchable photoelectric responses and above-bandgap photovoltages that violate conventional photovoltaic theory. However, their relatively low photocurrent and power conversion efficiency limit their potential application in solar cells. To improve performance, conventional strategies focus mainly on narrowing the bandgap to better match the solar spectrum, leaving the fundamental connection between polar order and photovoltaic effect largely overlooked. We report large photovoltaic enhancement by A-site substitutions in a model ferroelectric photovoltaic material, BiFeO3. As revealed by optical measurements and supported by theoretical calculations, the enhancement is accompanied by the chemically driven rotational instability of the polarization, which, in turn, affects the charge transfer at the band edges and drives a direct-to-indirect bandgap transition, highlighting the strong coupling between polarization, lattice, and orbital order parameters in ferroelectrics. In conclusion, polar order engineering thus provides an additional degree of freedom to further boost photovoltaic efficiency in ferroelectrics and related materials.},
doi = {10.1126/sciadv.aat3438},
journal = {Science Advances},
number = 7,
volume = 4,
place = {United States},
year = {2018},
month = {7}
}

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