Upper limit to the photovoltaic efficiency of imperfect crystals from first principles

Sunghyun Kim, José A. Márquez, Thomas Unold, Aron Walsh

Research output: Contribution to journalArticlepeer-review

71 Citations (Scopus)


The Shockley-Queisser (SQ) limit provides a convenient metric for predicting light-to-electricity conversion efficiency of a solar cell based on the band gap of the light-absorbing layer. In reality, few materials approach this radiative limit. We develop a formalism and computational method to predict the maximum photovoltaic efficiency of imperfect crystals from first principles. The trap-limited conversion efficiency includes equilibrium populations of native defects, their carrier-capture coefficients, and the associated recombination rates. When applied to kesterite solar cells, we reveal an intrinsic limit of 20% for Cu2ZnSnSe4, which falls far below the SQ limit of 32%. The effects of atomic substitution and extrinsic doping are studied, leading to pathways for an enhanced efficiency of 31%. This approach can be applied to support targeted-materials selection for future solar-energy technologies.

Original languageEnglish
Pages (from-to)1481-1491
Number of pages11
JournalEnergy and Environmental Science
Issue number5
Publication statusPublished - 2020

Bibliographical note

Funding Information:
We thank Samantha N. Hood, John Buckeridge, and Ji-Sang Park for valuable discussions. This research has been funded by the EU Horizon2020 Framework (STARCELL, Grant No. 720907). We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1). Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202), this work used the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk). This work was also supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (No. 2018R1C1B6008728).

Publisher Copyright:
© The Royal Society 2020 of Chemistry.

All Science Journal Classification (ASJC) codes

  • Environmental Chemistry
  • Renewable Energy, Sustainability and the Environment
  • Nuclear Energy and Engineering
  • Pollution


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