“…37 ■ ASSOCIATED CONTENT * sı Supporting InformationThe Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaem.1c03247.Evolution of solar cell parameters with increasing annealing temperature; log J−V plots of a new, degraded, and annealed CZTSSe device fitted with the two-diode model; HAADF-STEM cross section images of CZTSSe lamellae at RT and 225 °C; peak fitting of the Raman spectra with a box plot of the B mode Raman peak height; peak fitting of PL spectra; bandgap value extraction of CZTSSe absorbers in the degraded and annealed solar cells; device simulation parameters (PDF) Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Newcastle upon Tyne NE1 8ST, United Kingdom; orcid.org/0000-0002-0098-4420; Email: neil.beattie@northumbria.ac.uk Yongtao Qu − Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Newcastle upon Tyne NE1 8ST, United Kingdom; Email: y.qu@ northumbria.ac.uk Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Newcastle upon Tyne NE1 8ST, United Kingdom Martial Duchamp − Laboratory for In Situ and Operando Electron Nanoscopy, School of Materials Science and Engineering, Nanyang Technological University, 637371, Singapore; orcid.org/0000-0003-2105-3059 Bethan Ford − Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Newcastle upon Tyne NE1 8ST, United Kingdom Michael Jones − Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Newcastle upon Tyne NE1 8ST, United Kingdom Linh Lan Nguyen − Laboratory for In Situ and Operando Electron Nanoscopy, School of Materials Science and Engineering, Nanyang Technological University, 637371, Singapore Matthew C. Naylor − Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Newcastle upon Tyne NE1 8ST, United Kingdom…”