Phase engineering approach for efficient wide-bandgap perovskite solar cells via regulation of perovskite precursor-solvent coordination

Sudhir Ranjan^a, Saurabh Srivastava^b, Anand Singh^c^,^d, Ashish Garg^d^,^e, Raju Kumar Gupta^a^,^d^,^e^,^f

^aDepartment of Chemical Engineering, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh, India

^bDepartment of Materials Science and Engineering, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh, India

^cDepartment of Chemistry, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh, India

^dDepartment of Sustainable Energy Engineering, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh, India

^eChandrakanta Kesavan Centre for Energy Policy and Climate Solutions, Indian Institute of Technology Kanpur, Uttar Pradesh, India

^fCentre for Environmental Science and Engineering, Indian Institute of Technology Kanpur, Uttar Pradesh, India

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)

#PeroMAT- Halide perovskite and perovskite- inspired materials: synthesis and applications

Lausanne, Switzerland, 2024 November 12th - 15th

Organizers: Raquel Galian, Lakshminarayana Polavarapu and Paola Vivo

Poster, Sudhir Ranjan, 384
Publication date: 28th August 2024

Recently, use of wide-bandgap perovskites (WBG) as absorber layer in top cell of tandem solar cells has offered tremendous promise for achieving power conversion efficiencies (PCEs) that can break theoretical limit of the single-junction solar cells. However, use of polar aprotic solvents such DMSO/DMF for perovskite precursors imbalances nucleation-growth kinetics owing to their strong mutual coordination, resulting in formation of complex intermediate phases. This generates in-situ stacking defects, leading to significant open-circuit voltage (Voc) deficit in WBG perovskite solar cells (PSCs). Recently, volatile ammonium chloride (NH₄Cl) has been used as co-additive to address issue of voltage loss in WBG PSCs. However, its sole effect on precursor phase, crystallization kinetics and phase-transition mechanism in WBG perovskites still needs to be investigated. This study elucidates critical role of NH₄Cl in weakening perovskite precursor-solvent coordination for destabilizing undesired intermediate hexagonal polytypes. In-situ characterizations revealed beneficial role of NH₄Cl in facilitating more balanced nucleation-growth kinetics that suppressed undesired intermediate phase formation and induced accelerated phase transition from 2H/4H phase to desirable cubic perovskite phase together with self-elimination of defects during crystallization. Improved crystallization dynamics favored the formation of high-quality perovskite films with better halide homogeneity and improved structural and optoelectronic properties. Consequently, this strategy led to 1.73 eV WBG perovskite solar cells achieving impressive PCE of ~19% with open circuit voltage (V_oc) of 1.22 V, complimented with suppressed halide segregation for better photostability.

Keywords: Photovoltaics, crystallization, halide homogenization, wide-bandgap perovskites, phase engineering,

References:

[1] Oliver, R.D., et al., Understanding and suppressing non-radiative losses in methylammonium-free wide-bandgap perovskite solar cells. Energy & Environmental Science, 2022. 15(2): p. 714-726

[2] Hang, P., et al., Highly efficient and stable wide‐bandgap perovskite solar cells via strain management. Advanced Functional Materials, 2023. 33(11): p. 2214381.

Acknowledgements:

Authors thank financial support from Department of Science and Technology (DST), India through Grant No. DST/TMD/CERI/C140(G) under Clean Energy Research Initiative, Science and Engineering Research Board (SERB), India through Grant No. IPA/2021/000096, IPA/2021/000031, SPR/2021/000700, and UKRI Global Challenge Research Fund through project SUNRISE (EP/P032591/1).

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