A Facile Process for Partial Ag Substitution in Kesterite Cu<sub>2</sub>ZnSn(S,Se)<sub>4</sub> Solar Cells Enabling a Device Efficiency of over 12%

Myeng Gil Gang, Vijay C. Karade, Mahesh P. Suryawanshi, Hyesun Yoo, Mingrui He, Xiaojing Hao, In Jae Lee, Byeong Hoon Lee, Seung Wook Shin, Jin Hyeok Kim

ACS Applied Materials & Interfaces · 2021 · 74 citations · 64 references

Concepts

TL;DR

Cation substitution in Cu₂ZnSn(S,Se)₄ can reduce the open‑circuit voltage deficit by modifying band‑tail states, antisite defects, and related defect clusters. The authors introduce a simple single‑step process that deposits a thin Ag layer on a metallic precursor to enhance the performance of (Agₓ,Cu₁₋ₓ)₂ZnSn(Sᵧ,Se₁₋ᵧ)₄ kesterite solar cells. This approach improves band‑tailing, extends minority carrier lifetime, improves diode factors, and reduces antisite defects and defect clusters compared to the parent CZTSSe material. The resulting ACZTSSe device achieved a 12.07 % efficiency with a record 561 mV Voc‑deficit, demonstrating that the thin Ag layer effectively suppresses defects and band‑tailing to lower the Voc‑deficit.

Abstract

A cation substitution in Cu2ZnSn(S,Se)4 (CZTSSe) offers a viable strategy to reduce the open-circuit voltage (Voc)-deficit by altering the characteristics of band-tail states, antisite defects, and related defect clusters. Herein, we report a facile single process, i.e., simply introducing a thin Ag layer on a metallic precursor, to effectively improve the device characteristics and performances in kesterite (Agx,Cu1–x)2ZnSn(Sy,Se1–y)4 (ACZTSSe) solar cells. Probing into the relationship between the external quantum efficiency derivative (dEQE/dλ) and device performances revealed the Voc-deficit characteristics in the ACZTSSe solar cells as a function of Cu and Ag contents. The fabricated champion ACZTSSe solar cell device showed an efficiency of 12.07% and a record low Voc-deficit of 561 mV. Thorough investigations into the mechanism underpinning the improved performance in the ACZTSSe device further revealed the improved band-tailing characteristic, effective minority carrier lifetime, and diode factors as well as reduced antisite defects and related defect clusters as compared to the CZTSSe device. This study demonstrates the feasibility of effectively suppressing antisite defects, related defect clusters, and band-tailing characteristics by simply introducing a thin Ag layer on a metallic precursor in the kesterite solar cells, which in turn effectively reduces the Voc-deficit.

References

64