n-type kesterite thermoelectric (Cu1−xAgx)2ZnSnS4 single crystals exceeding dimensionless figure of merit value of 1.0

The lack of attractive n-type thermoelectric materials greatly restricts their applications because most high-performance materials are p-type conductors, such as the kesterite compound Cu2ZnSnS4. This study reports high-quality n-type kesterite (Cu1−xAgx)2ZnSnS4 (CAZTS) single crystals that exhibit a record high dimensionless figure of merit value of 1.1 at approximately 800 K, primarily owing to Ag alloying, cation compositional optimization, and intrinsic low thermal conductivity. An n-type CAZTS-based single-leg device was fabricated using a Mo-barrier layer. The device exhibited a thermoelectric conversion efficiency of 3.4% at a temperature gradient of 473 K. This study provides insights into developing thermoelectric modules using environmentally friendly kesterite materials.