Quadruple-band synglisis enables high thermoelectric efficiency in earth-abundant tin sulfide crystals

Thermoelectrics have been limited by the scarcity of their constituent elements, especially telluride. The earth-abundant, wide-bandgap (<i>E</i>_g ≈ 46 <i>k</i>_B<i>T</i>) tin sulfide (SnS) has shown promising performance in its crystal form. We improved the thermoelectric efficiency in SnS crystals by promoting the convergence of energy and momentum of four valance bands, termed quadruple-band synglisis. We introduced more Sn vacancies to activate quadruple-band synglisis and facilitate carrier transport by inducing SnS₂ in selenium (Se)-alloyed SnS, leading to a high dimensionless figure of merit (<i>ZT</i>) of ~1.0 at 300 kelvin and an average <i>ZT</i> of ~1.3 at 300 to 773 kelvin in p-type SnS crystals. We further obtained an experimental efficiency of ~6.5%, and our fabricated cooler demonstrated a maximum cooling temperature difference of ~48.4 kelvin at 353 kelvin. Our observations should draw interest to earth-abundant SnS crystals for applications of waste-heat recovery and thermoelectric cooling.