In
thermoelectrics, the material’s performance stems from
a delicate tradeoff between atomic order and disorder. Generally,
dopants and thus atomic disorder are indispensable for optimizing
the carrier concentration and scatter short-wavelength heat-carrying
phonons. However, the strong disorder has been perceived as detrimental
to the semiconductor’s electrical conductivity owing to the
deteriorated carrier mobility. Here, we report the sustainable role
of strong atomic disorder in suppressing the detrimental phase transition
and enhancing the thermoelectric performance in GeTe. We found that
AgSnSe2 and Sb co-alloying eliminates the unfavorable phase
transition due to the high configurational entropy and achieve the
cubic Ge1–x–y
Sb
y
Te1–x
(AgSnSe2)
x
solid solutions
with cationic and anionic site disorder. Though AgSnSe2 substitution drives the carrier mean free path toward the Ioffe–Regel
limit and minimizes the carrier mobility, the increased carrier concentration
could render a decent electrical conductivity, affording enough phase
room for further performance optimization. Given the lowermost carrier
mean free path, further Sb alloying on Ge sites was implemented to
progressively optimize the carrier concentration and enhance the density-of-state
effective mass, thereby substantially enhancing the Seebeck coefficient.
In addition, the high density of nanoscale strain clusters induced
by strong atomic disorders significantly restrains the lattice thermal
conductivity. As a result, a state-of-the-art zT ≈
1.54 at 773 K was attained in cubic Ge0.58Sb0.22Te0.8(AgSnSe2)0.2. These results
demonstrate that the strong atomic disorder at the high entropy scale
is a previously underheeded but promising approach in thermoelectric
material research, especially for the numerous low carrier mobility
materials.