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The development of intrinsic vacancies in SnSe single crystalswas investigated as a function of annealing temperature bymeans of positron annihilation spectroscopy accompanied bytransport measurements. It has been demonstrated that two typesof vacancies are present in single-crystalline SnSe. While Snvacancies dominate in the low-temperature region, Se vacanciesand vacancy clusters govern the high-temperature region. Thesefindings are supported by theoretical calculations enablingdirect detection and quantification of the most favorable typeof vacancies. The experiments show that Sn vacancies couplewith one or more Se vacancies with increasing temperature toform vacancy clusters. Interestingly, the clusters survive thealpha ->beta transition at approximate to 800 K and even growin size with temperature. The concentration of both Sevacancies and vacancy clusters increases with temperature,similar to thermoelectric performance. This indicates that theextraordinary thermoelectric properties of SnSe are related topoint defects. We suggest that either these defects vary theband structure in favor of high thermoelectric performance orintroduce an energy-dependent scattering of free carriersrealizing, in fact, energy filtering of the free carriers.Cluster defects account for the glasslike thermal conductivityof SnSe at elevated temperatures.

Vacancies in SnSe single crystals in a near-equilibrium state