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The electronic structures of Heusler-type FeV Ta Al and FeVAl Ta alloys were investigated by electronic band structure calculations and synchrotron radiation photoelectron spectroscopy measurements to elucidate the change in the electronic structure due to the Ta substitution. While V and Ta atoms have the same electron configuration, the hybridization between Fe 3  and V 3  states gradually decreases in Ta-substituted FeVAl alloy and the valence band is only shifted to lower binding energy side. This change of the electronic structure is hypothesized to be the underlying reason behind the improved p-type thermoelectric performance in FeV Ta Al alloy, but the degraded n-type thermoelectric performance in FeVAl Ta alloy. Ta substitution is a promising way to further improve the thermoelectric properties of p-type Heusler-type FeVAl-based alloy because of not only an increasing power factor but also decreasing thermal conductivity.


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