Ferroelectric and pyroelectric properties of polycrystalline La-doped HfO2 thin films

Lanthanum has been identified as a promising dopant to achieve ferroelectricity in HfO2 thin films in recent theoretical and experimental studies. In this work, the pyroelectric properties of 10 nm thick polycrystalline La-doped HfO2 layers manufactured by thermal atomic layer deposition are assessed employing a sinusoidal temperature profile. Compared to Si doping, La offers a broader dopant range in which ferroelectric behavior is obtained, making the material interesting for large-scale integration and deposition on area-enhanced substrates. Pyroelectric coefficients of up to −80 μC/m2 K are obtained using an optimized stoichiometry, which is comparable to earlier measurements with Si-doped HfO2 samples. Phase-sensitive evaluation of the measured current confirms the pyroelectric origin with minimal spurious contributions. The results are discussed with respect to the ferroelectric switching behavior, which is analyzed employing first-order reversal curve measurements. It is found that there is no simple linear relationship between the remanent polarization and the pyroelectric coefficient. Experimental evidence indicates that the pyroelectric response in polycrystalline thin films is modulated by internal bias fields, which can arise from charged defects. This illustrates the need for careful tuning of the manufacturing conditions and the film phase composition in future applications such as pyroelectric sensors, energy harvesting, or solid-state cooling.