TY - JOUR
T1 - Thermally Stable Capacitive Energy-Density and Colossal Electrocaloric and Pyroelectric Effects of Sm-Doped Pb(Mg1/3Nb2/3)O3-PbTiO3 Thin Films
AU - Hanani, Zouhair
AU - Belhadi, Jamal
AU - Trstenjak, Urška
AU - Shepelin, Nick A.
AU - Bobnar, Vid
AU - Uršič, Hana
AU - Daneu, Nina
AU - Novak, Nikola
AU - Fabijan, David
AU - Razumnaya, Anna
AU - Tikhonov, Yuri
AU - Lippert, Thomas
AU - Kutnjak, Zdravko
AU - Koster, Gertjan
AU - Lukyanchuk, Igor
AU - Spreitzer, Matjaž
N1 - Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society.
PY - 2024/11/18
Y1 - 2024/11/18
N2 - Sm-doped Pb(Mg1/3Nb2/3)O3-PbTiO3 (Sm-PMN-PT) bulk materials have revealed outstanding ferroelectric and piezoelectric properties due to enhanced local structural heterogeneity. In this study, we further explore the potential of Sm-PMN-PT by fabricating epitaxial thin films by pulsed laser deposition, revealing that Sm doping significantly improves the capacitive energy-storage, piezoelectric, electrocaloric, and pyroelectric properties of PMN-PT thin films. These Sm-PMN-PT thin films exhibit fatigue-free performance up to 109 charge-discharge cycles and maintain thermal stability across a wide temperature range from −40 to 200 °C. Notably, the films demonstrate a colossal electrocaloric effect with a temperature change of 59.4 K and a remarkable pyroelectric energy density reaching 40 J cm-3. By using scanning transmission electron microscopy and phase-field modeling, we revealed that these exceptional properties arise from the increased local structural heterogeneity and strong local electric fields along spontaneous polarization directions, facilitating the nucleation of polymorphic nanodomains characterized by a slush-like polar structure. These findings highlight the enormous potential of Sm-PMN-PT films in capacitive energy storage and solid-state electrothermal energy interconversion. Furthermore, this approach holds broad potential for other relaxor ferroelectrics by enabling the manipulation of nanodomain structures, paving the way for developing robust multifunctional materials.
AB - Sm-doped Pb(Mg1/3Nb2/3)O3-PbTiO3 (Sm-PMN-PT) bulk materials have revealed outstanding ferroelectric and piezoelectric properties due to enhanced local structural heterogeneity. In this study, we further explore the potential of Sm-PMN-PT by fabricating epitaxial thin films by pulsed laser deposition, revealing that Sm doping significantly improves the capacitive energy-storage, piezoelectric, electrocaloric, and pyroelectric properties of PMN-PT thin films. These Sm-PMN-PT thin films exhibit fatigue-free performance up to 109 charge-discharge cycles and maintain thermal stability across a wide temperature range from −40 to 200 °C. Notably, the films demonstrate a colossal electrocaloric effect with a temperature change of 59.4 K and a remarkable pyroelectric energy density reaching 40 J cm-3. By using scanning transmission electron microscopy and phase-field modeling, we revealed that these exceptional properties arise from the increased local structural heterogeneity and strong local electric fields along spontaneous polarization directions, facilitating the nucleation of polymorphic nanodomains characterized by a slush-like polar structure. These findings highlight the enormous potential of Sm-PMN-PT films in capacitive energy storage and solid-state electrothermal energy interconversion. Furthermore, this approach holds broad potential for other relaxor ferroelectrics by enabling the manipulation of nanodomain structures, paving the way for developing robust multifunctional materials.
UR - http://www.scopus.com/inward/record.url?scp=85209678552&partnerID=8YFLogxK
U2 - 10.1021/jacs.4c11555
DO - 10.1021/jacs.4c11555
M3 - Article
C2 - 39556522
AN - SCOPUS:85209678552
SN - 0002-7863
VL - 146
SP - 32595
EP - 32604
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 47
ER -