Characterizations by Piezoresponse Force Microscopy on Relaxor Properties of Pb(Mg,Nb)O3-PbTiO3 Ultra-thin Films

doi:10.15541/jim20240471

Abstract

Abstract:

Relaxor ferroelectrics exhibit extensive applications in sensing technology, optoelectronics, high-density memory storage, and neuromorphic computing, owing to their superior dielectric and piezoelectric characteristics. However, conventional methods, including the Sawyer-Tower circuit and the positive-up-negative-down (PUND) pulse train, prove inadequate for nanoscale ultra-thin films, since the relaxor characteristics may be hindered by substantial leakage currents. In this study, a piezoresponse force microscopy (PFM)-based method for characterizing nanoscale relaxor properties was proposed. Taking ultra-thin Pb(Mg,Nb)O₃-PbTiO₃ (PMN-PT) films as examples, this work compares polarization hysteresis behavior under On-field and Off-field modes of the dual AC resonance tracking (DART) PFM measurements between relaxor PMN-PT and ferroelectric Pb(Zr,Ti)O₃ (PZT) thin films with varying thicknesses. Relaxor characteristics of nanometer-thick PMN-PT films are characterized by modulating amplitude of AC readout to eliminate potential false signals. Furthermore, PFM characterizations of PMN-PT ultra-thin films under different in-plane compressive strains and thicknesses demonstrate that the relaxor characteristics are suppressed and ferroelectric properties are observed at relatively large compressive strains of 3.19%. Additionally, the critical thickness for ferroelectric-relaxor transition is identified. These results verify availability of the proposed PFM-based method for characterizing nanoscale relaxor properties. Therefore, this study not only provides a novel characterization method for exploration of the relaxor in ultra-thin films, but also establishes a foundation for understanding the relaxor polarization behavior in ferroelectric materials, thereby advancing applications of relaxor ferroelectric materials in low-dimensional electronic devices.

Key words: relaxor ferroelectric, piezoresponse force microscope, PMN-PT, ultra-thin film, polarization property

CLC Number:

TQ174

DONG Chenyu, ZHENG Weijie, MA Yifan, ZHENG Chunyan, WEN Zheng. Characterizations by Piezoresponse Force Microscopy on Relaxor Properties of Pb(Mg,Nb)O₃-PbTiO₃ Ultra-thin Films[J]. Journal of Inorganic Materials, 2025, 40(6): 675-682.

Figures/Tables 10

Fig. 1 (a) XRD patterns of PMN-PT/SRO/GSO and PZT/SRO/GSO heterostructures, where PMN-PT and PZT are both 100 nm thick, in which the * symbols indicate the (00l) Bragg reflections peaks of GSO, with insets showing the AFM surface morphologies of GSO substrate, SRO/GSO, PMN-PT(5 nm)/SRO/GSO, PMN-PT(100 nm)/SRO/GSO thin-film heterostructures; (b) Cross-sectional STEM image and elemental distributions of the 5 nm thick PMN-PT/SRO/GSO heterostructure; (c) HAADF image of the PMN-PT layer

Fig. 2 Polarization-electric field hysteresis loops of PZT (a) and PMN-PT (b) thin-film capacitors with different thicknesses

Fig. 3 PFM hysteresis characterizations on PZT and PMN-PT thin-film heterostructures with different thicknesses (a) Triangular pulse waveform for PFM test, where the red line represents the DC bias to polarize sample and the blue line represents the AC signal (VAC) used for readout. The polarization is read out in the Off-field mode when the DC bias is zero, and in the On-field mode when the DC bias is non-zero; (b) Sketches of the polarization response of the sample; (c) PFM hysteresis loops with various VAC; (d-g) PFM phases and amplitude hysteresis loops obtained under On-field and Off-field modes with various VAC: 40 nm-thick PZT (d) and PMN-PT (e), 5 nm-thick PZT (f) and PMN-PT (g). Colorful figures are available on website

Fig. 4 PFM hysteresis loops of 5 nm-thick PMN-PT films on various substrates (a) PMN-PT/SRO/GSO; (b) PMN-PT/SRO/DSO; (c) PMN-PT/SRO/STO. Colorful figures are available on website

Fig. 5 PFM hysteresis loops of PMN-PT/SRO/STO heterostructures with different thicknesses

Fig. S1 Surface morphologies, PFM amplitudes and phase images of 100 nm-thick PZT and PMN-PT thin films

Fig. S2 S2 PFM hysteresis loops of 100 nm-thick PMN-PT films

Fig. S3 PFM hysteresis loops of STO crystal

Fig. S4 (a) PMN-PT/SRO/GSO and (b) PMN-PT/SRO/STO PFM read/write domain characterizations

Fig. S5 PFM hysteresis loops of PMN-PT films with different thicknesses (a) 10 nm; (b) 15 nm; (c) 20 nm

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Characterizations by Piezoresponse Force Microscopy on Relaxor Properties of Pb(Mg,Nb)O₃-PbTiO₃ Ultra-thin Films

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