
The SiO₂/Si substrate serves as the foundational platform for CIPS flakes. However, organic contaminants, nanoscale dust, and microscopic impurities on its surface can easily lead to poor adhesion, interfacial bubbles, and lattice distortion in subsequently exfoliated CIPS flakes. These issues may even introduce additional substrate strain, interfering with the intrinsic structural phase transition laws and piezoelectric performance characterization of CIPS, ultimately causing deviations in experimental data. Therefore, the cleanliness and surface condition of the substrate directly determine the authenticity and accuracy of all subsequent experimental characterizations.
In this study, bulk CIPS crystals were mechanically exfoliated and deposited onto 285 nm SiO₂/Si substrates, yielding flakes with thicknesses ranging from 10 to 250 nm after plasma cleaning. Leveraging its highly efficient, precise, and non-destructive plasma surface treatment capabilities, the CIF CPC-G Plasma Cleaner successfully achieved deep cleaning and surface activation of the SiO₂/Si substrates, thoroughly removing organic residues and particulate impurities. This ensured that the mechanically exfoliated CIPS flakes across the entire 10–250 nm thickness range achieved perfect adhesion to the substrates, effectively eliminating experimental interferences caused by interfacial defects.

Verified the practical application potential of CIPS-based devices:
fabricated at the optimal thickness of 100 nm successfully achieves a synergistic combination of high electromechanical coupling efficiency and excellent voltage sensitivity—a performance combination difficult to realize in traditional piezoelectric devices. Furthermore, the device exhibits a linear correlation between output voltage and applied pressure, along with good stability and repeatability. These findings provide specific material thickness and structural references for the design of next-generation flexible sensors, precision actuators, and low-power energy harvesters.

Figure 1 |
(a) Schematic diagram of the contact resonance atomic force microscopy (CR-AFM) setup; the inset illustrates the contact resonance frequency shift and the crystal structure of CuInP₂S₆ (CIPS).
(b) Topography and contact resonance frequency maps of CIPS flakes with varying thicknesses. Scale bar: 2 μm.
(c) Line profiles of sample height and contact resonance frequency measured along the solid line in (b).
(d) Thickness dependence of the contact resonance frequency shift (Δf).
(e) Extracted out-of-plane modulus (C₃₃) as a function of sample thickness. The blue and red curves correspond to the modulus evolution of the triclinic and monoclinic phases, respectively.

Figure 2 |
(a, b) Selected area electron diffraction (SAED) patterns of CIPS flakes with thicknesses of 20 nm and 130 nm, respectively, along the out-of-plane (z) direction; the insets show the side-view structural schematics of the triclinic and monoclinic phases viewed along the y-axis.
(c–e) Atomic force microscopy (AFM) topography, Kelvin probe force microscopy (KPFM) images, and lateral force images, illustrating the thickness-dependent friction characteristics of CIPS flakes with varying thicknesses.
(f) Schematic illustration of the thickness-dependent evolution of surface energy and friction characteristics on the thin film surface.
(g) Typical load–friction curves of CIPS flakes with thicknesses of 48 nm and 148 nm.

Figure 3 |
(a) Piezoresponse force microscopy (PFM) amplitude response (with resonance amplification effect eliminated) of CIPS under different applied voltages. The thickness of the used flake is 75 nm.
(b) Thickness-dependent piezoelectric coefficients extracted from the PFM test results, along with the corresponding fitting curves.
(c) Comparison of the out-of-plane electromechanical coupling coefficient ( ) between CIPS and various representative materials, evaluated under matched crystal orientations and comparable thickness ranges.

Figure 4 |
(a) Schematic diagram of the CIPS-based piezoelectric sensor; the inset illustrates the applied cyclic loading mode.
(b) Periodic piezoelectric response curves generated by the device, along with an enlarged view of the selected area.
(c) Thickness-dependent voltage output characteristics measured under a constant pressure of 2 N.
(d) Voltage response of the device under various applied pressures.
(e) Thickness dependence of the piezoelectric voltage coefficient.
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