“…The XRD pattern of the as-deposited flake (Fig. 3a ) reveals two dominant peaks at 24.4° and 27.3°, corresponding to the (003) and (102) planes of trigonal α-GaPO 4 , respectively 14 , 17 , 27 . Fig.…”
Two-dimensional piezotronics will benefit from the emergence of new crystals featuring high piezoelectric coefficients. Gallium phosphate (GaPO4) is an archetypal piezoelectric material, which does not naturally crystallise in a stratified structure and hence cannot be exfoliated using conventional methods. Here, we report a low-temperature liquid metal-based two-dimensional printing and synthesis strategy to achieve this goal. We exfoliate and surface print the interfacial oxide layer of liquid gallium, followed by a vapour phase reaction. The method offers access to large-area, wide bandgap two-dimensional (2D) GaPO4 nanosheets of unit cell thickness, while featuring lateral dimensions reaching centimetres. The unit cell thick nanosheets present a large effective out-of-plane piezoelectric coefficient of 7.5 ± 0.8 pm V−1. The developed printing process is also suitable for the synthesis of free standing GaPO4 nanosheets. The low temperature synthesis method is compatible with a variety of electronic device fabrication procedures, providing a route for the development of future 2D piezoelectric materials.
“…The XRD pattern of the as-deposited flake (Fig. 3a ) reveals two dominant peaks at 24.4° and 27.3°, corresponding to the (003) and (102) planes of trigonal α-GaPO 4 , respectively 14 , 17 , 27 . Fig.…”
Two-dimensional piezotronics will benefit from the emergence of new crystals featuring high piezoelectric coefficients. Gallium phosphate (GaPO4) is an archetypal piezoelectric material, which does not naturally crystallise in a stratified structure and hence cannot be exfoliated using conventional methods. Here, we report a low-temperature liquid metal-based two-dimensional printing and synthesis strategy to achieve this goal. We exfoliate and surface print the interfacial oxide layer of liquid gallium, followed by a vapour phase reaction. The method offers access to large-area, wide bandgap two-dimensional (2D) GaPO4 nanosheets of unit cell thickness, while featuring lateral dimensions reaching centimetres. The unit cell thick nanosheets present a large effective out-of-plane piezoelectric coefficient of 7.5 ± 0.8 pm V−1. The developed printing process is also suitable for the synthesis of free standing GaPO4 nanosheets. The low temperature synthesis method is compatible with a variety of electronic device fabrication procedures, providing a route for the development of future 2D piezoelectric materials.
“…The high-temperature flux-growth method consists of using mineral fluxes as solvents for growing α-GaPO 4 single crystals at temperatures below their allotropic transformation. − The interesting effect of both the anhydrous solvent and the high temperature is a prevention of hydroxyl group incorporation during growth experiments. From room-temperature infrared measurements in the transmission mode, the virgin flux-grown α-GaPO 4 crystals have been found, as expected, free from OH impurities.…”
The lattice parameter change with respect to temperature (T) has been measured using high-temperature powder X-ray diffraction techniques for high-temperature flux-grown GaPO(4) single crystals with the alpha-quartz structure. The lattice and the volume linear thermal expansion coefficients in the temperature range 303-1173 K were computed from the X-ray data. The percentage linear thermal expansions along the a and c axes at 1173 K are 1.5 and 0.51, respectively. The temperature dependence of the mass density rho of flux-grown GaPO(4) single crystals was evaluated using the volume thermal expansion coefficient alpha(V)(T) = 3.291 x 10(-5) - 2.786 x 10(-8) [T] + 4.598 x 10(-11)[T](2). Single-crystal high-resolution Brillouin spectroscopy measurements have been carried out at ambient pressure from 303 to 1123 K to determine the elastic constants C(IJ) of high-temperature flux-grown GaPO(4) material. The single-crystal elastic moduli were calculated using the sound velocities via the measured Brillouin frequency shifts Deltanu(B). These are, to our knowledge, the highest temperatures at which single-crystal elastic constants of alpha-GaPO(4) have been measured. Most of the room-temperature elastic constant values measured on flux-grown GaPO(4) material are higher than the ones found for hydrothermally grown GaPO(4) single crystals. The fourth-order temperature coefficients of both the Brillouin frequency shifts T(nuB)((n)) and the single-crystal elastic moduli T(C(IJ))((n)) were obtained. The first-order temperature coefficients of the C(IJ) are in excellent agreement with previous reports on low-temperature hydrothermally grown alpha-GaPO(4) single crystals, while small discrepancies in the higher-order temperature coefficients are observed. This is explained in terms of the OH content in the GaPO(4) network, which is an important parameter in the crystal thermal behavior.
“…The XRD measurements also reaffirmed that the crystalline structure of the 2D GaPO 4 lm is dominated by the (003) and ( 102) planes of trigonal a-GaPO 4 (ref. [199][200][201][202] (Fig. 20f).…”
Two-dimensional (2D) surface oxide films of post-transition liquid metals and their alloys have been recently introduced as an emerging category of ultra-thin functional semiconductor materials with fascinating physico-chemical and structural characteristics.
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