The 0.72Bi(Fe1−xAlx)O3–0.28BaTiO3 (x = 0, 0.01, 0.03, 0.05, and 0.07, abbreviated as BFAx–BT) lead‐free high‐temperature ceramics were prepared by the conventional ceramic processing. Systematic investigation on the microstructures, crystalline structures, dielectric and piezoelectric properties, and high‐temperature stability of piezoelectric properties was carried out. The crystalline structures of BFAx–BT ceramics evolve from rhombohedral structure with x < 0.01 to the coexistence of rhombohedral structure and pseudocubic phases with x ≈ 0.01, finally to pseudocubic phases when x > 0.03. Remarkably high‐temperature stability with near‐zero temperature coefficient of piezoelectric properties (TCkp), together with improved piezoelectric properties has been achieved for x = 0.01 BFAx–BT ceramics. The BFAx–BT(x = 0.01) ceramics simultaneously show the excellent piezoelectric properties of d33 = 151 pC/N, kp = 0.31 and super‐high‐temperature stability of Td = 420°C, TCkp = 1 × 10−4. It is considered that the observed strong piezoelectricity and remarkably high‐temperature stability should be ascribed to the phase coexistence of rhombohedral and pseudocubic phases. The rhombohedral phases have a positive TCkp value and the pseudocubic phases possess a negative TCkp value. Thus, the TCkp value of BFAx–BT ceramics can be tuned by composition of x.

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The properties of one-photon absorption (OPA), emission and two-photon absorption (TPA) of a di-2-picolylaminebased zinc ion sensor are investigated by employing the density functional theory in combination with response functions. The responsive mechanism is explored. It is found that the calculated OPA and TPA properties are quite consistent with experimental data. Because the intra-molecular charge transfer (ICT) increases upon zinc ion binding, the TPA intensity is enhanced dramatically. According to the model sensor, we design a series of zinc ion probes which differ by conjugation center, acceptor and donor moieties. The properties of OPA, emission and TPA of the designed molecules are calculated at the same computational level. Our results demonstrate that the OPA and emission wavelengths of the designed probes have large red-shifts after zinc ions have been bound. Comparing with the model sensor, the TPA intensities of the designed probes are enhanced significantly and the absorption positions are red-shifted to longer wavelength range. Furthermore, the TPA intensity can be improved greatly upon zinc ion binding due to the increased ICT mechanism. These compounds are potential excellent candidates for two-photon fluorescent zinc ion probes.