“…The pyroelectric effect, i.e., the change of spontaneous polarization in polar materials induced by the variation of temperature, is used in a wide range of applications such as infrared (IR) sensing and thermal energy harvesting. − Pyroelectricity has been extensively investigated in inorganic ferroelectrics (such as single crystals and ceramics) and organic polymers. − High pyroelectric effect was first explored in triglycine sulfate (TGS) for IR sensors, a typical order–disorder ferroelectric single crystal whose spontaneous polarization originates from the ordering of the positively charged NH 3 groups of G1 glycine molecules. − Nowadays, displacive ferroelectrics such as lithium tantalite (LT), lead zirconate titanate (PZT), lead niobium magnesium–lead titanate (PMN–PT), barium strontium titanate (BST) single crystals, and ceramics have been extensively equipped in IR detectors and thermal energy harvesters, in which the pyroelectric response is generated by the change of ion displacement (electric dipole moment) caused by the variation of temperature. − Besides, poly(vinylidene fluoride) (PVDF)-based ferroelectric polymers showing an order–disorder phase transition at around the Curie temperature have also been widely used for flexible pyroelectric devices. , Over the last few decades, strenuous efforts have been made to increase the pyroelectric coefficient of the materials for high-sensitivity IR detectors and high-efficiency thermal energy harvesters. − However, high figures of merit (FOMs) are essential for high-performance pyroelectric devices, in which not only high pyroelectric coefficient but also other complementary parameters, e.g., low dielectric constant, are all indispensable. − , Taking IR sensors for instance, F V = p /(ε 0 ε r C v ) ( p , ε 0 , ε r , and C v are the pyroelectric coefficient, vacuum permittivity, relative dielectric constant, and volumetric specific heat, respectively) denotes the maximum pyroelectric voltage that can input into the circuit of the devices, determining the sensitivity of the detectors. Analogously, for thermal energy harvesters, F E = p 2 /(ε 0 ε r ) represents the amount of electric power converted by the pyroelectrics with a given thermal energy.…”