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Perpendicularly oriented vinylidene fluoride oligomer thin films with six molecular layers were poled during vacuum evaporation (in situ poling) using a micro-gapped comb-like electrode, and their pyroelectric characteristics were investigated. The extent of polarization achieved with in situ poling performed by applying a low electric field (7.7 MV m−1) is the same as that achieved by conventional post-poling with the application of a high electric field (>100 MV m−1). Despite using a film with a few molecular layers, the in situ poled sensor showed pyroelectric response without the use of an infrared ray absorption layer; voltage sensitivity of 198 V W−1 was obtained, which is much higher than that of the post-poled sensor (∼16 V W−1). The improvement in sensitivity is attributed to the amount of charge injected during the poling treatment.

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