Flexible organic optoelectronic devices simultaneously targeting mechanical conformability and fast responsivity in the near-infrared (IR) region are a prerequisite to expand the capabilities of practical optical science and engineering for on-skin optoelectronic applications. Here, an ultraflexible near-IR responsive skin-conformal photoplethysmogram sensor based on a bulk heterojunction photovoltaic active layer containing regioregular polyin-dacenodithiophene-pyridyl[2,1,3]thiadiazole-cyclopentadithiophene (PIPCP) is reported. The ultrathin (3 µm thick) photodetector exhibits unprecedented operational stability under severe mechanical deformation at a bending radius of less than 3 µm, even after more than 103 bending cycles. Deliberate optimization of the physical dimensions of the active layer used in the device enables precise on/off switching and high device yield simultaneously. The response frequency over 1 kHz under mechanically deformed conditions facilitates conformal electronic sensors at the machine/human interface. Finally, a mechanically stretchable, flexible, and skin-conformal photoplethysmogram (PPG) device with higher sensitivity than those of rigid devices is demonstrated, through conformal adherence to the flexuous surface of a fingerprint.
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