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The fabrication of high-performance Organic Phototransistors (OPTs) by depositing Al-islands atop Poly(3-hexylthiophene) (P3HT) thin film coated using the unidirectional floating-film transfer method (UFTM) has been realized. Further, the effect of Al-island thickness on the OPTs’ performance has been intensively investigated using X-ray photoelectron spectroscopy, X-ray Diffraction, Atomic force microscopy and UV-Vis spectroscopy analysis. Under the optimized conditions, OPTs’ mobility and on–off ratio were found to be 2 × 10−2 cm2 V−1 s−1 and 3 × 104, respectively. Further, the device exhibited high photosensitivity of 105, responsivity of 339 A/W, detectivity of 3 × 1014 Jones, and external quantum efficiency of 7.8 × 103% when illuminated with a 525 nm LED laser (0.3 mW/cm2).

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Fabrication of uniform and oriented thin films of conjugated polymers (CPs) with controlled thickness is essential for the implementation of organic devices. Over the years, unidirectional floating film transfer method (UFTM) has emerged as a facile technique for the fabrication of oriented thin films but its distribution of orientation in vertical (thickness) direction has not been explored yet. To investigate this, thin films of nonregioregular poly(3‐hexylthiophene) are fabricated using UFTM with different concentrations of CPs to obtain thickness variation from 11 to 47 nm. Thin films of 4% and 9% polymer solution have similar dichroic ratio of 5.5 but have an appreciable difference in film thickness of 12 and 47 nm where thicker films are disordered as probed by polarized absorption spectra. Organic field‐effect transistors fabricated using thinner films (12 nm) exhibit a saturated charge carrier mobility of 2.3 × 10−3cm2 V−1 s−1, an order of magnitude higher than its thicker (47 nm) counterpart. This difference in device performance can be attributed to the fact that charge transport is principally governed by the top polymer surface at air–polymer interface, which is found to be more disordered owing to the vertical distribution of orientation.