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Incorporating multifunctionality along with the spin-related phenomenon in a single device is of great interest for the development of next generation spintronic devices. One of these challenges is to couple the photo-response of the device together with its magneto-response to exploit the multifunctional operation at room temperature. Here, the multifunctional operation of a single layer p-type molecular spin valve is presented, where the device shows a photovoltaic effect at the room temperature on a transparent glass substrate. The generated photovoltage is almost three times larger than the applied bias to the device which facilitates the modulation of the magnetic response of the device both with bias and light. It is observed that the photovoltage modulation with light and magnetic field is linear with the light intensity. The device shows an increase in power conversion efficiency under magnetic field, an ability to invert the current with magnetic field and under certain conditions it can act as a spin-photodetector with zero power consumption in the standby mode. The room temperature exploitation of the interplay among light, bias and magnetic field in the single device with a p-type molecule opens a way towards more complex and efficient operation of a complete spin-photovoltaic cell., 17 pages, 7 Figures, included supplementary

The quantification of the electronic transport energy gap of a molecular semiconductor is essential for pursuing any challenge in molecular optoelectronics. However, this remains largely elusive because of the difficulties in its determination by conventional spectroscopic methods. This communication presents an in-device molecular spectroscopy (i-MOS) technique, which permits measuring this gap seamlessly, in real device operative conditions, at room temperature and without any previous knowledge of the material's parameters. This result is achieved by determining the occupied and unoccupied molecular orbitals of an organic semiconductor thin-film by using a single three terminal solid-state device., Materials horizons;2019, 6, 1663--166

An approach for the synthesis of pyrene-fused acenes that allows the introduction of electron-withdrawing cyano groups in key positions that simultaneously (i) induce twists in the aromatic framework and (ii) stabilize the LUMO level is reported. This combination of steric and electronic features provide a twisted, stable, and n-type tetrabenzoheptacene as confirmed by a combination of theoretical calculations and optical, electrochemical, thermal, and electrical characterization.

The realization of both p-type and n-type operations in a single organic field effect transistor (OFET) is critical for simplifying the design of complex organic circuits. Typically, only p-type or n-type operation is realized in an OFET, while the respective counterpart is either suppressed by charge trapping or limited by the injection barrier with the electrodes. Here we show that only the presence of a top dielectric turns an n-type polymer semiconductor (N2200, Polyera ActiveInk) into an ambipolar one, as detected from both bottom and top gated OFET operation. The effect is independent of the channel thickness and the top dielectric combinations. Variable temperature transfer characteristics show that both the electrons and holes can be equally transported through the bulk of the polymer semiconductor., Comment: 16 pages, 3 figures

Polymer field-effect transistors with 2D graphene electrodes are devices that merge the best of two worlds: on the one hand, the low-cost and processability of organic materials and, on the other hand, the chemical robustness, extreme thinness and flexibility of graphene. Here, we demonstrate the tuning of the ambipolar nature of the semiconductor polymer N2200 from Polyera ActiveInk by incorporating graphene electrodes in a transistor geometry. Our devices show a balanced ambipolar behavior with high current ON-OFF ratio and charge carrier mobilities. These effects are caused by both the effective energy barrier modulation and by the weak electric field screening effect at the graphene-polymer interface. Our results provide a strategy to integrate 2D graphene electrodes in ambipolar transistors in order to improve and modulate their characteristics, paving the way for the design of novel organic electronic devices., 16 pages, 4 figures, Accepted Manuscript

Marcus’s theory of electron transfer, initially formulated six decades ago for redox reactions in solution, is now of great importance for very diverse scientific communities. The molecular scale tunability of electronic properties renders organic semiconductor materials in principle an ideal platform to test this theory. However, the demonstration of charge transfer in different Marcus regions requires a precise control over the driving force acting on the charge carriers. Here, we make use of a three-terminal hot-electron molecular transistor, which lets us access unconventional transport regimes. Thanks to the control of the injection energy of hot carriers in the molecular thin film we induce an effective negative differential resistance state that is a direct consequence of the Marcus Inverted Region., To demonstrate charge transfer in different Marcus regimes in an organic semiconductor, precise tuning of the material’s electronic properties is required. Here, the authors use a three-terminal hot-electron technique to access the Marcus regimes for electronic transport in organic thin films.