Tunable two-dimensional interfacial coupling in molecular heterostructures.

Xu, Beibei; Chakraborty, Himanshu; Yadav, Vivek K; Zhang, Zhuolei; Klein, Michael L; Ren, Shenqiang · Nat Commun · 2017

basic_science · Level V

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Abstract

Two-dimensional van der Waals heterostructures are of considerable interest for the next generation nanoelectronics because of their unique interlayer coupling and optoelectronic properties. Here, we report a modified Langmuir-Blodgett method to organize two-dimensional molecular charge transfer crystals into arbitrarily and vertically stacked heterostructures, consisting of bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF)/C<sub>60</sub> and poly(3-dodecylthiophene-2,5-diyl) (P3DDT)/C<sub>60</sub> nanosheets. A strong and anisotropic interfacial coupling between the charge transfer pairs is demonstrated. The van der Waals heterostructures exhibit pressure dependent sensitivity with a high piezoresistance coefficient of -4.4 × 10<sup>-6</sup> Pa<sup>-1</sup>, and conductance and capacitance tunable by external stimuli (ferroelectric field and magnetic field). Density functional theory calculations confirm charge transfer between the n-orbitals of the S atoms in BEDT-TTF of the BEDT-TTF/C<sub>60</sub> layer and the π* orbitals of C atoms in C<sub>60</sub> of the P3DDT/C<sub>60</sub> layer contribute to the inter-complex CT. The two-dimensional molecular van der Waals heterostructures with tunable optical-electronic-magnetic coupling properties are promising for flexible electronic applications.Two-dimensional van der Waals heterostructures are of interest due to their unique interlayer coupling and optoelectronic properties. Here authors develop a Langmuir-Blodgett method to organize charge transfer molecular heterostructures with externally tunable conductance and capacitance and broadband photoresponse.