Tunable two-dimensional interfacial coupling in molecular heterostructures

Beibei Xu, Himanshu Chakraborty, Vivek K. Yadav, Zhuolei Zhang, Michael L. Klein and Shenqiang Ren ()
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Beibei Xu: Temple University
Himanshu Chakraborty: Temple University
Vivek K. Yadav: Temple University
Zhuolei Zhang: Temple University
Michael L. Klein: Temple Materials Institute, Temple University
Shenqiang Ren: Temple University

Nature Communications, 2017, vol. 8, issue 1, 1-11

Abstract: 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)/C60 and poly(3-dodecylthiophene-2,5-diyl) (P3DDT)/C60 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 × 10−6 Pa−1, 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/C60 layer and the π* orbitals of C atoms in C60 of the P3DDT/C60 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.

Date: 2017
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DOI: 10.1038/s41467-017-00390-1

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