Tunable two-dimensional interfacial coupling in molecular heterostructures

Xu, Beibei; Chakraborty, Himanshu; Yadav, Vivek K.; Zhang, Zhuolei; Klein, Michael L.; Ren, Shenqiang

doi:10.1038/s41467-017-00390-1

Tunable two-dimensional interfacial coupling in molecular heterostructures

Journal Article · Tue Aug 22 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/s41467-017-00390-1· OSTI ID:1425646

Xu, Beibei ^[1]; Chakraborty, Himanshu ^[2]; Yadav, Vivek K. ^[3]; Zhang, Zhuolei ^[4]; Klein, Michael L. ^[5]; Ren, Shenqiang ^[4]

Temple Univ., Philadelphia, PA (United States). Dept. of Mechanical Engineering and Temple Materials Inst.; Department of Mechanical Engineering, Temple University, Philadelphia, PA 19122, USA
Temple Univ., Philadelphia, PA (United States). Dept. of Chemistry and Inst. for Computational Molecular Science and Center for the Computational Design of Functional Layered Materials
Temple Univ., Philadelphia, PA (United States). Dept. of Chemistry and Inst. for Computational Molecular Science
Temple Univ., Philadelphia, PA (United States). Dept. of Mechanical Engineering and Temple Materials Inst.
Temple Univ., Philadelphia, PA (United States). Temple Materials Inst. and Dept. of Chemistry and Inst. for Computational Molecular Science

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 twodimensional 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. Thus, the two-dimensional molecular van der Waals heterostructures with tunable optical–electronic–magnetic coupling properties are promising for flexible electronic applications.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Temple Univ., Philadelphia, PA (United States)

Sponsoring Organization:: National Science Foundation (NSF); State of Illinois; US Army Research Office (ARO); USDOE Office of Science (SC)Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0012575

OSTI ID:: 1425646

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Light-induced dilation in nanosheets of charge-transfer complexes Zhang, Zhuolei; Remsing, Richard C.; Chakraborty, Himanshu Proceedings of the National Academy of Sciences, Vol. 115, Issue 15 https://doi.org/10.1073/pnas.1800234115	journal	March 2018
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