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

Title: Tunable two-dimensional interfacial coupling in molecular heterostructures

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 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.

Authors:

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

Temple Univ., Philadelphia, PA (United States). Dept. of Mechanical Engineering and Temple Materials Inst.
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). Temple Materials Inst. and Dept. of Chemistry and Inst. for Computational Molecular Science

Publication Date:: Tue Aug 22 00:00:00 EDT 2017

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

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

OSTI Identifier:: 1425646

Grant/Contract Number:: SC0012575; OCI-0725070; ACI-1238993; AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Molecular self-assembly; Organic molecules in materials science

Citation Formats


                    Xu, Beibei, Chakraborty, Himanshu, Yadav, Vivek K., Zhang, Zhuolei, Klein, Michael L., and Ren, Shenqiang. Tunable two-dimensional interfacial coupling in molecular heterostructures.  United States: N. p., 2017. 
Web.  doi:10.1038/s41467-017-00390-1.

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                    Xu, Beibei, Chakraborty, Himanshu, Yadav, Vivek K., Zhang, Zhuolei, Klein, Michael L., & Ren, Shenqiang. Tunable two-dimensional interfacial coupling in molecular heterostructures.  United States.  https://doi.org/10.1038/s41467-017-00390-1

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                    Xu, Beibei, Chakraborty, Himanshu, Yadav, Vivek K., Zhang, Zhuolei, Klein, Michael L., and Ren, Shenqiang. Tue .  
"Tunable two-dimensional interfacial coupling in molecular heterostructures".  United States.  https://doi.org/10.1038/s41467-017-00390-1.  https://www.osti.gov/servlets/purl/1425646.

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@article{osti_1425646,

  title        = {Tunable two-dimensional interfacial coupling in molecular heterostructures},

  author       = {Xu, Beibei and Chakraborty, Himanshu and Yadav, Vivek K. and Zhang, Zhuolei and Klein, Michael L. and Ren, Shenqiang},

  abstractNote = {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.},

  doi          = {10.1038/s41467-017-00390-1},

  journal      = {Nature Communications},

  number       = 1,

  volume       = 8,

  place        = {United States},

  year         = {Tue Aug 22 00:00:00 EDT 2017},

  month        = {Tue Aug 22 00:00:00 EDT 2017}

}

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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
DOI: 10.1103/PhysRevLett.77.3865