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Title: Tunable two-dimensional interfacial coupling in molecular heterostructures

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)/C 60 and poly (3-dodecylthiophene-2,5-diyl) (P3DDT)/C 60 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/C 60 layer and the π* orbitals of C atoms in C 60 of the P3DDT/C 60 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.
 [1] ;  [2] ;  [3] ;  [1] ;  [4] ;  [1]
  1. Temple Univ., Philadelphia, PA (United States). Dept. of Mechanical Engineering and Temple Materials Inst.
  2. 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
  3. Temple Univ., Philadelphia, PA (United States). Dept. of Chemistry and Inst. for Computational Molecular Science
  4. Temple Univ., Philadelphia, PA (United States). Temple Materials Inst. and Dept. of Chemistry and Inst. for Computational Molecular Science
Publication Date:
Grant/Contract Number:
SC0012575; OCI-0725070; ACI-1238993; AC02-05CH11231
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Nature Publishing Group
Research Org:
Temple Univ., Philadelphia, PA (United States)
Sponsoring Org:
USDOE Office of Science (SC)Basic Energy Sciences (BES) (SC-22); US Army Research Office (ARO); National Science Foundation (NSF); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Country of Publication:
United States
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Molecular self-assembly; Organic molecules in materials science
OSTI Identifier: