Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 15, Pages 3776-3781Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1800234115
Keywords
charge transfer; self-assembling; 2D nanosheets; photostriction; conformational disorder
Categories
Funding
- US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0017928]
- Center for the Computational Design of Functional Layered Materials, an Energy Frontier Research Center - US Department of Energy, Office of Science, and Basic Energy Sciences [DE-SC0012575]
- National Science Foundation through Major Research Instrumentation Award [1625061]
- National Science Foundation [OCI-0725070, ACI-1238993]
- state of Illinois
- Blue Waters sustained-petascale computing project
- U.S. Department of Energy (DOE) [DE-SC0017928] Funding Source: U.S. Department of Energy (DOE)
- Direct For Computer & Info Scie & Enginr
- Division Of Computer and Network Systems [1625061] Funding Source: National Science Foundation
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We report the observation of a sizable photostrictive effect of 5.7% with fast, submillisecond response times, arising from a light-induced lattice dilation of a molecular nanosheet, composed of the molecular charge-transfer compound dibenzotetrathiaful-valene (DBTTF) and C-60. An interfacial self-assembly approach is introduced for the thickness-controlled growth of the thin films. From photoabsorption measurements, molecular simulations, and electronic structure calculations, we suggest that photostriction within these films arises from a transformation in the molecular structure of constituent molecules upon photoinduced charge transfer, as well as the accommodation of free charge carriers within the material. Additionally, we find that the photostrictive properties of the nanosheets are thickness-dependent, a phenomenon that we suggest arises from surface-induced conformational disorder in the molecular components of the film. Moreover, because of the molecular structure in the films, which results largely from interactions between the constituent p-systems and the sulfur atoms of DBTTF, the optoelectronic properties are found to be anisotropic. This work enables the fabrication of 2D molecular charge-transfer nanosheets with tunable thicknesses and properties, suitable for a wide range of applications in flexible electronic technologies.
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