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Autoperforation of 2D materials for generating two-terminal memristive Janus particles


Graphene and other two-dimensional materials possess desirable mechanical, electrical and chemical properties for incorporation into or onto colloidal particles, potentially granting them unique electronic functions. However, this application has not yet been realized, because conventional top-down lithography scales poorly for producing colloidal solutions. Here, we develop an ‘autoperforation technique that provides a means of spontaneous assembly for surfaces composed of two-dimensional molecular scaffolds. Chemical vapour deposited two-dimensional sheets can autoperforate into circular envelopes when sandwiching a microprinted polymer composite disk of nanoparticle ink, allowing liftoff into solution and simultaneous assembly. The resulting colloidal microparticles have two independently addressable, external Janus faces that we show can function as an intraparticle array of vertically aligned, two-terminal electronic devices. Such particles demonstrate remarkable chemical and mechanical stability and form the basis of particulate electronic devices capable of collecting and storing information about their surroundings, extending nanoelectronics into previously inaccessible environments.

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All relevant data and computer codes are available from the authors and most of them are included within the Supplementary Information, including sections on modelling and simulations, Supplementary Figs 1–60 and Supplementary Videos 112. Correspondence and requests for materials should be addressed to M.S.S.

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This work was primarily funded by a 2015 US Air Force Office of Scientific Research (AFOSR) Multi University Research Initiative (MURI) grant on Foldable and Adaptive Two-Dimensional Electronics (FATE) at MIT, Harvard University and University of Southern California (award no. FA9550-15-1-0514). The authors acknowledge characterization support from The MIT Center for Materials Science and Engineering, and support for graphene synthesis and characterization from the Army Research Office and support via award no. 64655-CH-ISN to the Institute for Soldier Nanotechnologies. P.L. acknowledges the ‘One-hundred Talents Program’ of Zhejiang University. A.T.L. acknowledges the MIT Presidential Fellow programme. D.K. is supported by a Grant-in-Aid for JSPS Fellows (JSPS KAKENHI grant no. 15J07423) and Encouragement of Young Scientists (B) (JSPS KAKENHI grant no. JP16K17485) from the Japan Society for the Promotion of Science. V.B.K. is supported by The Swiss National Science Foundation (project no. P2ELP3_162149).

Author information

P.L., A.T.L. and M.S.S. conceived of the experiments and wrote the paper. P.L., A.T.L. and M.S.S. performed experiments and data analysis. P.L., A.T.L. and M.S.S. designed the physical models to explain the controlled fracture of 2D materials. A.T.L. and M.S. performed the calculations and finite-element simulation. D.K. assisted in fluorescence characterization of the microparticles with MoS2 layers, J.D. assisted with the inkjet printing, and J.F.Y. performed statistical analyses for the memristor data to generate Fig. 3i. V.B.K. assisted with building the memristor function of the microparticles. S.W. and Y.S. assisted in the growth and transfer of 2D materials. M.H.W. set up the flow cell used to track liquid-phase particle translocation. All authors have given their approval to the final version of the manuscript.

Competing interests

The authors declare no competing interests.

Correspondence to Michael S. Strano.

Supplementary information

Supplementary Information

Supplementary Figures 1–60, Supplementary Table 1, Supplementary References 1–23.

Supplementary Video 1

Strain guided fracture propagation of graphene with stochastic seed crack formation.

Supplementary Video 2

Finite element coarse grained MD simulation for mould-based graphene folding.

Supplementary Video 3

Autoperforation for G-PS-G microparticles—lift-off process on SiO2-Si substrate—I.

Supplementary Video 4

Autoperforation for G-PS-G microparticles—lift-off process on SiO2-Si substrate—II.

Supplementary Video 5

Autoperforation for G-PS-G microparticles—lift-off process on PDMS substrate.

Supplementary Video 6

Control—lift-off process of PS control microparticles without grapheme.

Supplementary Video 7

Flowing and rotating of G-PS-G microparticles in microfluidic channel.

Supplementary Video 8

Magnetic propulsion of Gr-Fe3O4-PS-Gr microparticles.

Supplementary Video 9

Autoperforation for G-PS microparticles with only one layer of graphene (Graphene A).

Supplementary Video 10

Autoperforation for PS-G microparticles with only one layer of graphene (Graphene B).

Supplementary Video 11

The whole process starting from autoperforation, capturing, information write in, lift-off, recapturing to information readout.

Supplementary Video 12

Aerosolization of G-PS-G microparticles with atomizer.

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Further reading

Fig. 1: Autoperforation of 2D materials to generate colloidal microparticles with 2D surfaces.
Fig. 2: Characterization of microparticles after liftoff.
Fig. 3: Electrical properties and memristive characteristics of the graphene (bilayer) microparticles.
Fig. 4: G-PS-G microparticles as a platform to sense and record environmental information.