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Published May 2013 | Supplemental Material
Journal Article Open

Single-nanoparticle phase transitions visualized by four-dimensional electron microscopy


The advancement of techniques that can probe the behaviour of individual nanoscopic objects is of paramount importance in various disciplines, including photonics and electronics. As it provides images with a spatiotemporal resolution, four-dimensional electron microscopy, in principle, should enable the visualization of single-nanoparticle structural dynamics in real and reciprocal space. Here, we demonstrate the selectivity and sensitivity of the technique by visualizing the spin crossover dynamics of single, isolated metal–organic framework nanocrystals. By introducing a small aperture in the microscope, it was possible to follow the phase transition and the associated structural dynamics within a single particle. Its behaviour was observed to be distinct from that imaged by averaging over ensembles of heterogeneous nanoparticles. The approach reported here has potential applications in other nanosystems and those that undergo (bio)chemical transformations.

Additional Information

© 2013 Macmillan Publishers Limited. Received 27 November 2012; Accepted 06 March 2013; Published online 14 April 2013. This work was supported by the National Science Foundation and the Air Force Office of Scientific Research in the Gordon and Betty Moore Center for Physical Biology at the California Institute of Technology. R.M.V. acknowledges funding from the Swiss National Science Foundation. We thank S. Tae Park for helpful collaboration in the phase-transition simulations, which will be published later in a full report. Author contributions: R.M.V., O.H.K. and A.H.Z. conceived and designed the experiments. R.M.V. and O.H.K. performed the experiments. A.H. and A.M.T. contributed materials and performed sample characterization. R.M.V., O.H.K., A.M.T., A.H. and A.H.Z. discussed the results and commented on the manuscript.

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