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Herein, a novel transmission electron microscopy (TEM) method that allows high-resolution imaging and spectroscopy of nanomaterials under simultaneous application of different stimuli, such as light excitation, has been reported to directly explore structure-activity relationships targeted towards device optimization. However, the experimental development of a photoelectric system capable of combining atomic-level visualization with simultaneous electrical current measurement with picoampere-precision still remains a great challenge due to light-induced drift while imaging and noise in the electrical components due to background current. Herein, we report a novel photoelectric TEM holder integrating an LED light source covering the whole visible range, a shielding system to avoid current noise, and a picoammeter, which enables stable TEM imaging at the atomic scale while measuring very small photocurrents (pico ampere range).

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