Real-Time Video Imaging of Mechanical Motions of a Single Molecular Shuttle with Sub-Millisecond Sub-Angstrom Precision

Abstract

Miniaturized machines have open up a new dimension of chemistry, studied usually as an average over numerous molecules or for a single molecule bound on a robust substrate. Mechanical motions at a single molecule level, however, are under quantum control, strongly coupled with fluctuations of its environment — a system rarely addressed because an efficient way of observing the nanomechanical motions in real time is lacking. Here, we report sub-millisecond sub-Å precision in situ video imaging of a single fullerene molecule shuttling, rotating, and interacting with a vibrating carbon nanotube at 0.625 milliseconds(ms)/frame or 1600 fps, using an electron microscope, a fast camera, and a denoising algorithm. We have achieved in situ observation of the mechanical motions of a molecule coupled with vibration of a carbon nanotube with standard error as small as 0.9 millisecond in time and 0.01 nm in space. We have revealed rich molecular dynamics, where motions are non-linear, stochastic and often non-repeatable, and a work and energy relationship at a molecular level previously undetected by time-averaged measurements or microscopy. The molecular video recording at a 1600-fps rate exceeds by 100 times the previous records of continuous recording of molecular motions.

Ultra-Fast Electron Microscopic Imaging of Single Molecules With a Direct Electron Detection Camera and Noise Reduction

“…The Chambolle algorithm was also effective in denoising high framerate video datasets. The method reduced the need for image superimposition, thus preserving the details of high-speed phenomenon (Shimizu et al, 2020). Additionally, when necessary, Chambolle superimposition allowed frames to be superimposed with less motion blur than pixel averaging superimposition.…”

Progress in Molecular Nanoarchitectonics and Materials Nanoarchitectonics

“…Real-time recordings of nanoscale motions are realized using a fast camera with the aid of a denoising algorithm. Nanoarchitectonics design of entrapped fullerene molecules (C 60 molecules) within a carbon tube revealed shuttling and rotating behaviours of a single C 60 molecule ( Figure 2 ) [ 69 ]. The molecular motions are coupled with carbon nanotube vibrations and can be observed in real-time mode with spatial resolution of 0.01 nm and standard error in time of 0.9 msec.…”

Nanoarchitectonics for Hierarchical Fullerene Nanomaterials

“…Undoubtedly, the preparation and fabrication of high-performance materials are crucial issues. Based on analyses and characterizations with high-resolution techniques upon advanced nanotechnology [ 25 , 26 , 27 ], the importance of the regulation of nanoscale structures for better functions has been revealed [ 28 , 29 , 30 ]. Accordingly, nanoscale materials sciences have been paid much attention.…”