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Precise electrokinetic position and three-dimensional orientation control of a nanowire bioprobe in solution

Abstract

Owing to Brownian-motion effects, the precise manipulation of individual micro- and nanoparticles in solution is challenging. Therefore, scanning-probe-based techniques, such as atomic force microscopy, attach particles to cantilevers to enable their use as nanoprobes. Here we demonstrate a versatile electrokinetic trap that simultaneously controls the two-dimensional position with a precision of 20 nm and 0.5° in the three-dimensional orientation of an untethered nanowire, as small as 300 nm in length, under an optical microscope. The method permits the active transport of nanowires with a speed-dependent accuracy reaching 90 nm at 2.7 μm s–1. It also allows for their synchronous three-dimensional alignment and rotation during translocation along complex trajectories. We use the electrokinetic trap to accurately move a nanoprobe and stably position it on the surface of a single bacterial cell for sensing secreted metabolites for extended periods. The precision-controlled manipulation underpins developing nanorobotic tools for assembly, micromanipulation and biological measurements with subcellular resolution.

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Fig. 1: Design and working principle of the electrokinetic trap.
Fig. 2: Angle-dependent precise manipulation.
Fig. 3: High-precision angular manipulation and optimization.
Fig. 4: High-precision trajectories with in-plane and out-of-plane control.
Fig. 5: 3D-oriented precision manipulation and assembling.
Fig. 6: Localized detection of metabolites from a single E. coli cell with SERS-active nanocapsule sensors.

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Data availability

All experimental data for the figures in the manuscript are available via Zenodo at https://doi.org/10.5281/zenodo.7765045. Source data are provided with this paper.

Code availability

The codes used for the imaging analysis are available via Zenodo at https://doi.org/10.5281/zenodo.7765045.

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Acknowledgements

This project is supported by the US National Science Foundation (NSF) 1710922 and 1930649 with INTERN, and Welch Foundation F-1734. This project also received partial support from NSF 2219221. H.K. and P.F. acknowledge support from the Max Planck–EPFL Center for Molecular Nanoscience and Technology. We thank B. Lian and S.-I. Hsueh for technical assistance and E. Zumalt for drawing the schematics in Figs. 1 and 6b.

Author information

Authors and Affiliations

Authors

Contributions

D.F. conceived the concept and approach and supervised the project. H.L. carried out the experiments, data analysis and theoretical calculation, with assistance from D.H. and A.J. D.T. designed and assembled the nanomanipulation system and programmed the software. Z.L. co-developed the system. H.K. and P.F. fabricated the 50-nm-tipped nanopens. H.L., D.F. and P.F. wrote the paper, and all authors confirmed its final form.

Corresponding author

Correspondence to Donglei Emma Fan.

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The authors declare no competing interests.

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Nature Nanotechnology thanks Natan Osterman and Allison Squires for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Electric voltage signals for different control modes.

Voltage signals for different control modes.

Extended Data Fig. 2 Schematic shows the synchronous control of position, orientation, and rotation of a nanowire along a sophisticated trajectory with prescribed temporal control.

A schematic showing the synchronously executed controls for position, orientation, and rotation of the nanowire along a sophisticated trajectory with precise temporal control.

Extended Data Fig. 3 Diffusion coefficients of nanowires (170 nm in diameter, ~2–7 µm in lengths) in deionized water along the a, b and x, y orthogonal directions in the body and lab frames, respectively.

(a) Diffusion coefficients of nanowires (170 nm in diameter, ~2–7 µm in lengths) in deionized water along the orthogonal a, b and x, y directions in the body and lab frames, respectively, in (b). Theoretical fit (solid lines) with the Broersma relation agrees well with experiments; the correction factors (ξ) are 0.883 and 0.801 for translational diffusivities along the long (Da) and short axis (Db), respectively.

Source data

Extended Data Fig. 4 Translational velocity of Au nanowires on different surfaces.

Translational velocity of Au nanowires with different surface treatment when 1 V is applied across a 500-μm electrode gap (Natively negatively charged NWs, zeta potential: −40.7 ± 8.8 mV; positively charged NWs, zeta potential: 40.5 ± 4.4 mV.). Data are presented as mean values ± SD. 20 measurements are made for natively negatively charged NWs, 12 measurements are made for PEG substrate, 20 measurements are made for positively charged NWs.

Source data

Extended Data Fig. 5 Precision manipulation can be readily realized for a wire either in-plane or oriented vertically when it traces a cat pattern.

The precision manipulation can be readily realized in both in-plane tracing and vertical drawing of cat.

Source data

Extended Data Fig. 6 Position error versus time during the tracing of ‘Nanopen’ at (a) 2.67 μm/s and (b) 35.6 μm/s.

Position error versus time as the nanopen traces ‘Nanopen’ at (a) 2.67 μm/s and (b) 35.6 μm/s.

Source data

Extended Data Fig. 7 Positioning manipulation precision of Au nanowires (4-μm in length) along x (σx) and y axis (σy), aligned at different angles with a rotational P control (with error bars).

Translocation manipulation precision of Au nanowires (4-μm in length) along x (σx) and y axis (σy), aligned at different angles with a rotational P control (with error bars). Data are presented as mean values ± SD. 5 nanowires are measured to derive statistics.

Source data

Extended Data Fig. 8 Zoom-in images of Fig. 4f and g.

The targeted and actual positions of the first letter ‘N’ in the ‘Nanopen’ trajectories when the velocity is (a) 2.67 and (b) 35.6 µm/s.

Source data

Extended Data Fig. 9 Power spectra when particles experience Brownian motion, P control, and PI control for (a) position control, (b) electro-alignment angle control, and (c) electro-rotation angle control.

The wire length is 4 μm, the frame rate is 160 FPS. The power spectra of the PI control (yellow and orange dotted curves) exhibit peaks at around a few Hz, indicating an oscillation. The results agree with the working mechanism of the PI control algorithm, the oscillation of which is intrinsic and benefits the obtained agreement of the average position of the particles with the targeted position.

Source data

Extended Data Table 1 Summary of the performance of the 3D electrokinetic trap

Supplementary information

Supplementary Information

Supplementary Figs. 1–9, Notes 1–18 and Tables 1–11.

Supplementary Video 1

Comparison of behaviours of Au nanowires with simple linear a.c. voltages applied in the Z direction (one of the electrodes grounded) without theoretical analysis considering the discontinuity of the dielectric medium or voltage on the chip plane for nanoparticle manipulation. Results show that the nanoparticles move towards the microelectrodes, leaving a large depletion area. This contrasts with the results if applying the a.c. voltages on the Z-direction electrode pairs obtained by judicious analysis and modelling. The video is played at 10× speed.

Supplementary Video 2

Versatile manipulation and assembly of 3D-oriented nanowires on a substrate with UV light.

Supplementary Video 3

Trapping of a 300-nm-long nanowire (125 nm in diameter) with controlled alignment.

Supplementary Video 4

The Au nanowire moves with various gaits, including transport, alignment and continuous rotation, along with the melody of Sicilienne (Gabriel Fauré) and unveils a ballerina’s image with its trajectory.

Supplementary Video 5

A nanowire pen draws a cat in two distinct sizes when orienting in the in-plane direction and vertically.

Supplementary Video 6

Transport of a designed nanopen possessing a 50 nm Au tip and an integrated magnetic Ni segment. The movements are shown at various speeds where the nanopen writes the word ‘nanopen’.

Supplementary Video 7

Manipulation and assembly of a 5 × 2 array made of 50 Au nanosegments. The video is played at 4× speed.

Supplementary Video 8

Two manipulation modes of the advanced 3D electric manipulation system: (1) trap a particle and move the stage in a same manner to trap/tweeze the particle; (2) directly propel a particle without any (mechanical) moving parts.

Supplementary Video 9

Vertically configured Raman nanocapsule sensor scans across and holds its position on a single E. coli cell for the localized detection of metabolites released from a single bacterial cell.

Source data

Source Data Fig. 2

Source data for the plots.

Source Data Fig. 3

Source data for the plots.

Source Data Fig. 4

Source data for the plots.

Source Data Fig. 5

Source data for the particle’s trajectory.

Source Data Fig. 6

Source data for the Raman spectra.

Source Data Extended Data Fig. 3

Source data for the plot.

Source Data Extended Data Fig. 4

Source data for the plot.

Source Data Extended Data Fig. 5

Source data for the particle’s trajectory.

Source Data Extended Data Fig. 6

Source data for the plot.

Source Data Extended Data Fig. 7

Source data for the plot.

Source Data Extended Data Fig. 8

Source data for the plot.

Source Data Extended Data Fig. 9

Source data for the plot.

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Li, H., Teal, D., Liang, Z. et al. Precise electrokinetic position and three-dimensional orientation control of a nanowire bioprobe in solution. Nat. Nanotechnol. 18, 1213–1221 (2023). https://doi.org/10.1038/s41565-023-01439-7

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