Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching
Abstract
Nanoarchitectural control of matter is crucial for next-generation technologies. DNA origami templates are harnessed to accurately position single molecules; however, direct single molecule evidence is lacking regarding how well DNA origami can control the orientation of such molecules in three-dimensional space, as well as the factors affecting control. Here, we present two strategies for controlling the polar (θ) and in-plane azimuthal (Φ) angular orientations of cyanine Cy5 single molecules tethered on rationally-designed DNA origami templates that are physically adsorbed (physisorbed) on glass substrates. By using dipolar imaging to evaluate Cy5's orientation and super-resolution microscopy, the absolute spatial orientation of Cy5 is calculated relative to the DNA template. The sequence-dependent partial intercalation of Cy5 is discovered and supported theoretically using density functional theory and molecular dynamics simulations, and it is harnessed as our first strategy to achieve θ control for a full revolution with dispersion as small as ±4.5°. In our second strategy, Φ control is achieved by mechanically stretching the Cy5 from its two tethers, being the dispersion ±10.3° for full stretching. These results can in principle be applied to any single molecule, expanding in this way the capabilities of DNA as a functional templating material for single-molecule orientation control.more »
- Authors:
-
- Boise State Univ., ID (United States)
- U.S. Naval Research Lab., Washington, DC (United States)
- Boise State Univ., ID (United States); Center for Advanced Energy Studies, Idaho Falls, ID (United States)
- Publication Date:
- Research Org.:
- Boise State Univ., ID (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Department of Navy, Office of Naval Science
- OSTI Identifier:
- 1876010
- Grant/Contract Number:
- SC0020089; N00014-19-1-2615
- Resource Type:
- Accepted Manuscript
- Journal Name:
- International Journal of Molecular Sciences (Online)
- Additional Journal Information:
- Journal Name: International Journal of Molecular Sciences (Online); Journal Volume: 23; Journal Issue: 14; Journal ID: ISSN 1422-0067
- Publisher:
- MDPI
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; nanoarchitectural control; DNA origami; dipolar imaging; super-resolution microscopy; cyanine Cy5 dyes; dye intercalation; mechanical stretching; density function theory; molecular dynamics simulations; DNA-PAINT
Citation Formats
Cervantes-Salguero, Keitel, Biaggne, Austin, Youngsman, John M., Ward, Brett M., Kim, Young C., Li, Lan, Hall, John A., Knowlton, William B., Graugnard, Elton, and Kuang, Wan. Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching. United States: N. p., 2022.
Web. doi:10.3390/ijms23147690.
Cervantes-Salguero, Keitel, Biaggne, Austin, Youngsman, John M., Ward, Brett M., Kim, Young C., Li, Lan, Hall, John A., Knowlton, William B., Graugnard, Elton, & Kuang, Wan. Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching. United States. https://doi.org/10.3390/ijms23147690
Cervantes-Salguero, Keitel, Biaggne, Austin, Youngsman, John M., Ward, Brett M., Kim, Young C., Li, Lan, Hall, John A., Knowlton, William B., Graugnard, Elton, and Kuang, Wan. Tue .
"Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching". United States. https://doi.org/10.3390/ijms23147690. https://www.osti.gov/servlets/purl/1876010.
@article{osti_1876010,
title = {Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching},
author = {Cervantes-Salguero, Keitel and Biaggne, Austin and Youngsman, John M. and Ward, Brett M. and Kim, Young C. and Li, Lan and Hall, John A. and Knowlton, William B. and Graugnard, Elton and Kuang, Wan},
abstractNote = {Nanoarchitectural control of matter is crucial for next-generation technologies. DNA origami templates are harnessed to accurately position single molecules; however, direct single molecule evidence is lacking regarding how well DNA origami can control the orientation of such molecules in three-dimensional space, as well as the factors affecting control. Here, we present two strategies for controlling the polar (θ) and in-plane azimuthal (Φ) angular orientations of cyanine Cy5 single molecules tethered on rationally-designed DNA origami templates that are physically adsorbed (physisorbed) on glass substrates. By using dipolar imaging to evaluate Cy5's orientation and super-resolution microscopy, the absolute spatial orientation of Cy5 is calculated relative to the DNA template. The sequence-dependent partial intercalation of Cy5 is discovered and supported theoretically using density functional theory and molecular dynamics simulations, and it is harnessed as our first strategy to achieve θ control for a full revolution with dispersion as small as ±4.5°. In our second strategy, Φ control is achieved by mechanically stretching the Cy5 from its two tethers, being the dispersion ±10.3° for full stretching. These results can in principle be applied to any single molecule, expanding in this way the capabilities of DNA as a functional templating material for single-molecule orientation control. The experimental and modeling insights provided herein will help engineer similar self-assembling molecular systems based on polymers, such as RNA and proteins.},
doi = {10.3390/ijms23147690},
journal = {International Journal of Molecular Sciences (Online)},
number = 14,
volume = 23,
place = {United States},
year = {Tue Jul 12 00:00:00 EDT 2022},
month = {Tue Jul 12 00:00:00 EDT 2022}
}
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