Methods of Synthesis and Characterization of Conductive DNA Nanowires Based on Metal Ion-Mediated Base Pairing for Single-Molecule Electronics

Authors

  • Simon Vecchioni Department of Biomedical Engineering at Columbia University, New York, NY 10027, USA
  • Mark C. Capece Department of Chemistry, Stanford University, Stanford, CA 94305, USA
  • Emily Toomey Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
  • Lynn Rothschild NASA Ames Research Center, Space Science and Astrobiology Division, Moffett Field, CA 94035, USA
  • Shalom J. Wind Department of Applied Physics and Applied Mathematics at Columbia University, New York, NY 10027, USA

DOI:

https://doi.org/10.13052/jsame2245-4551.6.004

Keywords:

Molecular electronics, DNA nanowire, nanomaterials, cytosine mismatch, methods.

Abstract

Advances in the field of molecular electronics have made possible the direct
measurement of charge transport across single molecules. In particular, work
on DNA oligomers has demonstrated that this weakly-conducting biomolecule
can be functionalized through metal-mediated nucleobase pairing in order to
significantly increase electron mobility across the molecule. The introduction
of interacting stacks of single metal ions inside the DNA helix is an attractive
platform for assay and optimization; for this reason we present a protocol
for the production and processing of nanowires with a metal base pair for
single-molecule applications. In particular, we describe the construction of DNA duplex wires with a cytosine-Ag+-cytosine base pair (dC:Ag+:dC).
A thorough investigation of buffer components suggests the use of divalent
magnesium counterions to stabilize highly mismatched oligonucleotides in
solution. We further analyse cleaning and processing of thin gold films for
batch-fabrication of conductive imaging substrates for use in conductive
scanning probe assays of single-molecule conductivity. With a clear path to
electrical assays, we suggest that the C:Ag+:C orthogonal nucleotide pair and
other similar chemistries may provide a foundation for molecular electronic
components in integrated devices

Downloads

Download data is not yet available.

Author Biographies

Simon Vecchioni, Department of Biomedical Engineering at Columbia University, New York, NY 10027, USA

Simon Vecchioni received his B.S. in Biology from Brown University in 2013.
That same year he joined the laboratory of Lynn Rothschild at NASA Ames
Research Center to investigate the biosynthesis of electronic materials. After
moving to Columbia University in New York to pursue a Ph.D. in Biomedical
Engineering, he joined the group of Shalom Wind to focus on nanoscale self-
assembly and DNA nanotechnology. Since 2014, he has been supported by a
NASA Space Technology Research Fellowship and has continued to pursue
work on DNA nanoelectronics with the support of Wind and Rothschild.

Mark C. Capece, Department of Chemistry, Stanford University, Stanford, CA 94305, USA

Mark C. Capece earned a B.S. in Chemistry and Physics from the University
of Louisville in 2011, where his honors thesis demonstrated the practical
lumped-element design of a magic angle spinning triple-resonance solid-
state NMR probe. He then received a Ph.D. in Chemistry from Stanford
University in 2018. His graduate work used solution NMR and single-
molecule fluorescence to model functional mRNA structures that regulate
translation. Capece’s research interests continue to focus on NMR technology
development and biological applications.

Emily Toomey, Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA 02139, USA

Emily Toomey received her Sc.B. in Electrical Engineering from Brown
University in 2015, where she studied the electrical characterization of DNA
in the laboratory of Prof. Jimmy Xu. She had previously interned at the
NASA Ames Research Center under Dr. Lynn Rothschild in 2013, where
she explored the modification of DNA structures by metal ion intercalation
in collaboration with Simon Vecchioni. Emily has been pursuing a Ph.D.
in Electrical Engineering from the Massachusetts Institute of Technology
since 2015. Her current work under Prof. Karl K. Berggren focuses on
superconducting nanoelectronics and nanofabrication.

Lynn Rothschild, NASA Ames Research Center, Space Science and Astrobiology Division, Moffett Field, CA 94035, USA

Lynn Rothschild is passionate about the origin and evolution of life on Earth
or elsewhere, while at the same time pioneering the use of synthetic biology
to enable space exploration. She is a senior scientist NASA’s Ames Research
Center, as well as Adjunct Professor at Brown University. Since 2011 she
has been the faculty advisor of the award-winning Stanford-Brown iGEM
team, which has pioneered the use of synthetic biology to accomplish NASA’s
missions, focusing on the human settlement of Mars, astrobiology and such
innovative projects as BioWires, making a biodegradable UAS (drone) and
using fungal mycelia as a building material. She is a fellow of the Linnean
Society of London, The California Academy of Sciences and the Explorer’s
Club

Shalom J. Wind, Department of Applied Physics and Applied Mathematics at Columbia University, New York, NY 10027, USA

Shalom J. Wind received his Ph.D. in Physics from Yale University in
1987. Following his doctoral studies, he worked at IBM’s Thomas J. Watson
Research Center, focusing primarily on nanoelectronic devices. He moved to
the Department of Applied Physics and Applied Mathematics at Columbia
University in 2003. Wind’s present research focuses on molecular-scale
fabrication and the interface between biological and technological materials
and systems.

References

E. Braun, et al. ‘DNA-templated assembly and electrode attachment of

a conducting silver wire’, Nature, 391(6669):775–778, 1998.

L. Montagnier, et al. ‘Electromagnetic signals are produced by aqueous

nanostructures derived from bacterial DNA sequences’, Interdisciplinary

Sciences: Computational Life Sciences, 1(2):81–90, 2009.

A. Storm, et al. ‘Insulating behavior for DNA molecules between

nanoelectrodes at the 100 nm length scale’, Applied Physics Letters,

(23):3881–3883, 2001.

A. Y. Kasumov, et al. ‘Proximity-induced superconductivity in DNA’,

Science, 291(5502): 280–282,2001.

G. I. Livshits, et al. ’Long-range charge transport in single G-quadruplex

DNA molecules’, Nature Nanotechnology, (9): 1040–1046, 2014.

L. Xiang, et al. ‘Intermediate tunnelling–hopping regime in DNA charge

transport’, Nature Chemistry, 7(3):221–226, 2015.

L. Venkataraman, et al. ‘Dependence of single-molecule junction conduc-

tance on molecular conformation’, Nature, 442(7105):904–907, 2006.

C. Bruot, et al. ‘Effect of mechanical stretching on DNA conductance’,

ACS Nano, 9(1):88–94, 2014.

B. Xu, et al. ‘Direct conductance measurement of single DNA molecules

in aqueous solution’, Nano Letters, 4(6):1105–1108, 2004.

E. Toomey, et al. ‘Comparison of Canonical versus Silver(I)-Mediated

Base-Pairing on Single Molecule Conductance in Polycytosine dsDNA’,

Journal of Physical Chemistry C, 120(14):7804–7809, 2016.

H. Torigoe, et al. ‘Thermodynamic and structural properties of the

specific binding between Ag(+) ion and C:C mismatched base pair in

Methods of Synthesis and Characterization of Conductive DNA Nanowires 87

duplex DNA to form C-Ag-C metal-mediated base pair’, Biochimie,

(11):2431–2440, 2012.

Y. Miyake, et al. ‘MercuryII-mediated formation of thymine-HgII-

thymine base pairs in DNA duplexes’, Journal of the American Chemical

Society, 128(7):2172–2173, 2006.

S. Johannsen, et al. ‘Solution structure of a DNA double helix with con-

secutive metal-mediated base pairs’, Nature Chemistry, 2(3):229–234,

G. H. Clever, M. Shionoya, ‘Metal-base pairing in DNA’, Coordination

Chemistry Reviews, 254(19–20): 2391–2402, 2010.

V. B. Pinheiro, P. Holliger, ‘Towards XNA nanotechnology: new

materials from synthetic genetic polymers’, Trends in Biotechnology,

(6):321–328, 2014.

H. Yamaguchi, et al. ‘The structure of metallo-DNA with consecutive

thymine-HgII-thymine base pairs explains positive entropy for the met-

allo base pair formation’, Nucleic Acids Research, 42(6):4094–4099,

S. S. Mallajosyula, S. K. Pati, ‘Conformational tuning of magnetic inter-

actions in metal–DNA complexes’, Angewandte Chemie, 121(27):5077–

, 2009.

S. Roche, ‘Sequence dependent DNA-mediated conduction’, Physical

Review Letters, 91(10):108101, 2003.

S. S. Mallajosyula, S. K. Pati, ‘Toward DNA conductivity: a theoretical

perspective’, The Journal of Physical Chemistry Letters, 1(12):1881–

, 2010.

H. Torigoe, et al. ‘Thermodynamic properties of the specific binding

between Ag+ ions and C:C mismatched base pairs in duplex DNA’,

Nucleotides, Nucleosides and Nucleic Acids, 30:149–167, 2011.

S. M. Swasey, et al. ‘Silver (I) as DNA glue: Ag+-mediated guanine

pairing revealed by removing Watson-Crick constraints’, Scientific

reports, 5: 10163, 2015.

L. Venkataraman, et al. ‘Single-molecule circuits with well-defined

molecular conductance’, Nano Letters, 6(3):458–462, 2006.

A. Ono, et al. ‘Specific interactions between silver(I) ions and cytosine-

cytosine pairs in DNA duplexes’, Chemical Communications (Cam-

bridge), (39):4825–4827, 2008.

N. Peyret, et al. ‘Nearest-neighbor thermodynamics and NMR of

DNA sequences with internal A.A, C.C, G.G, and T.T mismatches’,

Biochemistry, 38(12):3468–3477, 1999.

S. Vecchioni et al.

R. Owczarzy, et al. ‘Predicting stability of DNA duplexes in solu-

tions containing magnesium and monovalent cations’, Biochemistry,

(19):5336–5353, 2008.

J.-L. Leroy, et al. ‘Intramolecular folding of a fragment of the cytosine-

rich strand of telomeric DNA into an i-motif’, Nucleic Acids Research,

(9):1600–1606, 1994.

C. M. Ritchie, et al. ‘Ag nanocluster formation using a cytosine oligonu-

cleotide template’, Journal of Physical Chemistry C, 111(1):175–181,

H. T. Allawi, J. SantaLucia, ‘Thermodynamics and NMR of internal

G⊙T mismatches in DNA’, Biochemistry, 36(34):10581–10594, 1997.

C. Nogues, M. Wanunu, ‘A rapid approach to reproducible, atomically

flat gold films on mica’, Surface Science, 573(3): L383-L389, 2004.

U. Maver, et al. ‘Preparation of Atomically Flat Gold Substrates for AFM

Measurements’, Acta Chimica Slovenica, 59(1), 2012.

T. Someya, et al. ‘Alcohol vapor sensors based on single-walled carbon

nanotube field effect transistors’, Nano Letters, 3(7):877–881, 2003.

D. Zikich, et al. ‘I-Motif Nanospheres: Unusual Self-Assembly of Long

Cytosine Strands’, Small, 7(8):1029–1034, 2011.

Downloads

Published

2023-03-18

How to Cite

Vecchioni, S., Capece, M. C., Toomey, E., Rothschild, L., & Wind, S. J. (2023). Methods of Synthesis and Characterization of Conductive DNA Nanowires Based on Metal Ion-Mediated Base Pairing for Single-Molecule Electronics. Journal of Self Assembly and Molecular Electronics, 6(1), 61–90. https://doi.org/10.13052/jsame2245-4551.6.004

Issue

Section

Articles