Electrical measurement of single molecule catalysis using carbon nanotubes
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Electrical Measurement of Single Molecule Catalysis using Carbon Nanotubes. Brett Goldsmith , Alexander Kane, Vaikunth Khalap , John Coroneus , Gregory Weiss, Phil Collins Department of Physics and Astronomy University of California Irvine. Outline. Single Molecule Sensor Construction

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Electrical measurement of single molecule catalysis using carbon nanotubes

Electrical Measurement of Single Molecule Catalysis using Carbon Nanotubes

Brett Goldsmith, Alexander Kane, VaikunthKhalap,

John Coroneus, Gregory Weiss, Phil Collins

Department of Physics and Astronomy

University of California Irvine


Outline
Outline Carbon Nanotubes

  • Single Molecule Sensor Construction

  • Measurement of Catalysis Reaction Rate

  • Dynamics of the Bound State


Single molecule sensors
Single Molecule Sensors Carbon Nanotubes

Ensemble

Stochastic

binding analyte absent

binding analyte absent

absent

absent

present

present


Device construction
Device Construction Carbon Nanotubes

Source

PMMA

PMMA

Drain

Coroneus, et al.Chem. Phys. Chem. accepted

Goldsmith, et al.Science2007, 315, 77.


Device characterization
Device Characterization Carbon Nanotubes


The catalysis reaction
The Catalysis Reaction Carbon Nanotubes

EDC

attached EDC

urea

+

+

EDC binds to the carboxyl group on the nanotube.

The bound EDC perturbs the current in the nanotube.

A reaction with water releases the bound EDC as a mixed urea.



Interaction with edc
Interaction With EDC Carbon Nanotubes

Goldsmith et al.Nano Lett.,8 (1), 189 -194, 2008


Interaction with edc1
Interaction With EDC Carbon Nanotubes

Turnover Time

Time Bonded

Waiting Time


Single molecule rate constant
Single Molecule Rate Constant Carbon Nanotubes

Turnover Time

Time Bonded

Waiting Time

k-1= 58.9 ± 18.3 s


Bound state lifetime
Bound State Lifetime Carbon Nanotubes

Bound State Lifetime:

<tbound> = 12.4 ± 2.1 s

k-1= 58.9 ± 18.3 s


Bound vs unbound
Bound vs. Unbound Carbon Nanotubes


Dynamics of the bound state
Dynamics of the Bound State Carbon Nanotubes


Energy of a two level system
Energy of a Two Level System Carbon Nanotubes

DE = kBTln(<tlo>/<thi>)

~11% of these states are

very different


Energy of a two level system1
Energy of a Two Level System Carbon Nanotubes

90%

10%

at experimental pH = 4.5



Summary
Summary Carbon Nanotubes

Goldsmith, et al.Science2007, 315, 77.

Goldsmith et al.Nano Lett.,8 (1), 189 -194, 2008

Goldsmith et al.JMR, accepted

Coroneus, et al.Chem. Phys. Lett., accepted

Dr. Phil Collins

Brett Goldsmith

Alex Kane

Bucky Khalap

Steve Hunt

Danny Wan

Tatyana Sheps

Dr. Gregory Weiss

John Coroneus

ACS-PRF


Other samples
Other Samples… Carbon Nanotubes

EDC

Pthalic Anhydride

JMR…



Amplitude of the two level system
Amplitude of the Two Level System Carbon Nanotubes

The amplitude of the two groups of bound states also differs.

These different bound state properties could be due to the ~10% protonated EDC in solution at our conditions.


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