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

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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

  • Single Molecule Sensor Construction

  • Measurement of Catalysis Reaction Rate

  • Dynamics of the Bound State


Single molecule sensors

Single Molecule Sensors

Ensemble

Stochastic

binding analyte absent

binding analyte absent

absent

absent

present

present


Device construction

Device Construction

Source

PMMA

PMMA

Drain

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

Goldsmith, et al.Science2007, 315, 77.


Device characterization

Device Characterization


The catalysis reaction

The Catalysis Reaction

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.


Functionalized cnts in buffer

Functionalized CNTs in Buffer


Interaction with edc

Interaction With EDC

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


Interaction with edc1

Interaction With EDC

Turnover Time

Time Bonded

Waiting Time


Single molecule rate constant

Single Molecule Rate Constant

Turnover Time

Time Bonded

Waiting Time

k-1= 58.9 ± 18.3 s


Bound state lifetime

Bound State Lifetime

Bound State Lifetime:

<tbound> = 12.4 ± 2.1 s

k-1= 58.9 ± 18.3 s


Bound vs unbound

Bound vs. Unbound


Dynamics of the bound state

Dynamics of the Bound State


Energy of a two level system

Energy of a Two Level System

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

~11% of these states are

very different


Energy of a two level system1

Energy of a Two Level System

90%

10%

at experimental pH = 4.5


Reaction intermediate states

Reaction Intermediate States


Summary

Summary

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…

EDC

Pthalic Anhydride

JMR…


Timescale of the two level system

Timescale of the Two Level System


Amplitude of the two level system

Amplitude of the Two Level System

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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