brett goldsmith, alexander kane, vaikunth khalap, john coroneus, gregory weiss, phil collins...
TRANSCRIPT
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Brett Go ldsmith , A l exander Kane , Va i kun th Kha lap , J ohn Coroneus , Gregory We i ss , Ph i l Co l l i n s
Depar tment o f Phys i cs and As t ronomyUn iver s i t y o f Ca l i f o rn i a I r v ine
Electrical Measurement of Single Molecule Catalysis using Carbon Nanotubes
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Outline
Single Molecule Sensor Construction
Measurement of Catalysis Reaction Rate
Dynamics of the Bound State
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Single Molecule Sensors Ensemble Stochastic
present absent
binding analyte absent present absent
binding analyte absent
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Device Construction
ReferenceCounter
Source Drain
PMMAcoating
Electrolytedrop
PMMA
PMMA
Source
Drain
Coroneus, et al. Chem. Phys. Chem. accepted
Goldsmith, et al. Science 2007, 315, 77.
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Device Characterization
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The Catalysis Reaction
EDC binds to the carboxyl group on the nanotube.
EDC
+ +
attached EDC urea
The bound EDC perturbs the current in the nanotube.
A reaction with water releases the bound EDC as a mixed urea.
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Functionalized CNTs in Buffer
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Interaction With EDC
Goldsmith et al. Nano Lett., 8 (1), 189 -194, 2008
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Interaction With EDC
Time Bonded Waiting Time
Turnover Time
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Single Molecule Rate Constant
Time Bonded Waiting Time
Turnover Time
k-1= 58.9 ± 18.3 s
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Bound State Lifetime
k-1= 58.9 ± 18.3 s
Bound State Lifetime:<tbound> = 12.4 ± 2.1 s
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Bound vs. Unbound
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Dynamics of the Bound State
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Energy of a Two Level System
DE = kBT ln(<tlo>/<thi>)
~11% of these states arevery different
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Energy of a Two Level System
90%
10%
at experimental pH = 4.5
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Reaction Intermediate States
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Summary
Dr. Phil CollinsBrett GoldsmithAlex KaneBucky KhalapSteve HuntDanny WanTatyana Sheps
Dr. Gregory WeissJohn Coroneus
ACS-PRF
Goldsmith, et al. Science 2007, 315, 77.
Goldsmith et al. Nano Lett., 8 (1), 189 -194, 2008
Goldsmith et al. JMR, accepted
Coroneus, et al. Chem. Phys. Lett., accepted
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Other Samples…
EDC Pthalic Anhydride
JMR…
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Timescale of the Two Level System
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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.