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in. 1 nm. Water in Nanopores. CCP5 Summer School 2002. Oliver Beckstein Laboratory of Molecular Biophysics, Oxford. Gating and Water Transport. Hydrophobic rings ( MscL , KcsA , nAChR ). Water pores ( Aqp , GlpF ). N. Unwin (2000). Model System. R M =10 Å. z. L M = 4 Å. L p =8 Å. - PowerPoint PPT Presentation

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in

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1 nm

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Oliver BecksteinLaboratory of Molecular Biophysics, Oxford

Water in NanoporesCCP5 Summer School 2002

Page 6: 1 nm

Gating and Water Transport

Hydrophobic rings (MscL, KcsA, nAChR)

Water pores (Aqp, GlpF)

N. Unwin (2000)

Page 7: 1 nm

Model System

MolecularDynamics

• CH4 spheres (hydrophobic)

• RMSD 1 Ă• GROMACS

RM=10 Å

Lp=8 Å

LM=4 Åz

Rp

Page 8: 1 nm

Pore Occupancy Fluctuations

Middle: Rp=5.5 Å

Rp=6 Å

Rp=5 Å

Page 9: 1 nm

Openness

Open state =1

Closed state =0

T

Topen

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Pore Occupancy Fluctuations

Rp=5.5 Å <>=0.28

Rp=6 Å <>=0.77

Rp=5 Å

<>=0.17

Page 11: 1 nm

“Capillary Condensation”

empty,closed

filled,open

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Water in Narrow Pores

•Dynamics (diffusion)• Kinetics (open/close times)• Free energy, chemical potential

Page 13: 1 nm

Kinetics

=1/kBT

Disruption of closed

state: close

Disruption of open

state: open

kin

open

closeeq

FeK

openclosekin FFF

eqK

open closed

Page 14: 1 nm

Pore Occupancy Distribution

)(ln),,( NPNVTF

Page 15: 1 nm

Free Energy of Water in a Nanopore

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Pore, Bulk

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Pore, Bulk, Vapour

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F (Rpore=6.0 Å)

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F (Rpore=5.5 Å)

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F (Rpore=5.0 Å)

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F (Rpore=4.5 Å)

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Free Energy F

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Free Energy Density f

V

NVTFnTf

),,(),(

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Chemical Potential

n

nTfnT

),(

),(

(neq) = 0:neq= 1.035 n0

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Equilibrium and Geometry

eqK

open closed

#

#

)(

)(

openclose

NN

NN

NP

NP

FFF

R

RF

)Å4.05.2(

)5.20.14()(1-

)](exp[)(eq RFRK

Page 26: 1 nm

What happens?• Two independent processes:

– Filling (ends the closed state): close

– Emptying (ends the open state): open

Occupancy fluctuations• Filling water evaporation

R independent

• Emptying rupture of hydrogen- bond network by waterfluctuations (“bubbles”)

volume dependent

Page 27: 1 nm

Summary/Biology…

N. Unwin (2000)

nAChR Hydrophobic Gating

~20 Å

R 1.4 Å Aqp/GlpF Water transport•“bulk” stabilisation: amphipathic pore

•Fast diffusion (“greasy slide”)

Page 28: 1 nm

The Future…•Long term water

behaviour in more complex geometries: approximating aqp, nAChR

•Theoretical understanding (thermodynamics)

•Behaviour of ions?

With the help of…Mark SansomJosé Faraldo Gómez

Phil Biggin

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Hydrophobic Gating…

RM

Rp

R RGeometry

z

Page 31: 1 nm

…+ Hydrophilic Pore Lining…

Dipole strength peptide bond dipole

apolar polar

Pore lining

Page 32: 1 nm

…+ Hydrophobic Pore Lining

closed open

R RGeometry

apolar polar

Pore lining

OB, P. C. Biggin, M.S.P. Sansom, J. Phys. Chem. B 105 (2001)

Dipole strength peptide bond dipole

GATED

Page 33: 1 nm

Water in Narrow Pores

•Dynamics (diffusion)• Kinetics (open/close times)• Free energy

z


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