workshop on hpc in india chemical dynamics in aqueous media amalendu chandra department of...
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Workshop on HPC in India
Chemical Dynamics in Aqueous Media
Amalendu ChandraDepartment of Chemistry, Indian
Institute of Technology Kanpur, India 208016
ATIP 1st Workshop on HPC in India @ SC-09
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Hydrogen bonded (tetrahedral) structure of water
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Hydrogen bond fluctuations in water and aqueous solutions
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Excess proton in water
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Experimental Methods
X-ray and Neutron Scattering Low frequency Raman ( < 200 cm-1) Time Resolved Infrared Spectroscopy
Transient hole burning studies using IR laser
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Pump-probe signal at different delay times
Variation of H-bond distance with time
Relaxation time ~ 1.0 psG.M.Gale etal PRL, 82, 1068 (1999)
= ~ 100-200 fs, ~ 1-2 ps A. Tokmakoff and coworkers JCP (2005) M.D. Fayer and coworkers, PNAS (2007)
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Computation of Aqueous Systems
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Ab initio Molecular Dynamics
Forces are calculated from electronic structure calculation that areperformed on-the-fly as the MD trajectory is generated.Car-Parrinello Method:
R. Car and M. Parrinello, Phys. Rev. Lett., 55, 2471 (1985) J. Hutter et al. CPMD, MPI Stuttgart and IBM Zurich
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A. Chandra and coworkers, JPC/A (2008); JCP (2008)
OH stretch frequency vs time in OH stretch frequency vs time in liquid waterliquid water
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Frequency vs hydrogen bond distance Frequency vs hydrogen bond distance (pure D(pure D22OO))
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Dynamics of vibrational spectral diffusion:
Hole creation and subsequent dynamics from Hole creation and subsequent dynamics from nonequilibrium probability distributionsnonequilibrium probability distributions
Hole creation: Monte Carlo algorithm
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Dynamics after hole creation: Excitation in Dynamics after hole creation: Excitation in blue/redblue/red
Experiments:G.M. Gale et al PRL (1999)
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Time dependence of average frequency after Time dependence of average frequency after hole creationhole creation
1 ~ 100 fs (dynamics of intact hydrogen bonds) 2 ~ 2 ps (lifetimes of hydrogen bonds) s ~ 100 cm-1 (intermolecular stretching/bending vibrations)
A. Chandra and coworkers, JPC/A (2008); JCP (2009)
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ScH2OSupercritical Supercritical waterwater
673K/0.0221
573K/0.0338423K/0.0334298K/0.0334
A.K Soper et al., JCP, 106, 249 (1996)A.K Soper et al., JCP, 106, 249 (1996)
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Correlations between OD frequency and D..O distance
A. Chandra and coworkers,JPC/A (2008)
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Proton Transfer in Proton Transfer in waterwaterEigen Eigen Zundel Zundel
complexcomplex
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Mobility of H3O+ in liquid
water
D H3O+
= 9.31x10-5 cm2/s
DH2O = 2.30x10-5 cm2/s
Mobility of OH- in liquid water
D OH_ = 5.3x10-5 cm2/s
M.E. Tuckerman, D.Marx and M. Parrinello, Nature, 417, 925 (2002)A.Chandra, M. Tuckerman and D.Marx, PRL (2007); Acc. Chem. Res. (2006)
Proton Migration Dynamics
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Protonic defects in water clusters
Where is the protonic defect located?Is there any proton transfer in clusters?
A. Bankura and A. Chandra, JCP (submitted)
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Describes chemically relevant part of large system using quantum mechanics (QM) and rest by molecular mechanics (MM)
QM/MM Technique
Long Range (LR)
Short Range (SR)
QM Density
H3O+/OH- in different carbon nanotube systems
Effects of confinement
Quantum-classical simulations
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Financial support:DST, CSIR, BRNS, MCIT (Government of India)AvH Foundation (Germany)
Group members:
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IIT Kanpur ….