TY - JOUR
T1 - Hydration and temperature interdependence of protein picosecond dynamics
JF - Physical Chemistry Chemical Physics
Y1 - 2012
A1 - Lipps, F.
A1 - Levy, S.
A1 - Markelz, A. G.
KW - Chemistry
KW - dielectric-relaxation
KW - fluctuations
KW - inelastic neutron-scattering
KW - lysozyme
KW - myoglobin
KW - percolation
KW - Physics
KW - spectra
KW - spectroscopy
KW - terahertz beams
KW - transition
KW - water
AB -
We investigate the nature of the solvent motions giving rise to the rapid temperature dependence of protein picoseconds motions at 220 K, often referred to as the protein dynamical transition. The interdependence of picoseconds dynamics on hydration and temperature is examined using terahertz time domain spectroscopy to measure the complex permittivity in the 0.2-2.0 THz range for myoglobin. Both the real and imaginary parts of the permittivity over the frequency range measured have a strong temperature dependence at >0.27 h (g water per g protein), however the permittivity change is strongest for frequencies <1 THz. The temperature dependence of the real part of the permittivity is not consistent with the relaxational response of the bound water, and may reflect the low frequency protein structural vibrations slaved to the solvent excitations. The hydration necessary to observe the dynamical transition is found to be frequency dependent, with a critical hydration of 0.19 h for frequencies >1 THz, and 0.27 h for frequencies <1 THz. The data are consistent with the dynamical transition solvent fluctuations requiring only clusters of similar to 5 water molecules, whereas the enhancement of lowest frequency motions requires a fully spanning water network.
VL - 14
SN - 1463-9076
N1 - ISI Document Delivery No.: 928AI
Times Cited: 25
Cited Reference Count: 39
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Lipps, Ferdinand Levy, Seth Markelz, A. G.
Markelz, Andrea/0000-0003-0443-4319
26
66
Royal soc chemistry
Cambridge
1463-9084
JO - Phys. Chem. Chem. Phys.Phys. Chem. Chem. Phys.
ER -
TY - JOUR
T1 - Hydration Effects on Energy Relaxation of Ferric Cytochrome C Films after Soret-Band Photoexcitation
JF - Journal of Physical Chemistry B
Y1 - 2010
A1 - Ye, S. J.
A1 - Markelz, A.
KW - Chemistry
KW - circular-dichroism
KW - conformation change
KW - dynamics
KW - ferricytochrome-c
KW - protein hydration
KW - resolved resonance raman
KW - spectroscopy
KW - unfolded states
KW - vibrational-relaxation
KW - water-molecules
AB - Protein hydration plays a critical role in protein dynamics and biological processes. Pump-probe transmission measurement has been applied to investigate the hydration effects on the energy relaxation of a heme protein ferric Cytochrome c (Cyt c) film after soret-band photoexcitation. Transient dynamics study indicates that the energy internal conversion time of similar to 300 fs is independent of hydration. The vibrationally excited electronic ground-state recovery rates show two transitions at the hydration level of h = 12.4-16.5% and 21.7-23.5%. The first transition occurs at the hydration level for the onset of an increasing ferric Cyt c flexibility while the second transition occurs at the saturated hydration level. The hydration dependence of steady-state electronic absorption spectrum results shows that the Q-band peak is nearly constant in center wavelength, but the line width surprisingly narrows with increasing hydration. For the similar to 695 nm absorbance associated with the MET80-Fe bond, the intensity increases with increasing hydration and slightly blue shifts. The 695 nm peak grows rapidly at h = 12.4% and then plateaus at h = 21.7%. This research shows that similar to 695 nm absorbance and ground-state recovery rates are sensitive to the hydration of the protein. This study will aid in understanding how hydration modulates the activity of the protein dynamics at a local level.
VL - 114
SN - 1520-6106
N1 - ISI Document Delivery No.: 681CT
Times Cited: 3
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Ye, Shuji Markelz, Andrea
Ye, Shuji/B-4479-2010
Markelz, Andrea/0000-0003-0443-4319
NSFNational Science Foundation (NSF) [PHY-0349256, DBI-2959989]; University of Science and Technology of China; Fundamental Research Funds for the Central UniversitiesFundamental Research Funds for the Central Universities; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [21073175]; National Basic Research Program of ChinaNational Basic Research Program of China [2010CB923300]
This work was supported by NSF CAREER Grant PHY-0349256 and NSF MRI-R2 Grant DBI-2959989, the start-up funding from University of Science and Technology of China, the Fundamental Research Funds for the Central Universities, National Natural Science Foundation of China (Grant 21073175), and National Basic Research Program of China (Grant 2010CB923300).
3
2
20
Amer chemical soc
Washington
JO - J. Phys. Chem. BJ. Phys. Chem. B
ER -
TY - JOUR
T1 - Hydration dependence of conformational dielectric relaxation of lysozyme
JF - Biophysical Journal
Y1 - 2006
A1 - Knab, Joseph
A1 - Chen, Jing-Yin
A1 - Markelz, Andrea
VL - 90
SN - 0006-3495
ER -
TY - Generic
T1 - High field pulsed terahertz measurements of nonlinear conductivity
T2 - Nonlinear Optics: Materials, Fundamentals, and Applications
Y1 - 2000
A1 - A. G. Markelz
KW - 0.5 THz
KW - 2D electron gases
KW - Conductivity measurement
KW - electrical conductivity measurement
KW - Electron emission
KW - FEL measurements
KW - Finite impulse response filter
KW - high field pulsed terahertz measurements
KW - high field pulsed terahertz spectroscopy
KW - high-speed optical techniques
KW - inplane nonlinear conductivity response
KW - LO phonon bottleneck weakening
KW - nonlinear conductivity
KW - nonlinear optics
KW - phonons
KW - Power measurement
KW - Pulse measurements
KW - Resonance
KW - semiconductor quantum wells
KW - spectroscopy
KW - Submillimeter wave measurements
KW - submillimetre wave spectroscopy
KW - two dimensional electron gases
KW - two-dimensional electron gas
AB - High field pulsed terahertz spectroscopy is used to measure the inplane nonlinear conductivity response of two dimensional electron gases. Results are compared to FEL measurements suggesting LO phonon bottleneck weakening at 0.5 THz.
JF - Nonlinear Optics: Materials, Fundamentals, and Applications
CY - Kaua'i-Lihue, HI, USA
VL - 46
UR - https://ieeexplore.ieee.org/document/883591/authors#authors
JO - Nonlinear Optics: Materials, Fundamentals, and Applications. Technical Digest. Postconference Edition. TOPS Vol.46 (IEEE Cat. No.00CH37174)
ER -