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991.
We report the de novo determination of 15N-1H bond orientations and motional order parameters for the protein ubiquitin with high accuracy based solely on NMR residual dipolar coupling measurements made in six distinct alignment media. The resulting bond orientations are in agreement with RDC-refined orientations of either solid or solution state coordinates to within approximately 2 degrees , which is also the estimated precision of the resulting orientations. The squared generalized order parameters, which reflect amplitudes of motion spanning the picosecond to millisecond time scales, exhibit a correlation with picosecond time scale order parameters derived from conventional NMR 15N spin relaxation methods. Provided that RDC measurements can be obtained using many different alignment media, this approach (called direct interpretation of dipolar couplings) may significantly impact the attainable accuracy and the molecular weight range accessible to NMR structure determination in the solution state, as well as provide a route for the study of motions occurring on the nanosecond to microsecond time scales, which have been traditionally difficult to study at atomic resolution. 相似文献
992.
Sensitive methods recently developed to measure laser-induced fluorescence from trapped ions have been applied to study the dynamics of double- and single-stranded oligonucleotides. In this paper, the fraying of duplex terminal base pairs has been identified by measuring the donor fluorescence as a function of temperature from an oligonucleotide duplex labeled with a pair of FRET dyes. Comparison of the degree of dissociation of 14-mer duplexes observed in the mass spectra with the fluorescence intensity of the donor enables intermediate conformations of the unzipping duplex at the weaker binding end of the duplex to be identified. The autodetachment of electrons from double- and single-stranded oligonucleotide anions has been observed in a gas phase environment. To characterize this process, measurements were performed on 7-mers prepared without FRET fluorophores attached. The dependence of the decay rates of trapped anions have been measured as a function of charge state and temperature for various base compositions. An exceptionally strong dependence of the decay rate on base composition has been identified. The physical basis for this process will be discussed. 相似文献
993.
Damrauer NH Hodgkiss JM Rosenthal J Nocera DG 《The journal of physical chemistry. B》2004,108(20):6315-6321
Proton-coupled electron transfer (PCET) kinetics of a Zn(II) porphyrin donor noncovalently bound to a naphthalene-diimide acceptor through an amidinium-carboxylate interface have been investigated by time-resolved spectroscopy. The S1 singlet excited-state of a Zn(II) 2-amidinium-5,10,15,20-tetramesitylporphyrin chloride (ZnP-beta-AmH+) donor is sufficiently energetic (2.04 eV) to reduce a carboxylate-diimide acceptor (DeltaG degrees = -460 mV, THF). Static quenching of the porphyrin fluorescence is observed and time-resolved measurements reveal more than a 3-fold reduction in the S1 lifetime of the porphyrin upon amidinium-carboxylate formation (THF, 298 K). Picosecond transient absorption spectra of the free ZnP-beta-AmH+ in THF reveal the existence of an excited-state isosbestic point between the S1 and T1 states at lambdaprobe = 650 nm, providing an effective 'zero-kinetics' background on which to observe the formation of PCET photoproducts. Distinct rise and decay kinetics are attributed to the build-up and subsequent loss of intermediates resulting from a forward and reverse PCET reaction, respectively (kPCET(fwd) = 9 x 108 s-1 and kPCET(rev) = 14 x 108 s-1). The forward rate constant is nearly 2 orders of magnitude slower than that measured for covalently linked Zn(II) porphyrin-acceptor dyads of comparable driving force and D-A distance, establishing the importance of a proximal proton network in controlling charge transport. 相似文献
994.
Two mechanisms for the predissociation of the C2Σu+ state of N2+ are discussed - the accidental mechanism and a direct, homogeneous process C → B2Σu+. The matrix elements for the latter channel are dominated by a contribution from the nuclear kinetic energy operator, containing a Franck-Condon integral of form 〈?|?/?R|υ′〉. 相似文献
995.
996.
Joel L. Lebowitz 《Journal of statistical physics》1977,16(1):3-9
In a recent note Barber showed, for a spin-1/2 Ising system with ferromagnetic pair interactions, that some critical exponents of the triplet order parameter
i
j
k
are the same as those of the magnetization
i
. Here we prove such results for all odd correlations and dispense with the requirement of pair interactions. We also prove that the critical temperatureT
c
, defined as the temperature below which there is a spontaneous magnetization, is for fixed even spin interactionsJ
e
independent of the way in which the odd interactionsJ
o
approach zero from above. This is achieved by using only the simplest, Griffiths-Kelley-Sherman (GKS), inequalities, which apply to the most general many-spin, ferromagnetic interactions.Research supported in part by NSF Grant #MPS 75-20638. 相似文献
997.
We study the bifurcation of radially symmetric solutions of +f(u)=0 onn-balls, into asymmetric ones. We show that ifu satisfies homogeneous Neumann boundary conditions, the asymmetric components in the kernel of the linearized operators can have arbitrarily high dimension. For general boundary conditions, we prove some theorems which give bounds on the dimensions of the set of asymmetric solutions, and on the structure of the kernels of the linearized operators.Research supported in part by the NSF under Grant No. MCS-800 2337 相似文献
998.
A study of the degradation effects of enzyme treatment on the dimensional changes of cellulose aggregate fibrils (CAFs) with
dimensions of ∼100,000 × 3,000 × 300 nm from fully bleached kraft fiber was performed. CAFs were incubated with cellulase
for up to 32 h. The insoluble CAFs fragments remaining after enzymatic hydrolysis were then subjected to variable relative
humidity (RH). Each sample was imaged by an atomic force microscope (AFM) in tapping mode. The images were analyzed to determine
the dimensional changes of the insoluble CAFs. Enzymatic hydrolysis continuously depolymerized the CAFs over 32 h, ultimately
causing 20% of the CAFs to become soluble. Compared to initial dimensions of the reference CAFs with no enzymatic treatment,
the dimensions of the enzyme treated CAFs were generally more responsive to humidity and exhibited an increased frequency
of plastic deformations. 相似文献
999.
Alexandre Joel Chorin 《Communications in Mathematical Physics》1988,114(1):167-176
The lattice vortex model of the intertial range in turbulence theory is reviewed; the model consists of an array of vortex tubes whose axes coincide with the bonds on a regular lattice, subjected to random stretching and successive scaling, and constrained by conservation laws for energy, specific volume, circulation, helicity, and an energy/vorticity relation. The scaling laws for vorticity are examined in detail, a Hausdorff dimension for the active portion of the vortex array is calculated, the origin of intermittency is exhibited, and it is pointed out that the Kolmogorov — 5/3 power law already accounts for intermittency effects.Partially supported by the Office of Energy Research, U.S. Department of Energy, under contract DE-AC03-76SF0098, and in part by the Office of Naval Research under contract N00014-76-C-0316 相似文献
1000.
Jean Bricmont Joel L. Lebowitz Charles E. Pfister 《Communications in Mathematical Physics》1979,66(1):1-20
We investigate the spatially inhomogeneous states of two component,A - B, Widom-Rowlinson type lattice systems. When the fugacity of the two components are equal and large, these systems can exist in two different homogeneous (translation invariant) pure phases oneA-rich and oneB-rich. We consider now the system in a box with boundaries favoring the segregation of these two phases into top and bottom parts of the box. Utilizing methods due to Dobrushin we prove the existence, in three or more dimensions, of a sharp interface for the system which persists in the limit of the size of the box going to infinity. We also give some background on rigorous results for the interface problem in Ising spin systems.Supported in part by NSF Grant PHY 77-22302Supported by the Swiss National Foundation for Scientific Research 相似文献