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1.
Bernt Wennberg 《Archive for Rational Mechanics and Analysis》1995,130(2):103-144
We prove existence, uniqueness and stability for solutions of the nonlinear Boltzmann equation in a periodic box in the case when the initial data are sufficiently close to a spatially homogeneous function. The results are given for a range of spaces, including L
1, and extend previous results in L
for the non-homogeneous equation, as well as the more developed L
p
-theory for the spatially homogeneous Boltzmann equation.We also give new L
-estimates for the spatially homogeneous equation in the case of Maxwellian interactions. 相似文献
2.
The paper considers the stability and strong convergence to equilibrium of solutions to the spatially homogeneous Boltzmann
equation for Fermi-Dirac particles. Under a cutoff condition on the collision kernel, we prove a strong stability in L
1
topology at any finite time interval, and, for hard and Maxwellian potentials, we prove that the solutions converge strongly
in L
1
to equilibrium under a high temperature condition. The basic tools used are moment-production estimates and the strong compactness
of the collision gain term.
(Accepted 25, October 2002)
Published online March 14, 2003
Communicated by P.-L. Lions 相似文献
3.
Crounse JD Paulot F Kjaergaard HG Wennberg PO 《Physical chemistry chemical physics : PCCP》2011,13(30):13607-13613
We report experimental evidence for the formation of C(5)-hydroperoxyaldehydes (HPALDs) from 1,6-H-shift isomerizations in peroxy radicals formed from the hydroxyl radical (OH) oxidation of 2-methyl-1,3-butadiene (isoprene). At 295 K, the isomerization rate of isoprene peroxy radicals (ISO2?) relative to the rate of reaction of ISO2? + HO2 is k(isom)(295)/(k(ISO2?+HO2)(295)) = (1.2 ± 0.6) x 10(8) mol cm(-3), or k(isom)(295) ? 0.002 s(-1). The temperature dependence of this rate was determined through experiments conducted at 295, 310 and 318 K and is well described by k(isom)(T)/(k(ISO2?+HO2)(T)) = 2.0 x 10(21) exp(-9000/T) mol cm(-3). The overall uncertainty in the isomerization rate (relative to k(ISO2?+HO2)) is estimated to be 50%. Peroxy radicals from the oxidation of the fully deuterated isoprene analog isomerize at a rate ~15 times slower than non-deuterated isoprene. The fraction of isoprene peroxy radicals reacting by 1,6-H-shift isomerization is estimated to be 8-11% globally, with values up to 20% in tropical regions. 相似文献
4.
Cumulant functions are introduced to describe the statistical state of a radiation field. These functions are simply related
to the optical coherence functions but have some interesting features. It is shown that if the cumulant functions of all orders
greater than some numberN
0 vanish then they also vanish for all orders greater than 2. Thermal field is the only field having this property. This property
holds whether the field is described by a classical stochastic process or by a quantum density operator. Further the particular
operator ordering used in defining these cumulant functions for the quantized field affects only the second order cumulant
function. To describe the statistical state of a vector field such as partially polarized or unpolarized radiation, one would
need to introduce cumulant tensors. 相似文献
5.
Fry JL Matthews J Lane JR Roehl CM Sinha A Kjaergaard HG Wennberg PO 《The journal of physical chemistry. A》2006,110(22):7072-7079
We report measurement and analysis of the photodissociation spectrum of hydroxymethyl hydroperoxide (HOCH(2)OOH) and its partially deuterated analogue, HOCD(2)OOH, in the OH-stretching region. Spectra are obtained by Fourier transform infrared spectroscopy in the 1nu(OH) and 2nu(OH) regions, and by laser induced fluorescence detection of the OH fragment produced from dissociation of HOCH(2)OOH initiated by excitation of the 4nu(OH) and 5nu(OH) overtone regions (action spectroscopy). A one-dimensional local-mode model of each OH chromophore is used with ab initio calculated OH-stretching potential energy and dipole moment curves at the coupled-cluster level of theory. Major features in the observed absorption and photodissociation spectra are explained by our local-mode model. In the 4nu(OH) region, explanation of the photodissocation spectrum requires a nonuniform quantum yield, which is estimated by assuming statistical energy distribution in the excited state. Based on the estimated dissociation threshold, overtone photodissociation is not expected to significantly influence the atmospheric lifetime of hydroxymethyl hydroperoxide. 相似文献
6.
The non-cutoff Boltzmann equation can be simulated using the DSMC method, by a truncation of the collision term. However,
even for computing stationary solutions this may be very time consuming, in particular in situations far from equilibrium.
By adding an appropriate diffusion, to the DSMC-method, the rate of convergence when the truncation is removed, may be greatly
improved. We illustrate the technique on a toy model, the Kac equation, as well as on the full Boltzmann equation in a special
case. 相似文献
7.
Jean Bourgain François Golse Bernt Wennberg 《Communications in Mathematical Physics》1998,190(3):491-508
Consider the domain
and let the free path length be defined as
The distribution of values of is studied in the limit as for all . It is shown that the value is critical for this problem: in other words, the limiting behavior of depends only on whether γ is larger or smaller than .
Received: 1 March 1996 / Accepted: 25 March 1997 相似文献
8.
The vibrational overtone induced unimolecular dissociation of HMHP (HOCH(2)OOH) and HMHP-d(2) (HOCD(2)OOH) into OH and HOCH(2)O (HOCD(2)O) fragments is investigated in the region of the 4nu(OH) and 5nu(OH) bands. The unimolecular dissociation rates in the threshold region, corresponding to the 4nu(OH) band, exhibit measurable differences associated with excitation of the OH stretch of the alcohol versus the peroxide functional group, with the higher energy alcohol OH stretching state exhibiting a slower dissociation rate compared to the lower energy peroxide OH stretch in both HMHP and HMHP-d(2). Predictions using the Rice-Ramsperger-Kassel-Marcus theory give rates that are in reasonably good agreement with the measured dissociation rate for the alcohol OH stretch but considerably differ from the measured rates for the peroxide OH stretch in both isotopomers. The present results are interpreted as suggesting that the extent of intramolecular vibrational energy redistribution (IVR) is different for the two OH stretching states associated with the two functional groups in HMHP, with IVR being substantially less complete for the peroxide OH stretch. Analysis of the OH fragment product state distributions in conjunction with phase-space theory simulation gives a D(0) value of 38+/-0.7 kcal/mole for breaking the peroxide bond in HMHP. 相似文献
9.
MA Freitas CL Hendrickson AG Marshall 《Rapid communications in mass spectrometry : RCM》1999,13(15):1639-1642
We present a novel approach for the determination of activation energy for the unimolecular dissociation of a large (>50 atoms) ion, based on measurement of the unimolecular dissociation rate constant as a function of continuous-wave CO(2) laser intensity. Following a short ( approximately 1 s) induction period, CO(2) laser irradiation produces an essentially blackbody internal energy distribution, whose 'temperature' varies inversely with laser intensity. The only currently available method for measuring such activation energies is blackbody infrared radiative dissociation (BIRD). Compared with BIRD, FRAGMENT: (a) eliminates the need to heat the surrounding ion trap and vacuum chamber to each of several temperatures (each requiring hours for temperature equilibration); (b) offers a three-fold wider range of effective blackbody temperature; and (c) extends the range of applications to include initially cold ions (e.g., gas-phase H/D exchange). Our FRAGMENT-determined activation energy for dissociation of protonated bradykinin, 1.2 +/- 0.1 eV, agrees within experimental error to the value, 1.3 +/- 0.1 eV, previously reported by Williams et al. from BIRD experiments. Copyright 1999 John Wiley & Sons, Ltd. 相似文献
10.
Crounse JD Knap HC Ørnsø KB Jørgensen S Paulot F Kjaergaard HG Wennberg PO 《The journal of physical chemistry. A》2012,116(24):5756-5762
Peroxy radicals formed by addition of OH and O(2) to the olefinic carbon atoms in methacrolein react with NO to form methacrolein hydroxy nitrate and hydroxyacetone. We observe that the ratio of these two compounds, however, unexpectedly decreases as the lifetime of the peroxy radical increases. We propose that this results from an isomerization involving the 1,4-H-shift of the aldehydic hydrogen atom to the peroxy group. The inferred rate (0.5 ± 0.3 s(-1) at T = 296 K) is consistent with estimates obtained from the potential energy surface determined by high level quantum calculations. The product, a hydroxy hydroperoxy carbonyl radical, decomposes rapidly, producing hydroxyacetone and re-forming OH. Simulations using a global chemical transport model suggest that most of the methacrolein hydroxy peroxy radicals formed in the atmosphere undergo isomerization and decomposition. 相似文献