Adsorption Regularity and Characteristics of sp^3-Hybridized Gas Molecules on Anatase TiO_2(101) Surface

We report the anatase titanium dioxide （101） surface adsorption of sp3-hybridized gas molecules, including NH3, 1-12 0 and CH4, using first-principles plane-wave ultrasoft pseudopotential based on the density functional theory. The results show that it is much easier for a surface with oxygen vacancies to adsorb gas molecules than it is for a surface without oxygen vacancies. The main factor affecting adsorption stability and energy is the polarizability of molecules, and adsorption is induced by surface oxygen vacancies of the negatively charged center. The analyses of state densities and charge population show that charge transfer occurs at the molecule surface upon adsorption and that the number of transferred charge reduces in the order of N, 0 and C. Moreover, the adsorption method is chemical adsorption, and adsorption stability decreases in the order of NH3, tt2 0 and CH4. Analyses of absorption and reflectance spectra reveal that after absorbed CH4 and H2 O, compared with the surface with oxygen vacancy, the optical properties of materials surface, including its absorption coefficients and reflectivity index, have slight changes, however, absorption coefficient and reflectivity would greatly increase after NH3 adsorption. These findings illustrate that anatase titanium dioxide （101） surface is extremely sensitive to NH3.

Theoretical calculation on permeation of gas molecules through crystalline poly(p-xylylene)(PPX) films

Molecular mechanics(MM) and the gradually reduced size(GRS) techniques were used to construct the crystalline poly-p-xylylene(PPX) films,including PPX N,PPX C and PPX D.The corresponding chain-end area of crystalline PPX films provides enough free volumes for adsorbing and transferring gas molecules.Then,the permeable properties of gases were calculated using Grand Canonical Monte Carlo(GCMC),NVT-Molecular Dynamics(MD) and cluster analysis methods.The calculated diffusion coefficients are in the same order of magnitude over a range of temperatures and pressures.And there is no permeation property of gases in the inner part of the crystalline PPX films.

Calculation of vibrational energy transition rates in acoustic relaxation processes for excitable gas molecules

To research the correlation between vibrational energy transition rates and acoustic relaxation processes in excitable gases, the vibrational relaxation theory provided by Tanczos [J. Chem. Phy3. 25, 439 （1956）] is applied to calculate the energy transition rates of Vibrational- Vibrational （V-V） and Vibrational-Translational （V-T） energy transfer in gas mixtures. The results of calculation for the multi-relaxation processes in various gas mixtures, consisting of carbon dioxide, methane, chlorine, nitrogen, and oxygen at room temperature, demonstrate that the acoustic energy stagnated in every vibrational mode is coupled with each other through V-V energy exchanges. The vibrational excitation energy will relax through the V-T de-excitation path of the lowest mode because of its fastest V-T transition rate, resulting in that only one absorption peak can be measured for most of excitable gas mixtures. Thus, an effective model is provided to analyze how the vibrational energy transition rates affect the characteristics of acoustic relaxation processes and acoustic propagation in excitable gas mixtures.

Study on terahertz spectra of SO_2 and H_2S

The spectral characteristics of air pollution gas sulfur dioxide and hydrogen sulfide has been studied experimentally and theo-retically in the range of 0.2-2.6 THz. The gases absorption spectra of sulfur dioxide and hydrogen sulfide, as measured by terahertz Time-Domain Spectroscopy (THz-TDS) technique, show equi-spaced absorption peaks. The peak intervals are varied for different gas and may relate with the molecule structures and rotation modes. We have calculated the intervals of rotational transition frequency according to the gases molecule structure and the rotational modes. The results are consistent with experimental results which confirm the suggestion that the absorption is coming from the molecular rotational transition. The study suggests a technique to detect air pollutants by THz-TDS and the rotational modes of gas molecules.