Settersten Thomas B, Patterson Brian D, Gray Jeffrey A
Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94551, USA.
J Chem Phys. 2006 Jun 21;124(23):234308. doi: 10.1063/1.2206783.
We report improved measurements of the temperature-dependent cross sections for the quenching of fluorescence from the A 2Sigma+(v'=0) state of NO. Cross sections were measured for gas temperatures ranging from 294 to 1300 K for quenching by NO(X (2)Pi), H(2)O, CO(2), O(2), CO, N(2), and C(2)H(2). The A 2Sigma+(v'=0) state was populated via two-photon excitation with a picosecond laser at 454 nm, and the decay rate of the fluorescence originating from A 2Sigma+(v'=0) was measured directly. Thermally averaged quenching cross sections were determined from the dependence of the fluorescence decay rate on the quencher gas pressure. Our measurements are compared to previous measurements and models of the quenching cross sections, and new empirical fits to the data are presented. Our new cross-section data enable predictions in excellent agreement with prior measurements of the fluorescence lifetime in an atmospheric-pressure methane-air diffusion flame. The agreement resolves discrepancies between the lifetime measurements and predictions based on the previous quenching models, primarily through improved models for the quenching by H(2)O, CO(2), and O(2) at temperatures less than 1300 K.
我们报告了对一氧化氮(NO)A 2Σ⁺(v' = 0)态荧光猝灭的温度依赖截面的改进测量结果。测量了在294至1300 K的气体温度范围内,由NO(X ²Π)、H₂O、CO₂、O₂、CO、N₂和C₂H₂进行猝灭的截面。通过用454 nm的皮秒激光进行双光子激发来填充A 2Σ⁺(v' = 0)态,并直接测量源自A 2Σ⁺(v' = 0)的荧光衰减率。根据荧光衰减率对猝灭气体压力的依赖性确定热平均猝灭截面。我们的测量结果与先前的猝灭截面测量和模型进行了比较,并给出了对数据的新经验拟合。我们的新截面数据使得预测结果与先前在大气压甲烷 - 空气扩散火焰中对荧光寿命的测量结果高度吻合。这种吻合主要通过改进低于1300 K温度下H₂O、CO₂和O₂猝灭的模型,解决了基于先前猝灭模型的寿命测量与预测之间的差异。