Li Xuan, Parker Gregory A, Brumer Paul, Thanopulos Ioannis, Shapiro Moshe
Homer L. Dodge Department of Physics and Astronomy, University of Oklahoma, Oklahoma 73019, USA.
J Chem Phys. 2008 Mar 28;128(12):124314. doi: 10.1063/1.2899666.
We present a nonperturbative time-dependent quantum mechanical theory of the laser catalysis and control of a bifurcating A+BC<-->(variant Planck's over 2pi omega(0))ABC*(v)<-->(variant Planck's over 2pi omega(0) )AB+C reaction, with ABC*(v) denoting an intermediate, electronically excited, complex of ABC in the vth vibrational state. We apply this theory to the low collision energy fermion-boson light-induced exchange reaction, (6)Li((2)S)+(7)Li(2)((3)Sigma(u)(+))<-->(variant Planck's over 2pi omega(0))((6)Li(7)Li(7)Li)*<-->(variant Planck's over 2pi omega(0))(6)Li(7)Li((3)Sigma(+))+(7)Li((2)S). We show that at very low collision energies and energetically narrow (approximately 0.01 cm(-1)) initial reactant wave packets, it is possible to tune the yield of the exchange reaction from 0 to near-unity (yield >or=99%) values. Controllability is somewhat reduced at collisions involving energetically wider (approximately 1 cm(-1)) initial reactant wave packets. At these energetic bandwidths, the radiative reactive control, although still impressive, is limited to the 0%-76% reactive-probabilities range.
我们提出了一种非微扰的含时量子力学理论，用于研究激光催化和控制分支反应A + BC ⇌ （普朗克常量除以2πω₀）ABC*（v）⇌ （普朗克常量除以2πω₀）AB + C，其中ABC*（v）表示处于第v个振动态的ABC的电子激发中间复合物。我们将该理论应用于低碰撞能费米子 - 玻色子光诱导交换反应，即（⁶Li（²S）） + （⁷Li₂（³Σᵤ⁺））⇌ （普朗克常量除以2πω₀）（⁶Li⁷Li⁷Li）*⇌ （普朗克常量除以2πω₀）⁶Li⁷Li（³Σ⁺） + （⁷Li（²S））。我们表明，在非常低的碰撞能和能量上很窄（约0.01 cm⁻¹）的初始反应物波包情况下，有可能将交换反应的产率从0调节到接近100%（产率≥99%）的值。在涉及能量上更宽（约1 cm⁻¹）的初始反应物波包的碰撞中，可控性会有所降低。在这些能量带宽下，辐射反应控制虽然仍然令人印象深刻，但仅限于0% - 76%的反应概率范围。
Zotero 插件