Quantum-Controlled Collisions of H2 Molecules.
Quantum-Controlled Collisions of H2 Molecules.
复制标题
H2 分子的量子控制碰撞。
DOI：
10.1021/acs.jpca.2c06808
复制
发表时间：
2023
期刊：
影响因子：
--
通讯作者：
N. Mukherjee
中科院分区：
文献类型：
--
作者：
N. Mukherjee
从散射实验中可以获得的信息量取决于在入射信道中定义量子态的精度。通过精确定义入射态和测量散射实验中的出射态，我们建立了实验求解薛定谔方程的边界条件。在这个角度来看，我们讨论冷非弹性散射实验使用最理论上易处理的H2和它的同位素作为目标。我们准备的目标在一个精确定义的振转（v，j，m）量子态使用一种特殊的相干光学技术称为斯塔克诱导绝热拉曼通道（SARP）。v和j表示振动和转动能级的量子数，m表示转动角动量矢量j在实验室坐标系中合适的量化轴上的投影。m量子数的选择定义了分子框架的排列，这是探测各向异性相互作用所必需的。为了使碰撞温度在几个开尔文的范围内，我们在混合超声束中共同扩展碰撞伙伴，该混合超声束被准直以定义碰撞速度的方向。当键轴相对于明确定义的碰撞速度对齐时，SARP在量子尺度上实现了立体动力学控制。通过旋转非弹性冷散射实验的各种例子，我们展示了SARP如何相干控制各向异性相互作用的动力学，通过在一个单一的振转（v，j）能态内制备取向m态的量子叠加。一个分波分析，这已被开发的冷散射实验，显示出主导地位的共振轨道，留下其标记的散射角分布。这些高度控制的冷碰撞实验在单分波极限允许最直接的比较与理论计算的结果，必要的精确建模的分子相互作用势。
The amount of information that can be obtained from a scattering experiment depends upon the precision with which the quantum states are defined in the incoming channel. By precisely defining the incoming states and measuring the outgoing states in a scattering experiment, we set up the boundary condition for experimentally solving the Schrödinger equation. In this Perspective we discuss cold inelastic scattering experiments using the most theoretically tractable H2 and its isotopologues as the target. We prepare the target in a precisely defined rovibrational (v, j, m) quantum state using a special coherent optical technique called the Stark-induced adiabatic Raman passage (SARP). v and j represent the quantum numbers of the vibrational and rotational energy levels, and m refers to the projection of the rotational angular momentum vector j on a suitable quantization axis in the laboratory frame. Selection of the m quantum numbers defines the alignment of the molecular frame, which is necessary to probe the anisotropic interactions. For us to achieve the collision temperature in the range of a few degrees Kelvin, we co-expand the colliding partners in a mixed supersonic beam that is collimated to define a direction for the collision velocity. When the bond axis is aligned with respect to a well-defined collision velocity, SARP achieves stereodynamic control at the quantum scale. Through various examples of rotationally inelastic cold scattering experiments, we show how SARP coherently controls the dynamics of anisotropic interactions by preparing quantum superpositions of the orientational m states within a single rovibrational (v, j) energy state. A partial wave analysis, which has been developed for the cold scattering experiments, shows dominance of a resonant orbital that leaves its mark in the scattering angular distribution. These highly controlled cold collision experiments at the single partial wave limit allow the most direct comparison with the results of theoretical computations, necessary for accurate modeling of the molecular interaction potential.
一对冷排列硅藻之间共振散射的各向异性动力学
影响因子：
21.8
作者：
Zhou, Haowen;Perreault, William E.;Mukherjee, Nandini;Zare, Richard N.
通讯作者：
Zare, Richard N.
影响因子：
56.9
作者：
Haowen Zhou;William E. Perreault;N. Mukherjee;R. Zare
通讯作者：
Haowen Zhou;William E. Perreault;N. Mukherjee;R. Zare
影响因子：
56.9
作者：
Hu, M. -G.;Liu, Y.;Ni, K. -K.
通讯作者：
Ni, K. -K.