Coherent superposition of M-states in a single rovibrational level of H2 by Stark-induced adiabatic Raman passage.

Coherent superposition of M-states in a single rovibrational level of H2 by Stark-induced adiabatic Raman passage.
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Stark 诱导的绝热拉曼通道在 H2 的单个旋转水平中 M 态的相干叠加。

DOI:
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发表时间:
2014
影响因子:
4.4
通讯作者:
R. Zare
R. Zare
中科院分区:
化学2区
文献类型:
--
作者:
N. Mukherjee;Wenrui Dong;R. Zare

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利用斯塔克诱导绝热拉曼通道,在532 nm,脉宽为1.6 ns,200 mJ/pulse的线偏振单模泵浦和699 nm,脉宽为1.4 ns,20 mJ/pulse的斯托克斯激光激发下,制备了一个处于磁性子能级M的锁相叠加态的孤立旋振激发(v = 1,J = 2)H2分子系综.利用线偏振但交叉偏振的抽运脉冲和Stokes激光脉冲沿量子化z轴沿着共同传播,制备了一个双轴叠加态:[line] v(t)= 1/(2)[[line] v = 1,J = 2,M = -2- [line] v = 1,J = 2,M = +2].相位相干度通过使用H2 E,F-X(0,1)带的O(2)线经由2 + 1共振增强多光子电离(REMPI)在210.8 nm处测量,通过在飞行时间质谱仪中记录REMPI信号中的干涉条纹,同时使用半波片旋转UV激光偏振的方向。当Stokes频率调谐到(v = 0,J = 0)→(v = 1,J = 2)拉曼共振时,从E,F-X(0,0)带的Q(0)线的耗尽测量到近60%的粒子数从H2(v = 0,J = 0)基态转移到H2(v = 1,J = 2)的叠加态.
We prepare an ensemble of isolated rovibrationally excited (v = 1, J = 2) H2 molecules in a phase-locked superposition of magnetic sublevels M using Stark-induced adiabatic Raman passage with linearly polarized single-mode pump (at 532 nm, ∼6 ns pulse duration, 200 mJ/pulse) and Stokes (699 nm, ∼4 ns pulse duration, 20 mJ/pulse) laser excitation. A biaxial superposition state, given by [line]ψ(t)⟩ = 1/√(2)[[line]ν = 1, J = 2, M = -2⟩ - [line]ν = 1, J = 2, M = +2⟩], is prepared with linearly but cross-polarized pump and Stokes laser pulses copropagating along the quantization z-axis. The degree of phase coherence is measured by using the O(2) line of the H2 E,F-X (0,1) band via 2 + 1 resonance enhanced multiphoton ionization (REMPI) at 210.8 nm by recording interference fringes in the REMPI signal in a time-of-flight mass spectrometer as the direction of the UV laser polarization is rotated using a half-wave plate. Nearly 60% population transfer from H2 (v = 0, J = 0) ground state to the superposition state in H2 (v = 1, J = 2) is measured from the depletion of the Q(0) line of the E,F-X (0,0) band as the Stokes frequency is tuned across the (v = 0, J = 0) → (v = 1, J = 2) Raman resonance.