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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >State-selective vibrational excitation and dissociation of H _2 ~+ by strong infrared laser pulses: Below-resonant versus resonant laser fields and electron-field following
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State-selective vibrational excitation and dissociation of H _2 ~+ by strong infrared laser pulses: Below-resonant versus resonant laser fields and electron-field following

机译：H _2〜+在强红外激光脉冲作用下的状态选择性振动激发和解离：低于共振和共振激光场和电子场

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摘要

The quantum dynamics of vibrational excitation and dissociation of H2 ~+ by strong and temporally shaped infrared (IR) laser pulses has been studied on the femtosecond (fs) time scale by numerical solution of the time-dependent Schr?dinger equation with explicit treatment of nuclear and electron motion beyond the Born-Oppenheimer approximation. Using sin ~2-shaped laser pulses of 120 fs duration with a peak intensity of I_0 > 10~(14) W/cm~2, it has been found that below-resonant vibrational excitation with a laser carrier frequency of ω < ω_(10)/~2 (where ω_(10) is the frequency of the |v = 0〉 → |v = 1〉 vibrational transition) is much more efficient than a quasi-resonant vibrational excitation at ω ≈ ω_(10). In particular, at the below-resonant laser carrier frequency ω = 0.3641 × 10~(-2) au (799.17 cm~(-1)), dissociation probabilities of H2~+ (15.3% at the end of the 120 fs laser pulse and 21% at t = 240 fs) are more than 3 orders of magnitude higher than those obtained for the quasi-resonant laser frequency ω = 1.013 × 10~(-2) au (2223.72 cm~(-1)). Probabilities of state-selective population transfer to vibrational states |v = 1〉, |v = 2〉, and |v = 3〉 from the vibrational ground state |v = 0〉 of about 85% have been calculated in the optimal below-resonant cases. The underlying mechanism of the efficient below-resonant vibrational excitation is the electron-field following and simultaneous transfer of energy to the nuclear coordinate.
机译：通过飞秒（fs）时标，通过时间相关的薛定er方程的数值解，并通过显式处理，研究了强时空成形的红外（IR）激光脉冲对H2〜+振动激发和解离的量子动力学。核和电子运动超出了Born-Oppenheimer近似。使用120 fs持续时间的sin〜2形激光脉冲，峰值强度为I_0> 10〜（14）W / cm〜2，发现低于共振的振动激发，激光载波频率为ω<ω_（ 10）/〜2（其中ω_（10）是| v = 0〉→| v = 1〉振动跃迁的频率）比在ω≈ω_（10）处的准共振振动激励要有效得多。尤其是在低于谐振频率的激光载波频率ω= 0.3641×10〜（-2）au（799.17 cm〜（-1））时，H2〜+的解离几率（在120 fs激光脉冲结束时为15.3％）在t = 240 fs时为21％;在准谐振激光频率ω= 1.013×10〜（-2）au（2223.72 cm〜（-1））下获得的值高出3个数量级。在下面的最佳条件下，已经计算出从振动基态| v = 0〉到大约85％的状态选择种群转移到振动状态| v = 1〉，| v = 2〉和| v = 3〉的概率。共振情况。有效的低于共振的振动激发的基本机理是电子场跟随并同时将能量转移到核坐标。

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