2-DIMENSIONAL FEMTOSECOND VIBRATIONAL SPECTROSCOPY OF LIQUIDS

2-DIMENSIONAL FEMTOSECOND VIBRATIONAL SPECTROSCOPY OF LIQUIDS
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DOI:
10.1063/1.465484
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发表时间:
1993-12-15
影响因子:
4.4
通讯作者:
MUKAMEL, S
MUKAMEL, S
中科院分区:
化学2区
文献类型:
--
作者:
TANIMURA, Y;MUKAMEL, S

文献摘要

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采用核运动的多模谐波模型计算了液体在N个飞秒激光脉冲作用下的非线性光学响应,并通过电子极化率的坐标依赖性与辐射场进行非线性耦合.使用电子非共振光场,这种多维光谱显示提供直接的信息,从光学双折射测量获得的光谱密度的均匀性或不均匀性。使用红外脉冲可以获得补充信息,其中探测核偶极矩的多个时间相关函数(而不是电子极化率)。
The nonlinear optical response of liquids subjected to a series of N femtosecond laser pulses is calculated using a multimode harmonic model for nuclear motions, with nonlinear coupling to the radiation field through the coordinate dependence of the electronic polarizability. Using electronically off-resonant optical fields, this multidimensional spectroscopy is shown to provide direct information regarding the homogeneous or the inhomogeneous nature of the spectral density obtained from optical birefringence measurements. Complementary information can be obtained using infrared pulses where the multiple time correlation functions of the nuclear dipole moment (rather than the electronic polarizability) are being probed.