Generalized magic angle for time-resolved spectroscopy with laser pulses of arbitrary ellipticity
Generalized magic angle for time-resolved spectroscopy with laser pulses of arbitrary ellipticity
复制标题
DOI：
10.1088/0953-4075/47/12/124014
复制
发表时间：
2014-06-28
影响因子：
1.6
通讯作者：
Brixner，Tobias
中科院分区：
文献类型：
--
作者：
Schott，Sebastian;Steinbacher，Andreas;Brixner，Tobias
我们提出了一种计算各向同性样品的时间分辨光谱的魔角条件的一般方法。允许每个脉冲的任意静态偏振和传播方向，使我们不仅可以获得已知的线偏振和圆偏振的魔角条件，而且可以获得使用椭圆偏振激光脉冲的无各向异性光谱的类似条件。结果在瞬态吸收上进行了举例，并转移到相干二维光谱上。此外，我们推导了瞬态吸收光谱中可测量的各向异性与分子结构之间的关系，即泵浦和探测跃迁偶极矩之间的夹角。以具有双重退化TDM的分子为例，讨论了多个频谱重叠信号的影响。
We present a general approach for calculating the magic-angle condition for time-resolved spectroscopy of isotropic samples. Allowing for arbitrary static polarizations and propagation directions of each pulse enables us to retrieve not only the known magic-angle conditions for linear and circular polarization, but also analogous conditions for anisotropy-free spectroscopy using elliptically polarized laser pulses. The results are exemplified on transient absorption and transferred to coherent two-dimensional spectroscopy. Furthermore we derive for transient absorption spectroscopy the relation between the measurable anisotropy and the molecular structure, ie, the angle between the pumped and probed transition dipole moments (TDMs). The impact of multiple spectrally overlapping signals is considered and discussed on the example of a molecule with a two-fold degenerate TDM.