Modelling multi-pulse population dynamics from ultrafast spectroscopy.
Modelling multi-pulse population dynamics from ultrafast spectroscopy.
复制标题
DOI：
10.1371/journal.pone.0017373
复制
发表时间：
2011-03-21
期刊：
影响因子：
3.7
通讯作者：
van Thor JJ
中科院分区：
文献类型：
--
作者：
van Wilderen LJ;Lincoln CN;van Thor JJ
当前先进的激光、光学和电子技术允许分子动力学的敏感记录，从单共振到多色和多脉冲实验。通过实验数据的全局分析提取发生的（生物）物理相关途径需要对连接方案进行系统的调查。这里我们提出了一个基于matlab的工具箱。该工具箱具有图形用户界面，方便了不同反应模型对数据的应用，以生成耦合微分方程。任何时间相关的数据集都可以通过梯度或直接搜索方法进行分析，以提取可观测值的时间无关相关性。特定的能力（即啁啾和仪器响应功能），用于分析超快泵-探针光谱数据包括在内。包含一个与瞬态相相互作用的额外脉冲可以帮助解开复杂的相互依赖的通路。因此，新理论（包含在工具箱中）扩展了路径建模，该理论描述了在种群衰变存在的情况下，单次和多次强极化飞秒脉冲对随机定向粒子集合的有限漂白（定向）效应。例如，通常假设的平顶多模光束轮廓适应于更现实的高斯形状，这暴露了需要进行多次修正才能进行准确的各向异性测量。此外，与单个或多个强偏振激光脉冲相互作用的（选择性）激发（光选择）和种群的各向异性被证明是功率密度和光束轮廓的函数。利用实际实验的实例值，计算了这在多大程度上有效地定向了粒子系综。最后，除了在光密集样本中进行深度平均之外，该实现还包括与多个脉冲的相互作用。总之，我们表明数学建模对于模拟和解决超快光谱中群体物理行为的细节至关重要，例如泵-探测、泵-倾倒-探测和泵-再泵-探测实验。
Current advanced laser, optics and electronics technology allows sensitive recording of molecular dynamics, from single resonance to multi-colour and multi-pulse experiments. Extracting the occurring (bio-) physical relevant pathways via global analysis of experimental data requires a systematic investigation of connectivity schemes. Here we present a Matlab-based toolbox for this purpose. The toolbox has a graphical user interface which facilitates the application of different reaction models to the data to generate the coupled differential equations. Any time-dependent dataset can be analysed to extract time-independent correlations of the observables by using gradient or direct search methods. Specific capabilities (i.e. chirp and instrument response function) for the analysis of ultrafast pump-probe spectroscopic data are included. The inclusion of an extra pulse that interacts with a transient phase can help to disentangle complex interdependent pathways. The modelling of pathways is therefore extended by new theory (which is included in the toolbox) that describes the finite bleach (orientation) effect of single and multiple intense polarised femtosecond pulses on an ensemble of randomly oriented particles in the presence of population decay. For instance, the generally assumed flat-top multimode beam profile is adapted to a more realistic Gaussian shape, exposing the need for several corrections for accurate anisotropy measurements. In addition, the (selective) excitation (photoselection) and anisotropy of populations that interact with single or multiple intense polarised laser pulses is demonstrated as function of power density and beam profile. Using example values of real world experiments it is calculated to what extent this effectively orients the ensemble of particles. Finally, the implementation includes the interaction with multiple pulses in addition to depth averaging in optically dense samples. In summary, we show that mathematical modelling is essential to model and resolve the details of physical behaviour of populations in ultrafast spectroscopy such as pump-probe, pump-dump-probe and pump-repump-probe experiments.
登录
查看更多内容
影响因子：
2.9
作者：
Borisov, VB;Liebl, U;Vos, MH
通讯作者：
Vos, MH
DOI：
10.1073/pnas.85.14.5062
发表时间：
1988-07-01
影响因子：
11.1
作者：
MOORE, JN;HANSEN, PA;HOCHSTRASSER, RM
通讯作者：
HOCHSTRASSER, RM
影响因子：
2.9
作者：
Kovalenko, SA;Dobryakov, AL;Ernsting, NP
通讯作者：
Ernsting, NP
影响因子：
3.1
作者：
Audet, C;Dennis, JE
通讯作者：
Dennis, JE
DOI：
10.1073/pnas.141220198
发表时间：
2001-07-17
影响因子：
11.1
作者：
Logunov, SL;Volkov, VV;El-Sayed, MA
通讯作者：
El-Sayed, MA