Coherent Two-Quantum Two-Dimensional Electronic Spectroscopy Using Incoherent Light,The Journal of Physical Chemistry A

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Coherent Two-Quantum Two-Dimensional Electronic Spectroscopy Using Incoherent Light
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2017-11-21 00:00:00 , DOI: 10.1021/acs.jpca.7b09443
Darin J. Ulness ₁ , Daniel B. Turner ₂

Affiliation

Two-quantum two-dimensional electronic spectroscopy (2Q 2D ES) may provide a measure of electron-correlation energies in molecules. Attempts to obtain this profound but elusive signal have relied on experimental implementations using femtosecond laser pulses, which induce an overwhelming background signal of nonresonant response. Here we explore theoretically the signatures of electron correlation in coherent 2Q 2D ES measurements that use spectrally incoherent light, I⁽⁴⁾ 2Q 2D ES. One can use such fields to suppress nonresonant response, and therefore this method may better isolate the desired signature of electron correlation. Using an appropriate treatment of the multilevel Bloch electronic system, we find that I⁽⁴⁾ 2Q 2D ES presents an opportunity to measure electron-correlation energies in molecules.

中文翻译：

使用非相干光的相干二维量子电子光谱

二维二维电子光谱（2Q 2D ES）可以提供分子中电子相关能的量度。尝试获得此深刻但难以捉摸的信号的方法依赖于使用飞秒激光脉冲的实验实现，飞秒激光脉冲会引起压倒性的非共振响应信号。在这里，我们在理论上探索使用光谱非相干光I ^（4） 2Q 2D ES的相干2Q 2D ES测量中电子相关性的特征。可以使用这样的场来抑制非谐振响应，因此该方法可以更好地隔离所需的电子相关特征。使用多级Bloch电子系统的适当处理，我们发现I ^（4） 2Q 2D ES为测量分子中的电子相关能提供了机会。

更新日期：2017-11-22

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