Otterpohl Florian, Keefer Daniel, Mukamel Shaul, Thorwart Michael
I. Institut für Theoretische Physik, <a href="https://ror.org/00g30e956">Universität Hamburg</a>, Notkestraße 9, 22607 Hamburg, Germany.
<a href="https://ror.org/00sb7hc59">Max-Planck-Institut für Polymerforschung</a>, 55128 Mainz, Germany.
Phys Rev Lett. 2024 Aug 30;133(9):098001. doi: 10.1103/PhysRevLett.133.098001.
The quantum coherent dynamics of a vibronic wave packet in a molecule passing through a conical intersection can be revealed using attosecond transient coherent Raman spectroscopy. In particular, the time evolution of the electronic coherence can be monitored in the presence of vibrational dynamics. So far, the technique has been investigated without including environmental quantum noise. Here, we employ the numerically exact hierarchy equation of motion approach to show that the transient coherent Raman signals are robust and accessible on times of up to a few hundred femtoseconds with respect to electonic and vibrational dephasing.
利用阿秒瞬态相干拉曼光谱,可以揭示分子中通过锥形交叉点的振转波包的量子相干动力学。特别是,在存在振动动力学的情况下,可以监测电子相干的时间演化。到目前为止,该技术的研究尚未考虑环境量子噪声。在此,我们采用数值精确的运动方程层级方法表明,瞬态相干拉曼信号在电子和振动退相干方面,在长达几百飞秒的时间内是稳健且可获取的。