Laser控制卟啉中的双质子转移。光子分子线的超快开关
Laser control of double proton transfer in porphycenes. Towards an ultrafast switch for photonic molecular wires
摘要：
电子激发能沿分子线的转移依赖于相邻发色团的电子跃迁偶极矩的相对取向。在卟啉中，这种取向在电子基态的双质子转移时发生变化。我们探索了通过红外泵浦-转储激光控制方案来触发这样的双质子转移反应的可能性。为此，使用密度泛函理论对不对称取代的卟啉进行量子化学表征。基态几何结构，双质子转移的势能面的拓扑结构，和S 0->S1跃迁能量与母体化合物卟啉和对称衍生物进行了比较。采用一个简单的二维模型的双质子转移，其中包括顺序和协调的运动，量子动力学模拟的激光驱动的动力学进行演示互变异构控制。基于跃迁偶极矩的取向，这种互变异构可能导致约60%的Förster转移耦合的估计变化。
英文摘要：
Electronic excitation energy transfer along a molecular wire depends on the relative orientation of the electronic transition dipole moments of neighboring chromophores. In porphycenes this orientation is changed upon double proton transfer in the electronic ground state. We explore the possibility to trigger such a double proton transfer reaction by means of an infrared pump-dump laser control scheme. To this end a quantum chemical characterization of an asymmetrically substituted porphycene is performed using density functional theory. Ground state geometries, the topology of the potential energy surface for double proton transfer, and S0->S1 transition energies are compared with the parent compound porphycene and a symmetric derivative. Employing a simple two-dimensional model for the double proton transfer, which incorporates sequential and concerted motions, quantum dynamics simulations of the laser driven dynamics are performed which demonstrate tautomerization control. Based on the orientation of the transition dipole moments this tautomerization may lead to an estimated change in the Förster transfer coupling of about 60%
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
