用实时格林函数计算donor-C60复合物中的电荷分离：非局部相关的重要性
Charge separation in donor-C60 complexes with real-time Green's functions: The importance of nonlocal correlations
摘要：
我们使用非平衡格林函数（NEGF）方法进行实时模拟的超快电子动力学的光激发供体C60复合物建模的Pariser-Parr-Pople哈密顿量。NEGF的结果进行了比较，平均场哈特里-福克（HF）计算解开相关性的作用。最初的基准对数值上高度精确的时间依赖的密度矩阵重整化群计算验证NEGF的准确性。然后，我们发现，电荷转移（CT）激子部分衰减到电荷分离（CS）状态，如果动态非局域相关修正。这种CS过程发生在光激发后约10 fs。相比之下，在HF模拟中激子复合的概率几乎是100%。这些结果在很大程度上不受核振动的影响;然而，当水平不对准阻碍CT过程时，后者变得至关重要。我们的研究结果的强大的性质表明，超快CS驱动的相关性诱导的退相干可能会发生在许多有机纳米尺度系统，但它只能正确预测的理论处理，包括时间非局部相关性。
英文摘要：
We use the Nonequilibrium Green's Function (NEGF) method to perform real-time simulations of the ultrafast electron dynamics of photoexcited donor-C60 complexes modeled by a Pariser-Parr-Pople Hamiltonian. The NEGF results are compared to mean-field Hartree-Fock (HF) calculations to disentangle the role of correlations. Initial benchmarking against numerically highly accurate time-dependent Density Matrix Renormalization Group calculations verifies the accuracy of NEGF. We then find that charge-transfer (CT) excitons partially decay into charge separated (CS) states if dynamical non-local correlation corrections are included. This CS process occurs in ~10 fs after photoexcitation. In contrast, the probability of exciton recombination is almost 100% in HF simulations. These results are largely unaffected by nuclear vibrations; the latter become however essential whenever level misalignment hinders the CT process. The robust nature of our findings indicate that ultrafast CS driven by correlation-induced decoherence may occur in many organic nanoscale systems, but it will only be correctly predicted by theoretical treatments that include time-nonlocal correlations.
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。
