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Internal Conversion Cascade in a Carbon Nanobelt: A Multiconfigurational Quantum Dynamical Study
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2024-09-11 , DOI: 10.1021/acs.jctc.4c00841 James A Green 1 , Dominik Brey 1 , Leyla P Razgatlioglu 1 , Badria Ali 1 , Bartosz Błasiak 1 , Irene Burghardt 1
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2024-09-11 , DOI: 10.1021/acs.jctc.4c00841 James A Green 1 , Dominik Brey 1 , Leyla P Razgatlioglu 1 , Badria Ali 1 , Bartosz Błasiak 1 , Irene Burghardt 1
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Carbon nanobelts feature intriguing photophysical properties, due to their high symmetry and structural rigidity. Here, we consider a (6,6) armchair carbon nanobelt, i.e., the very first carbon nanobelt to be synthesized [Povie et al., Science 2017, 356, 172] and characterize the internal conversion dynamics using multiconfigurational quantum dynamics via the multi-layer multiconfiguration time-dependent Hartree (ML-MCTDH) method. A symmetry-adapted linear vibronic coupling Hamiltonian for 26 electronic states and 210 vibrational modes is employed. Electronic excitations are found to decay through a dense manifold of excited states, which interact via multiple conical intersections, while inducing minimal geometry change. It is shown that a rapid coherent decay, exhibiting a nonvanishing quantum flux on a time scale of less than 50 fs, transitions toward a slower, decoherent decay at longer times. As previously suggested in the literature, electronic relaxation is hindered by phonon bottlenecks such that a stepwise internal conversion cascade is observed. The computed vibronic absorption spectrum is shown to be in good agreement with the experimental spectrum.
中文翻译：
碳纳米带中的内部转换级联：多构型量子动力学研究
碳纳米带由于其高对称性和结构刚性而具有令人着迷的光物理性质。在这里，我们考虑 (6,6) 扶手椅碳纳米带，即第一个合成的碳纳米带 [Povie et al., Science 2017 , 356, 172]，并通过多构型量子动力学表征内部转换动力学。层多配置时间相关 Hartree (ML-MCTDH) 方法。采用适用于 26 种电子态和 210 种振动模式的对称自适应线性振动耦合哈密顿量。人们发现电子激发会通过密集的激发态衰减，这些激发态通过多个圆锥形交叉点相互作用，同时引起最小的几何变化。结果表明，快速相干衰变在小于 50 fs 的时间尺度上表现出不消失的量子通量，在较长时间内过渡到较慢的退相干衰变。正如先前文献中所建议的，电子弛豫受到声子瓶颈的阻碍，从而观察到逐步的内部转换级联。计算的电子振动吸收光谱与实验光谱非常吻合。
更新日期：2024-09-11
中文翻译：
碳纳米带中的内部转换级联：多构型量子动力学研究
碳纳米带由于其高对称性和结构刚性而具有令人着迷的光物理性质。在这里，我们考虑 (6,6) 扶手椅碳纳米带，即第一个合成的碳纳米带 [Povie et al., Science 2017 , 356, 172]，并通过多构型量子动力学表征内部转换动力学。层多配置时间相关 Hartree (ML-MCTDH) 方法。采用适用于 26 种电子态和 210 种振动模式的对称自适应线性振动耦合哈密顿量。人们发现电子激发会通过密集的激发态衰减，这些激发态通过多个圆锥形交叉点相互作用，同时引起最小的几何变化。结果表明，快速相干衰变在小于 50 fs 的时间尺度上表现出不消失的量子通量，在较长时间内过渡到较慢的退相干衰变。正如先前文献中所建议的，电子弛豫受到声子瓶颈的阻碍，从而观察到逐步的内部转换级联。计算的电子振动吸收光谱与实验光谱非常吻合。
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