Structural rigidity accelerates quantum decoherence and extends carrier lifetime in porphyrin nanoballs: a time domain atomistic simulation

Abstract

Structural rigidity assists to weaken the NA electron–phonon coupling, shorten the quantum coherence and thus suppress the dynamics of electron–hole recombination.

Mixed Metals Slow Down Nonradiative Recombination in Saddle-Shaped Porphyrin Nanorings: A Time-Domain Atomistic Simulation

“…Introduction of Cd centers into the nanorings causes gap contraction (Figure b,c and Table ). The decrease in the optical gap is explained by the increasing molecular weight of the macrostructures with the replacement of Zn by Cd; this is similar to our previous work …”

“…CPA is applicable when any significant structural changes such as isomerization, reorganization, or fragmentation do not occur due to an electronic transition, and the nuclear dynamics is dominated by thermal fluctuations. To account for the effect of decoherence, the decoherence-induced surface hopping (DISH) approach is used, as implemented in the PYthon eXtension for Ab Initio Dynamics (PYXAID) code. , The SCC-DFTB method combined with NAMD has been successfully employed in a variety of systems including CNT nanohybrid composites, − cadmium chalcogenide quantum dots and nanoplatelets, , and porphyrin macromolecular systems . The closely related approach based on ab initio DFT has been applied to an even broader set of systems. − The details of the theoretical method are given in the Supporting Information.…”

“…46,47 The SCC-DFTB method combined with NAMD has been successfully employed in a variety of systems including CNT nanohybrid composites, 48−52 cadmium chalcogenide quantum dots 53 and nanoplatelets, 54,55 and porphyrin macromolecular systems. 56 The closely related approach based on ab initio DFT has been applied to an even broader set of systems. 57−65 The details of the theoretical method are given in the Supporting Information.…”

Common Defects Accelerate Charge Separation and Reduce Recombination in CNT/Molecule Composites: Atomistic Quantum Dynamics

“…The methodology has been successfully applied to a variety of nano systems, including pristine CNT [14][15] and CNT composite, 16 cadmium chalcogenide quantum dots 17 and nanoplateletes, [18][19] and various porphyrin macro structures. 20 Fewest switching surface hopping (FSSH) [21][22][23] is used to simulate the charge separation process. Decoherence-induced surface hopping (DISH) 24 is applied for the simulation of the e-h recombination across the wide energy gap.…”

“…The more recent DISH approach has been used successfully for investigation of excited state dynamics in various systems. 16,20,25 Both FSSH and DISH are implemented in the PYthon eXtension for Ab Initio Dynamics (PYXAID) software package. [26][27]…”