Jump to main content
Jump to site search


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

Author affiliations

Abstract

Nonradiative electron–hole (e–h) recombination is the primary source of energy loss in photovoltaic cells and inevitably, it competes with the charge transfer process, leading to poor device performance. Therefore, much attention has to be paid for delaying such processes; increasing the excitonic lifetime may be a solution for this. Using the real-time, density functional tight-binding theory (DFTB) combined with nonadiabatic molecular dynamics (NAMD) simulations, we demonstrate the exciton relaxation phenomena of different metal-centered porphyrin nanoballs, which are supposed to be very important for the light-harvesting process. It has been revealed that the carrier recombination rate gradually decreases with the increase in the molecular stiffness by introducing metal-coordinating templating agents into the nanoball. Our simulation demonstrates that the lower atomic fluctuations lead to poorer electron–phonon nonadiabatic coupling in association with weak phonon modes and these as a whole are responsible for shorter quantum coherence and hence delayed recombination events. Our analysis is in good agreement with the recent experimental observation. By replacing the Zn metal center with a heavier Cd atom, a similar trend is observed; however, the rate slows down abruptly. The present simulation study provides the fundamental mechanism in detail behind the undesired energy loss during exciton recombination and suggests a rational design of impressive nanosystems for future device fabrication.

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

Back to tab navigation

Supplementary files

Article information


Submitted
02 Jan 2020
Accepted
18 Feb 2020
First published
18 Feb 2020

This article is Open Access

Nanoscale Adv., 2020, Advance Article
Article type
Paper

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

R. Sarkar, M. Habib, M. Kar, A. Pramanik, S. Pal and P. Sarkar, Nanoscale Adv., 2020, Advance Article , DOI: 10.1039/D0NA00001A

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material and it is not used for commercial purposes.

Reproduced material should be attributed as follows:

  • For reproduction of material from NJC:
    [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
  • For reproduction of material from PCCP:
    [Original citation] - Published by the PCCP Owner Societies.
  • For reproduction of material from PPS:
    [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
  • For reproduction of material from all other RSC journals:
    [Original citation] - Published by The Royal Society of Chemistry.

Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.


Social activity

Search articles by author

Spotlight

Advertisements