On-the-Fly Nonadiabatic Dynamics Simulations of Single-Walled Carbon Nanotubes with Covalent Defects.
ACS Nano
; 17(7): 6208-6219, 2023 Apr 11.
Article
in En
| MEDLINE
| ID: mdl-36972076
ABSTRACT
Single-walled carbon nanotubes (SWCNTs) with covalent surface defects have been explored recently due to their promise for use in single-photon telecommunication emission and in spintronic applications. The all-atom dynamic evolution of electrostatically bound excitons (the primary electronic excitations) in these systems has only been loosely explored from a theoretical perspective due to the size limitations of these large systems (>500 atoms). In this work, we present computational modeling of nonradiative relaxation in a variety of SWCNT chiralities with single-defect functionalizations. Our excited-state dynamics modeling uses a trajectory surface hopping algorithm accounting for excitonic effects with a configuration interaction approach. We find a strong chirality and defect-composition dependence on the population relaxation (varying over 50-500 fs) between the primary nanotube band gap excitation E11 and the defect-associated, single-photon-emitting E11* state. These simulations give direct insight into the relaxation between the band-edge states and the localized excitonic state, in competition with dynamic trapping/detrapping processes observed in experiment. Engineering fast population decay into the quasi-two-level subsystem with weak coupling to higher-energy states increases the effectiveness and controllability of these quantum light emitters.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
ACS Nano
Year:
2023
Type:
Article
Affiliation country:
United States