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Incidence of Quantum Confinement on Dark Triplet Excitons in Carbon Nanotubes.

ABSTRACT: The photophysics of single-wall carbon nanotubes (SWCNTs) is intensively studied due to their potential application in light harvesting and optoelectronics. Excited states of SWCNTs form strongly bound electron-hole pairs, excitons, of which only singlet excitons participate in application relevant optical transitions. Long-living spin-triplet states hinder applications, but they emerge as candidates for quantum information storage. Therefore, knowledge of the triplet exciton energy structure, in particular in a SWCNT chirality dependent manner, is greatly desired. We report the observation of light emission from triplet state recombination, i.e., phosphorescence, for several SWCNT chiralities using a purpose-built spectrometer. This yields the singlet-triplet gap as a function of the SWCNT diameter, and it follows predictions based on quantum confinement effects. Saturation under high microwave power (up to 10 W) irradiation allows the spin-relaxation time for triplet states to be determined. Our study sensitively discriminates whether the lowest optically active state is populated from an excited state on the same nanotube or through Förster exciton energy transfer from a neighboring nanotube.

SUBMITTER: Palotas J

PROVIDER: S-EPMC7513465 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

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Incidence of Quantum Confinement on Dark Triplet Excitons in Carbon Nanotubes.

Palotás J J Negyedi M M Kollarics S S Bojtor A A Rohringer P P Pichler T T Simon F F

ACS nano 20200819 9

The photophysics of single-wall carbon nanotubes (SWCNTs) is intensively studied due to their potential application in light harvesting and optoelectronics. Excited states of SWCNTs form strongly bound electron-hole pairs, excitons, of which only singlet excitons participate in application relevant optical transitions. Long-living spin-triplet states hinder applications, but they emerge as candidates for quantum information storage. Therefore, knowledge of the triplet exciton energy structure, i ...[more]

PMID: 32790277

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Project description:Singlet fission is an exciton multiplication process in organic molecules in which a photogenerated spin-singlet exciton is rapidly and efficiently converted to two spin-triplet excitons. This process offers a mechanism to break the Shockley-Queisser limit by overcoming the thermalization losses inherent to all single-junction photovoltaics. One of the most promising methods to harness the singlet fission process is via the efficient extraction of the dark triplet excitons into quantum dots (QDs) where they can recombine radiatively, thereby converting high-energy photons to pairs of low-energy photons, which can then be captured in traditional inorganic PVs such as Si. Such a singlet fission photon multiplication (SF-PM) process could increase the efficiency of the best Si cells from 26.7% to 32.5%, breaking the Shockley-Queisser limit. However, there has been no demonstration of such a singlet fission photon multiplication (SF-PM) process in a bulk system to date. Here, we demonstrate a solution-based bulk SF-PM system based on the singlet fission material TIPS-Tc combined with PbS QDs. Using a range of steady-state and time-resolved measurements combined with analytical modeling we study the dynamics and mechanism of the triplet harvesting process. We show that the system absorbs >95% of incident photons within the singlet fission material to form singlet excitons, which then undergo efficient singlet fission in the solution phase (135 ± 5%) before quantitative harvesting of the triplet excitons (95 ± 5%) via a low concentration of QD acceptors, followed by the emission of IR photons. We find that in order to achieve efficient triplet harvesting it is critical to engineer the surface of the QD with a triplet transfer ligand and that bimolecular decay of triplets is potentially a major loss pathway which can be controlled via tuning the concentration of QD acceptors. We demonstrate that the photon multiplication efficiency is maintained up to solar fluence. Our results establish the solution-based SF-PM system as a simple and highly tunable platform to understand the dynamics of a triplet energy transfer process between organic semiconductors and QDs, one that can provide clear design rules for new materials.

Dataset Information

Incidence of Quantum Confinement on Dark Triplet Excitons in Carbon Nanotubes.

Publications

Incidence of Quantum Confinement on Dark Triplet Excitons in Carbon Nanotubes.

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