arXiv subjects

Claire Tonnelé

Publications and source records attributed to Claire Tonnelé.

4 recordsLinked to original sources

arXiv2023

Efficient near-infrared organic light-emitting diodes with emission from spin doublet excitons

The development of luminescent organic radicals has resulted in materials with excellent optical properties for near-infrared (NIR) emission. Applications of light generation in this range span from bioimaging to surveillance. Whilst the unpaired electron arrangements of radicals enable efficient radiative transitions within the doublet-spin manifold in organic light-emitting diodes (OLEDs), their performance is limited by non-radiative pathways introduced in electroluminescence. Here, we present a host:guest design for OLEDs that exploits energy transfer with demonstration of up to 9.6% external quantum efficiency (EQE) for 800 nm emission. The tris(2,4,6-trichlorophenyl)methyl-triphenylamine (TTM-TPA) radical guest is energy-matched to the triplet state in a charge-transporting anthracene-derivative host. We show from optical spectroscopy and quantum-chemical modelling that reversible host-guest triplet-doublet energy transfer allows efficient harvesting of host triplet excitons.

physics.app-ph↗

arXiv2023

Reversible spin-optical interface in luminescent organic radicals

Molecules present a versatile platform for quantum information science, and are candidates for sensing and computation applications. Robust spin-optical interfaces are key to harnessing the quantum resources of materials. To date, carbon-based candidates have been non-luminescent, which prevents optical read-out. Here we report the first organic molecules displaying both efficient luminescence and near-unity generation yield of high-spin multiplicity excited states. This is achieved by designing an energy resonance between emissive doublet and triplet levels, here on covalently coupled tris(2,4,6-trichlorophenyl) methyl-carbazole radicals (TTM-1Cz) and anthracene. We observe the doublet photoexcitation delocalise onto the linked acene within a few picoseconds and subsequently evolve to a pure high spin state (quartet for monoradicals, quintet for biradical) of mixed radical-triplet character near 1.8 eV. These high-spin states are coherently addressable with microwaves even at 295 K, with optical read-out enabled by intersystem crossing to emissive states. Furthermore, for the biradical, on return to the ground state the previously uncorrelated radical spins either side of the anthracene show strong spin correlation. Our approach simultaneously supports a high efficiency of initialisation, spin manipulations and light-based read-out at room temperature. The integration of luminescence and high-spin states creates an organic materials platform for emerging quantum technologies.

cond-mat.mtrl-sci↗

arXiv2021

Spontaneous exciton dissociation enables spin state interconversion in delayed fluorescence organic semiconductors

Engineering a low singlet-triplet energy gap (ΔEST) is necessary for efficient reverse intersystem crossing (rISC) in delayed fluorescence (DF) organic semiconductors, but results in a small radiative rate that limits performance in LEDs. Here, we study a model DF material, BF2, that exhibits a strong optical absorption (absorption coefficient =3.8x10^5 cm^-1) and a relatively large ΔEST of 0.2 eV. In isolated BF2 molecules, intramolecular rISC is slow (260 μs), but in aggregated films, BF2 generates intermolecular CT (inter-CT) states on picosecond timescales. In contrast to the microsecond intramolecular rISC that is promoted by spin-orbit interactions in most isolated DF molecules, photoluminescence-detected magnetic resonance shows that these inter-CT states undergo rISC mediated by hyperfine interactions on a ~24 ns timescale and have an average electron-hole separation of >1.5 nm. Transfer back to the emissive singlet exciton then enables efficient DF and LED operation. Thus, access to these inter-CT states resolves the conflicting requirements of fast radiative emission and low ΔEST.

physics.app-ph↗

arXiv2019

Towards a background-free neutrinoless double beta decay experiment based on a fluorescent bicolor sensor

Searching for neutrinoless double beta decays ($β\beta0ν$) is the only practical way to establish if the neutrinos are their own antiparticles. Due to the smallness of neutrino masses, the lifetime of $β\beta0ν$ is expected to be at least ten orders of magnitude smaller than the noise associated with the natural radioactive chains. A positive identification of $β\beta0ν$ decays requires, ultimately, finding a signal that cannot be mimicked by radioactive backgrounds. This signal could be the observation of the daughter atom in the decay, since no known background processes induce a Z+2 transformation. In particular, the $β\beta0ν$ decay of Xe-136 could be established by detecting the doubly ionised daughter atom, Ba$^{2+}$. Such a detection could be achieved via a sensor made of a monolayer of molecular indicators. The Ba$^{2+}$ would be captured by one of the molecules in the sensor, and the presence of the single chelated indicator would be subsequently revealed by a strong fluorescent response from repeated interrogation with a laser system. Here we describe a fluorescent bicolor indicator that binds strongly to Ba$^{2+}$ and shines very brightly, shifting its emission colour from green to blue when chelated in dry medium, thus allowing the unambiguous identification of single barium atoms in the sensor, and permitting a positive identification of the $β\beta0ν$ decay of Xe-136 in a gas chamber, that could led to a background-free experiment.

physics.ins-det↗