Exciton Diffusion and Annihilation in Nanophotonic Purcell Landscapes

T.V. Raziman; C. Peter Visser; Shaojun Wang; Jaime Gómez Rivas; Alberto G. Curto

doi:10.1002/adom.202200103

Exciton Diffusion and Annihilation in Nanophotonic Purcell Landscapes

T.V. Raziman, C. Peter Visser, Shaojun Wang, Jaime Gómez Rivas, Alberto G. Curto (Corresponding author)

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Abstract

Excitons spread through diffusion and interact through exciton–exciton annihilation. Nanophotonics can counteract the resulting decrease in light emission. However, conventional enhancement treats emitters as immobile and non-interacting. It neglects exciton redistribution between regions with different enhancements and the increase in non-radiative decay at high exciton densities. Here, the authors went beyond the localized Purcell effect to exploit exciton dynamics and turn their typically detrimental impact into additional emission. As interacting excitons diffuse through optical hotspots, the balance of excitonic and nanophotonic properties leads to either enhanced or suppressed photoluminescence. The dominant enhancement mechanisms are identified in the limits of high and low diffusion and annihilation. Diffusion lifts the requirement of spatial overlap between excitation and emission enhancements, which are harnessed to maximize emission from highly diffusive excitons. In the presence of annihilation, improved enhancement is predicted at increasing powers in nanophotonic systems dominated by emission enhancement. The guidelines are relevant for efficient and high-power light-emitting diodes and lasers tailored to the rich dynamics of excitonic materials such as monolayer semiconductors, perovskites, or organic crystals.

Original language	English
Article number	2200103
Number of pages	8
Journal	Advanced Optical Materials
Volume	10
Issue number	17
DOIs	https://doi.org/10.1002/adom.202200103
Publication status	Published - 5 Sept 2022

Bibliographical note

Funding Information:
The authors thank Rasmus H. Godiksen for illuminating discussions. This work was financially supported by the Netherlands Organization for Scientific Research (NWO) through Gravitation grant “Research Centre for Integrated Nanophotonics” (024.002.033), START‐UP grant (740.018.009), and Innovational Research Incentives Scheme (VICI Grant no. 680‐47‐628). S.W. was supported by Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Simulations in this work were carried out on the Dutch national e‐infrastructure with the support of SURF Cooperative.

Funding Information:
The authors thank Rasmus H. Godiksen for illuminating discussions. This work was financially supported by the Netherlands Organization for Scientific Research (NWO) through Gravitation grant “Research Centre for Integrated Nanophotonics” (024.002.033), START-UP grant (740.018.009), and Innovational Research Incentives Scheme (VICI Grant no. 680-47-628). S.W. was supported by Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Simulations in this work were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative.

Funding

The authors thank Rasmus H. Godiksen for illuminating discussions. This work was financially supported by the Netherlands Organization for Scientific Research (NWO) through Gravitation grant “Research Centre for Integrated Nanophotonics” (024.002.033), START‐UP grant (740.018.009), and Innovational Research Incentives Scheme (VICI Grant no. 680‐47‐628). S.W. was supported by Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Simulations in this work were carried out on the Dutch national e‐infrastructure with the support of SURF Cooperative. The authors thank Rasmus H. Godiksen for illuminating discussions. This work was financially supported by the Netherlands Organization for Scientific Research (NWO) through Gravitation grant “Research Centre for Integrated Nanophotonics” (024.002.033), START-UP grant (740.018.009), and Innovational Research Incentives Scheme (VICI Grant no. 680-47-628). S.W. was supported by Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Simulations in this work were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative.

Keywords

exciton transport
exciton–exciton annihilation
Mie resonances
nanoparticle arrays
plasmonic resonances
Purcell effect

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title = "Exciton Diffusion and Annihilation in Nanophotonic Purcell Landscapes",

abstract = "Excitons spread through diffusion and interact through exciton–exciton annihilation. Nanophotonics can counteract the resulting decrease in light emission. However, conventional enhancement treats emitters as immobile and non-interacting. It neglects exciton redistribution between regions with different enhancements and the increase in non-radiative decay at high exciton densities. Here, the authors went beyond the localized Purcell effect to exploit exciton dynamics and turn their typically detrimental impact into additional emission. As interacting excitons diffuse through optical hotspots, the balance of excitonic and nanophotonic properties leads to either enhanced or suppressed photoluminescence. The dominant enhancement mechanisms are identified in the limits of high and low diffusion and annihilation. Diffusion lifts the requirement of spatial overlap between excitation and emission enhancements, which are harnessed to maximize emission from highly diffusive excitons. In the presence of annihilation, improved enhancement is predicted at increasing powers in nanophotonic systems dominated by emission enhancement. The guidelines are relevant for efficient and high-power light-emitting diodes and lasers tailored to the rich dynamics of excitonic materials such as monolayer semiconductors, perovskites, or organic crystals.",

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author = "T.V. Raziman and Visser, {C. Peter} and Shaojun Wang and {G{\'o}mez Rivas}, Jaime and Curto, {Alberto G.}",

note = "Funding Information: The authors thank Rasmus H. Godiksen for illuminating discussions. This work was financially supported by the Netherlands Organization for Scientific Research (NWO) through Gravitation grant “Research Centre for Integrated Nanophotonics” (024.002.033), START‐UP grant (740.018.009), and Innovational Research Incentives Scheme (VICI Grant no. 680‐47‐628). S.W. was supported by Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Simulations in this work were carried out on the Dutch national e‐infrastructure with the support of SURF Cooperative. Funding Information: The authors thank Rasmus H. Godiksen for illuminating discussions. This work was financially supported by the Netherlands Organization for Scientific Research (NWO) through Gravitation grant “Research Centre for Integrated Nanophotonics” (024.002.033), START-UP grant (740.018.009), and Innovational Research Incentives Scheme (VICI Grant no. 680-47-628). S.W. was supported by Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Simulations in this work were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. ",

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AU - Wang, Shaojun

AU - Gómez Rivas, Jaime

AU - Curto, Alberto G.

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N2 - Excitons spread through diffusion and interact through exciton–exciton annihilation. Nanophotonics can counteract the resulting decrease in light emission. However, conventional enhancement treats emitters as immobile and non-interacting. It neglects exciton redistribution between regions with different enhancements and the increase in non-radiative decay at high exciton densities. Here, the authors went beyond the localized Purcell effect to exploit exciton dynamics and turn their typically detrimental impact into additional emission. As interacting excitons diffuse through optical hotspots, the balance of excitonic and nanophotonic properties leads to either enhanced or suppressed photoluminescence. The dominant enhancement mechanisms are identified in the limits of high and low diffusion and annihilation. Diffusion lifts the requirement of spatial overlap between excitation and emission enhancements, which are harnessed to maximize emission from highly diffusive excitons. In the presence of annihilation, improved enhancement is predicted at increasing powers in nanophotonic systems dominated by emission enhancement. The guidelines are relevant for efficient and high-power light-emitting diodes and lasers tailored to the rich dynamics of excitonic materials such as monolayer semiconductors, perovskites, or organic crystals.

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ER -

Exciton Diffusion and Annihilation in Nanophotonic Purcell Landscapes

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Keywords

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