Predicting the Excitation Dynamics in Lanthanide Nanoparticles

authored by: Simon Spelthann, Jonas Thiem, Oliver Melchert, Rajesh Komban, Christoph Gimmler, Ayhan Demicran, Axel Ruehl, Detlev Ristau
Abstract: With their dipole-forbidden 4f transitions, lanthanides doped in nanoparticles promise high excited state lifetimes and quantum yields that are required for applications such as composite lasers or nanoscale quantum memories. Quenching at the nanoparticle surface, however, severely reduces the lifetime and quantum yield and requires resource-consuming experimental optimization that could not be replaced by simulations due to the limitations of existing approaches until now. Here, a versatile approach is presented that fully accounts for spatiotemporal dynamics and reliably predicts the lifetimes and quantum yields of lanthanide nanoparticles. LiYF₄:Pr³⁺nanoparticles are synthesized as a model system, and the lifetimes of a concentration series (≈10 nm, 0.7−1.47 at%) are used to match the model parameters to the experimental conditions. Employing these parameters, the lifetimes and quantum yields of a size series (≈5 at%, 12−21 nm) are predicted with a maximum uncertainty of 12.6%. To demonstrate the potential of the model, a neutral shell is added around the core particles in the model which extends the lifetime by up to 44%. Furthermore, spatiotemporal analysis of single nanoparticles points toward a new type of energy trapping in lanthanide nanoparticles. Consequently, the numerical optimization brings applications such as efficient nanoparticle lasers or quantum memories within reach.
Organisation(s): Institute of Quantum Optics
PhoenixD: Photonics, Optics, and Engineering - Innovation Across Disciplines
QUEST-Leibniz Research School
External Organisation(s): Fraunhofer Center for Applied Nanotechnology (CAN)
Type: Article
Journal: Advanced optical materials
Volume: 11
ISSN: 2195-1071
Publication date: 18.07.2023
Publication status: Published
Peer reviewed: Yes
ASJC Scopus subject areas: Electronic, Optical and Magnetic Materials, Atomic and Molecular Physics, and Optics
Electronic version(s): https://doi.org/10.1002/adom.202300096 (Access: Open)

BibTeX

@article{7c9d819bd5ef45f2b0118b7b248a3280,
title = "Predicting the Excitation Dynamics in Lanthanide Nanoparticles",
abstract = "With their dipole-forbidden 4f transitions, lanthanides doped in nanoparticles promise high excited state lifetimes and quantum yields that are required for applications such as composite lasers or nanoscale quantum memories. Quenching at the nanoparticle surface, however, severely reduces the lifetime and quantum yield and requires resource-consuming experimental optimization that could not be replaced by simulations due to the limitations of existing approaches until now. Here, a versatile approach is presented that fully accounts for spatiotemporal dynamics and reliably predicts the lifetimes and quantum yields of lanthanide nanoparticles. LiYF4:Pr3+nanoparticles are synthesized as a model system, and the lifetimes of a concentration series (≈10 nm, 0.7−1.47 at%) are used to match the model parameters to the experimental conditions. Employing these parameters, the lifetimes and quantum yields of a size series (≈5 at%, 12−21 nm) are predicted with a maximum uncertainty of 12.6%. To demonstrate the potential of the model, a neutral shell is added around the core particles in the model which extends the lifetime by up to 44%. Furthermore, spatiotemporal analysis of single nanoparticles points toward a new type of energy trapping in lanthanide nanoparticles. Consequently, the numerical optimization brings applications such as efficient nanoparticle lasers or quantum memories within reach.",
keywords = "core/shell nanoparticles, luminescence, Monte Carlo simulations, praseodymium",
author = "Simon Spelthann and Jonas Thiem and Oliver Melchert and Rajesh Komban and Christoph Gimmler and Ayhan Demicran and Axel Ruehl and Detlev Ristau",
note = "Funding Information: Funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy – EXC‐2123 Quantum Frontiers – 390837967. O.M., A.D., and D. R. would like to thank the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for partly funding this work under Germany's Excellence Strategy within the Cluster of Excellence PhoenixD (EXC‐2122, Project ID 390833453). R. K. and C. G. would like to thank the Free and Hanseatic City of Hamburg, Germany for the financial support. The numerical results presented here were achieved by computations carried out on the LUH cluster system funded by the Leibniz Universit{\"a}t Hannover, the Nieders{\"a}chsisches Ministerium f{\"u}r Wissenschaft und Kultur (MWK, Lower Saxony Ministry of Science and Culture), and the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation). Dr. Christian Kraenkel and Dr. Sascha Kalusniak, Leibniz‐Institut f{\"u}r Kristallz{\"u}chtung Berlin, Germany provided absorption and emission data for the overlap spectra. S.S. thanks Tamara Grossmann, University of Cambridge, and Dr. Torben Sell, University of Edinburgh, for helpful discussions on probability theory. The authors thank Dan Huy Chau for the graphic realization of the ToC figure. ",
year = "2023",
month = jul,
day = "18",
doi = "10.1002/adom.202300096",
language = "English",
volume = "11",
journal = "Advanced optical materials",
issn = "2195-1071",
publisher = "John Wiley and Sons Inc.",
number = "14",
}