Phonon-mediated temperature dependence of Er3+ optical transitions in Er2O3

Adam Dodson; Hongrui Wu; Anuruddh Rai; Sohm Apte; Andrew O’Hara; Benjamin Lawrie; Yongqiang Wang; Akira Ueda; Halina Krzyżanowska; Michael Titze; Jimmy Davidson; Anthony Hmelo; Agham B. Posadas; Alexander A. Demkov; Sokrates T. Pantelides; Leonard C. Feldman; Norman H. Tolk

doi:10.1038/s42005-024-01559-z

Phonon-mediated temperature dependence of Er³⁺ optical transitions in Er₂O₃

Adam Dodson, Hongrui Wu, Anuruddh Rai, Sohm Apte, Andrew O’Hara, Benjamin Lawrie, Yongqiang Wang, Akira Ueda, Halina Krzyżanowska, Michael Titze, Jimmy Davidson, Anthony Hmelo, Agham B. Posadas, Alexander A. Demkov, Sokrates T. Pantelides, Leonard C. Feldman, Norman H. Tolk

Quantum Heterostructures

Research output: Contribution to journal › Article › peer-review

Abstract

Characterization of the atomic level processes that determine optical transitions in emerging materials is critical to the development of new platforms for classical and quantum networking. Such understanding often emerges from studies of the temperature dependence of the transitions. We report measurements of the temperature dependent Er³⁺ photoluminescence in single crystal Er₂O₃ thin films epitaxially grown on Si(111) focused on transitions that involve the closely spaced Stark-split levels. Radiative intensities are compared to a model that includes relevant Stark-split states, single phonon-assisted excitations, and the well-established level population redistribution due to thermalization. This approach, applied to the individual Stark-split states and employing Er₂O₃ specific single-phonon-assisted excitations, gives good agreement with experiment. This model allows us to demonstrate the difference in the electron-phonon coupling of the ⁴S_3/2 and ²H_11/2 states of Er³⁺ in E₂O₃ and suggests that the temperature dependence of Er³⁺ emission intensity may vary significantly with small shifts in the wavelength (~0.1 nm) of the excitation source.

Original language	English
Article number	69
Journal	Communications Physics
Volume	7
Issue number	1
DOIs	https://doi.org/10.1038/s42005-024-01559-z
State	Published - Dec 2024

Funding

The work at Vanderbilt University was supported by funds from the School of Arts and Science and by the McMinn Endowment. The work at the University of Texas was supported by the Air Force Office of Scientific Research under grant FA9550-18-1-0053. Photoluminescence microscopy was supported by the Center for Nanophase Materials Sciences (CNMS2022-B-01577), a U.S. Department of Energy Office of Science User Facility. This work was performed, in part, at the Center for Integrated Nanotechnologies (CINT#2022AU0120), an Office of Science User Facility operated by the U.S. Department of Energy (DOE) Office of Science. Los Alamos National Laboratory, an affirmative action-equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy’s NNSA, under contract 89233218CNA000001.

Funders	Funder number
Center for Nanophase Materials Sciences	CNMS2022-B-01577
McMinn Endowment
U.S. Department of Energy
Air Force Office of Scientific Research	FA9550-18-1-0053
Office of Science	2022AU0120
Los Alamos National Laboratory	89233218CNA000001
School of Arts and Sciences, University of Richmond

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Dodson, A., Wu, H., Rai, A., Apte, S., O’Hara, A., Lawrie, B., Wang, Y., Ueda, A., Krzyżanowska, H., Titze, M., Davidson, J., Hmelo, A., Posadas, A. B., Demkov, A. A., Pantelides, S. T., Feldman, L. C., & Tolk, N. H. (2024). Phonon-mediated temperature dependence of Er³⁺ optical transitions in Er₂O₃. Communications Physics, 7(1), Article 69. https://doi.org/10.1038/s42005-024-01559-z

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abstract = "Characterization of the atomic level processes that determine optical transitions in emerging materials is critical to the development of new platforms for classical and quantum networking. Such understanding often emerges from studies of the temperature dependence of the transitions. We report measurements of the temperature dependent Er3+ photoluminescence in single crystal Er2O3 thin films epitaxially grown on Si(111) focused on transitions that involve the closely spaced Stark-split levels. Radiative intensities are compared to a model that includes relevant Stark-split states, single phonon-assisted excitations, and the well-established level population redistribution due to thermalization. This approach, applied to the individual Stark-split states and employing Er2O3 specific single-phonon-assisted excitations, gives good agreement with experiment. This model allows us to demonstrate the difference in the electron-phonon coupling of the 4S3/2 and 2H11/2 states of Er3+ in E2O3 and suggests that the temperature dependence of Er3+ emission intensity may vary significantly with small shifts in the wavelength (~0.1 nm) of the excitation source.",

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AU - Dodson, Adam

AU - Wu, Hongrui

AU - Rai, Anuruddh

AU - Apte, Sohm

AU - O’Hara, Andrew

AU - Lawrie, Benjamin

AU - Wang, Yongqiang

AU - Ueda, Akira

AU - Krzyżanowska, Halina

AU - Titze, Michael

AU - Davidson, Jimmy

AU - Hmelo, Anthony

AU - Posadas, Agham B.

AU - Demkov, Alexander A.

AU - Pantelides, Sokrates T.

AU - Feldman, Leonard C.

AU - Tolk, Norman H.

PY - 2024/12

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N2 - Characterization of the atomic level processes that determine optical transitions in emerging materials is critical to the development of new platforms for classical and quantum networking. Such understanding often emerges from studies of the temperature dependence of the transitions. We report measurements of the temperature dependent Er3+ photoluminescence in single crystal Er2O3 thin films epitaxially grown on Si(111) focused on transitions that involve the closely spaced Stark-split levels. Radiative intensities are compared to a model that includes relevant Stark-split states, single phonon-assisted excitations, and the well-established level population redistribution due to thermalization. This approach, applied to the individual Stark-split states and employing Er2O3 specific single-phonon-assisted excitations, gives good agreement with experiment. This model allows us to demonstrate the difference in the electron-phonon coupling of the 4S3/2 and 2H11/2 states of Er3+ in E2O3 and suggests that the temperature dependence of Er3+ emission intensity may vary significantly with small shifts in the wavelength (~0.1 nm) of the excitation source.

AB - Characterization of the atomic level processes that determine optical transitions in emerging materials is critical to the development of new platforms for classical and quantum networking. Such understanding often emerges from studies of the temperature dependence of the transitions. We report measurements of the temperature dependent Er3+ photoluminescence in single crystal Er2O3 thin films epitaxially grown on Si(111) focused on transitions that involve the closely spaced Stark-split levels. Radiative intensities are compared to a model that includes relevant Stark-split states, single phonon-assisted excitations, and the well-established level population redistribution due to thermalization. This approach, applied to the individual Stark-split states and employing Er2O3 specific single-phonon-assisted excitations, gives good agreement with experiment. This model allows us to demonstrate the difference in the electron-phonon coupling of the 4S3/2 and 2H11/2 states of Er3+ in E2O3 and suggests that the temperature dependence of Er3+ emission intensity may vary significantly with small shifts in the wavelength (~0.1 nm) of the excitation source.

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Phonon-mediated temperature dependence of Er³⁺ optical transitions in Er₂O₃

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