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Applied Physics Letters

Zeeman-effect-induced luminescence suppression in Er3+-doped GdF3 nanoparticles under dual-wavelength excitation

Shuwu Xu, Huajie Chen, Lingxiao Wang, Yunxia Huang

Published Apr 1, 2025• 0 citations
Publisher

Abstract

Magnetic field-modulated luminescence in lanthanide-doped nanomaterials offers crucial insights for advancing magneto-optical technologies, yet the fundamental mechanisms governing luminescence are still not fully understood. Here, we report Zeeman-effect-induced luminescence suppression in Er3+-doped GdF3 nanoparticles under dual-wavelength excitation (808 nm broadband and 527 nm narrowband) at moderate magnetic fields (up to 1.3 T). Under 808 nm excitation, upconversion emissions (528, 546, and 656 nm) dominated by two-photon absorption exhibit >79% intensity suppression (0.89 T), attributed to energy mismatch caused by Zeeman splitting of sublevels. In contrast, under 527 nm excitation, downconversion emissions (656, 842, and 983 nm) show uniform suppression (∼66% at 1.3 T) due to magnetic field-induced splitting of the 2H11/2 energy level. A simplified model elucidates how Zeeman splitting alters absorption resonance, with theoretical calculations aligning closely with experimental trends. This study reveals the physical mechanisms of magnetic field modulation using dual-wavelength excitation, providing a foundation for expanding magneto-optical technologies in imaging and sensing applications.

DOI
10.1063/5.0267611

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Magnetic field-modulated luminescence in lanthanide-doped nanomaterials offers crucial insights for advancing magneto-optical technologies, yet the fundamental mechanisms governing luminescence are still not fully understood. Here, we report Zeeman-effect-induced luminescence suppression in Er3+-doped GdF3 nanoparticles under dual-wavelength excitation (808 nm broadband and 527 nm narrowband) at moderate magnetic fields (up to 1.3 T). Under 808 nm excitation, upconversion emissions (528, 546, and 656 nm) dominated by two-photon absorption exhibit >79% intensity suppression (0.89 T), attributed to energy mismatch caused by Zeeman splitting of sublevels. In contrast, under 527 nm excitation, downconversion emissions (656, 842, and 983 nm) show uniform suppression (∼66% at 1.3 T) due to magnetic field-induced splitting of the 2H11/2 energy level. A simplified model elucidates how Zeeman splitting alters absorption resonance, with theoretical calculations aligning closely with experimental trends. This study reveals the physical mechanisms of magnetic field modulation using dual-wavelength excitation, providing a foundation for expanding magneto-optical technologies in imaging and sensing applications.
An optical method for the sensitive detection of excited energy levels in rare-earth luminescent materials is developed based on the magnetic field induced photoluminescence (PL) enhancement phenomenon observed in Er3+:YVO4 crystals. Since the PL intensity of rare-earth luminescent materials is sensitive to the excitation efficiency, continuous tuning of the excitation laser wavelength under a magnetic field could result in a mapping of PL enhancement peaks vs excitation wavelength. This enables us to figure out the fine energy levels and the corresponding Lander g factors of materials, such as Er3+:YVO4 crystal as an example. Comparison between this method and the Zeeman splitting technique demonstrates that the proposed technique is a powerful solution to detect the fine energy structures and Lander g factors of rare-earth luminescent materials.
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The effect of magnetic field on luminescence intensity is generally expected to be rather weak. Contrary to this expectation, we report here an extraordinary strong intensity suppression (by two orders of magnitude) of the Er3+ S43/2→I415/2 green emission line in Er3+-doped nano-glass-ceramics by applying magnetic field up to 50 T. We argue that this effect arises from different site geometries and, consequently, strongly differing Judd–Ofelt intensities of transitions for the two Kramers doublets of the emitting S43/2 multiplet.
A bright green photoluminescence (PL) from 4S3∕2 → 4I15∕2 emission band in Er3+:YVO4 single crystal has been observed with the excitation of an argon laser at 488.0 nm. More than two orders of PL enhancement have been obtained under the effect of magnetic fields, and the enhancement factor f reaches 170 when the applied magnetic field is 7.7 T under the sample temperature of 4.2 K. Unusually, the PL enhancements only happen at some certain magnetic fields (Bcs), and a decrease of sample temperature will lead to the increase of f and decrease of Bc. The results confirm that this PL enhancement originates from the resonance excitation of the electron transitions induced by the cross of the laser energy and the absorption energy modulated by both the magnetic field and temperature. This special PL enhancement in Er3+:YVO4 single crystal can be applied in the calibration of pulsed high magnetic field, detection of material fine energy structures, and modulation of magneto-optical devices.
Fundamental studies of light-matter interactions are important for basic knowledge and in applications. Thanks to advances in experimental and theoretical methods, nowadays it is possible to perform such studies in a broad dynamic range, covering timescales from that of elementary interactions to real time. In the present work, we perform an experimental-theoretical study of light intensity-dependent femtosecond and CW-laser induced frequency upconversion in hierarchically structured core-multishell nanoparticles co-doped with NdIII, YbIII, and ErIII. Upconversion spectra recorded with CW and femtosecond excitation are qualitatively similar whereas the intensity dependence of upconversion depends on excitation mode (CW or femtosecond). To further assess the observed intensity dependence, we perform light-matter interaction simulations in the dynamic range from 100 fs to 3 ms for 18-level system describing the UCNPs, including 9 NdIII levels, 2 YbIII, and 7 ErIII levels and a classical model for the excitation source. The calculated time- and intensity-dependent energy level population are compared with measured spectra to understand CW vs femtosecond laser-induced upconversion. To further discuss the differences between CW and femtosecond laser-induced light-matter interactions for the systems studied here, we perform semi-classical pulse propagation simulations and ultrafast pump-probe measurements to study how the light source bandwidth, relative to the absorption linewidth, influence light absorption and transmission and further connect these results with the intensity dependence. Overall, we report our progress toward mechanistic studies of light-matter interaction and photophysical pathways following femtosecond excitation and UCNPs.
We present a dual-wavelength analysis of nitrogen-vacancy (NV) center quantum magnetometry enhanced by uniformly coated gold nanoparticles (AuNPs). An ensemble-averaged model is developed to analyze the AuNP-enhanced stimulated absorption at the 532 nm excitation wavelength and the spontaneous emission at 637 nm. The resulting detected optically magnetic resonance (ODMR) signal profiles are simulated for both enhancement mechanisms. We find that the enhanced stimulated absorption at 532 nm significantly amplifies the ODMR signal intensity without broadening the linewidth, thereby improving the signal-to-noise ratio (SNR) without sacrificing the magnetic field sensing resolution. Conversely, enhancing the 637 nm spontaneous emission increases the total photo emission rate but simultaneously broadens the ODMR detection linewidth due to the direct reduction in the effective spin coherence time of excited states by the enhanced spontaneous rate. The dual-wavelength analysis provides valuable design guidance for the development of low-cost spin-coated AuNP-enhanced NV-center quantum magnetometry technologies.