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arXiv:2609.38892

Optical studies of negative g-factor dopants in an antiferromagnet: Nd:GdVO$_4$

Lachlan W. Cronin, Masaya Hiraishi, Luke S. Trainor, Jevon J. Longdell

quant-phcond-mat.str-elSubmitted Sep 30, 2026• Announced Oct 1, 2026• 0 citations
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Abstract

Neodymium-doped gadolinium vanadate (Nd:GdVO$_4$) is a popular laser material at room temperature. It has received limited attention for quantum technologies because of the linebroadening effects of disordered gadolinium spins in the host. Here we investigate the optical properties at temperatures below the 2.5 K Néel temperature, revealing narrow optical transitions. We demonstrate that rare earth ions in magnetic hosts give us a new way of observing the signs of magnetic g-factors. The interplay between the exchange and Zeeman interactions means that we see clear evidence of negative g-factors. These results provide a detailed spectroscopic foundation for Nd:GdVO$_4$ and expand the understanding of its candidacy as a material for hybrid quantum systems.

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A Cluster-Based Model of the Spectrum of Erbium-Doped GdVO$_4$

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Experimental observations of rare-earth ions doped into an antiferromagnetic crystal show an enriched optical spectrum. In this paper we present a cluster-based model to describe erbium ions doped into a gadolinium vanadate (Er:GdVO$_4$) host crystal, wherein the erbium ion couples directly to its four nearest neighbour gadolinium ions, which in turn couple to the mean field of the rest of the crystal. Compared to previous models in the literature, the parameters used to fit this model are fewer in number, with clearer physical origins. Agreement with the experimentally observed optical spectrum of Er:GdVO$_4$ suggests that our model succeeds in capturing the most important interactions of the system, suggesting that it may be useful for predicting microwave-to-optical transduction in future experiments.

cond-mat.mtrl-sciCross-listedarXiv:2607.10924•Jul 14, 2026•0 citations

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The narrowness of the optical transitions of rare-earth-ion dopants makes them highly sensitive probes of their environment. We measured the optical transitions Er$^{3+}$ dopants to determine the previously unknown magnetic ordering of Gd$_{2}$SiO$_{5}$ -- a promising host for quantum applications of rare-earth dopants. By measuring the transitions' magnetic-field dependence we determined an antiferromagnetic ordering with spins oriented along or slightly canted from the crystal's $a^*$ axis. The optical transitions are narrower than the coupling to gadolinium spins revealing information about the coupling strengths. We further optically measured a Néel temperature of $1.86\pm0.01_\mathrm{stat.}\pm0.07_\mathrm{syst.}$ K, and assembled a phase diagram in applied field and temperature showcasing a triple point where two gadolinium sites order semi-independently from each other. At high applied field the erbium dopants show long optical coherence times up to 0.4 ms at 3 T; at low fields these are probably limited by three low-frequency magnon modes below 10 GHz, observed directly. This study can be used to benchmark a method of magnetic structure determination.

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Microwave and optical transitions of rare-earth ions enable microwave-to-optical frequency transduction. This transduction is a coherent process; therefore, the narrow linewidths and long coherence times of rare-earth ions are crucial for achieving efficient frequency conversion. Particularly long coherence times can be achieved with small-spin materials, as unpaired electronic and nuclear spins introduce magnetic noise, serving as a decoherent source of the transitions. However, complete spin-free rare-earth materials cannot exist without charge compensation. Consequently, residual spins in existing rare-earth materials act as a bottleneck, limiting both their spin and optical coherence times. Rather than focusing on nearly spin-free materials, this thesis investigates the microwave and optical transitions of rare-earth ions in materials that are fully concentrated with electronic spins. Recent studies on rare-earth magnetic materials have demonstrated narrow optical linewidths resulting from magnetic ordering and a particularly strong coupling between microwave cavity modes and the collective excitations of rare-earth ions. Although these recent studies are noteworthy, the energy-level transitions, especially optical transitions, of rare-earth ions in magnetic materials remain largely unexamined. In this thesis, various spectroscopic studies are employed to characterise their transition properties and to develop a model of energy levels. The model presented is expected to be applicable to other rare-earth magnetic materials, thereby opening avenues for further investigation in this class of systems. Two types of rare-earth magnetic materials are investigated: neodymium gallate with a stoichiometric concentration of neodymium ions, and gadolinium vanadate doped with a low (ppm) concentration of erbium ions. Microwave and optical transmission spectroscopy are employed under externally applied magnetic fields to characterise the energy-state transitions of the rare-earth ions in both materials. The magnetic phases and corresponding spin configurations influence the observed spectra, making conventional approaches to spectral simulation inadequate. To address this challenge, mean field and magnon-coupled crystal-field models are developed in this thesis to predict magnon and optical transition spectra. These simulations exhibit good agreement with experimental results, allowing for the characterisation of transition properties. Following the characterisation of the material, a new transduction approach is introduced, developed, and implemented using doped rare-earth ions in a magnetic material. In this scheme, coherent conversion between microwave and optical modes is achieved by exciting an optical transition of the doped ions.

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We identify and analyze dephasing mechanisms that broaden the optical transitions of rare-earth ions in randomly oriented transparent ceramics. The study examines the narrow $^{7}F_{0}\phantom{\rule{4pt}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{4pt}{0ex}}^{5}D_{0}$ transition of ${\mathrm{Eu}}^{3+}$ dopants in a series of ${\mathrm{Y}}_{2}{\mathrm{O}}_{3}$ ceramic samples prepared under varying conditions. We characterize the temperature and magnetic field dependence of the homogeneous linewidth, as well as long-term spectral diffusion on time scales up to 1 s. The results highlight significant differences between samples with differing thermal treatments and ${\mathrm{Zr}}^{4+}$ additive concentrations. In particular, several distinct magnetic interactions from defect centers are observed, which are clearly distinguished from the broadening due to interactions with two-level systems and phonons. By minimizing the broadening due to the different defect centers, linewidths of the order of 4 kHz are achieved for all samples. The linewidths are limited by temperature-dependent interactions and by an interaction that is yet to be identified. Although the homogeneous linewidth can be narrowed further in these ceramic samples, the broadening is now comparable to the linewidths achieved in rare-earth-ion--doped single crystals. Thus, this work emphasizes the usefulness of studying ceramics to gain insights into dephasing mechanisms relevant to single crystals and suggests that ceramics may be an interesting alternative for applications in classical and quantum information processing.

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arXiv:1609.07406•Physical review. B./Physical review. B•Nov 21, 2016•25 citations
Optical studies of negative g-factor dopants in an antiferromagnet: Nd:GdVO4_44​
Neodymium-doped gadolinium vanadate (Nd:GdVO4_44​) is a popular laser material at room temperature. It has received limited attention for quantum technologies because of the linebroadening effects of disordered gadolinium spins in the host. Here we investigate the optical properties at temperatures below the 2.5 K Néel temperature, revealing narrow optical transitions. We demonstrate that rare earth ions in magnetic hosts give us a new way of observing the signs of magnetic g-factors. The interplay between the exchange and Zeeman interactions means that we see clear evidence of negative g-factors. These results provide a detailed spectroscopic foundation for Nd:GdVO4_44​ and expand the understanding of its candidacy as a material for hybrid quantum systems.
A Cluster-Based Model of the Spectrum of Erbium-Doped GdVO4_44​
Experimental observations of rare-earth ions doped into an antiferromagnetic crystal show an enriched optical spectrum. In this paper we present a cluster-based model to describe erbium ions doped into a gadolinium vanadate (Er:GdVO4_44​) host crystal, wherein the erbium ion couples directly to its four nearest neighbour gadolinium ions, which in turn couple to the mean field of the rest of the crystal. Compared to previous models in the literature, the parameters used to fit this model are fewer in number, with clearer physical origins. Agreement with the experimentally observed optical spectrum of Er:GdVO4_44​ suggests that our model succeeds in capturing the most important interactions of the system, suggesting that it may be useful for predicting microwave-to-optical transduction in future experiments.
Elucidating magnetic structure with optical dopants: erbium-doped Gd2_22​SiO5_55​
The narrowness of the optical transitions of rare-earth-ion dopants makes them highly sensitive probes of their environment. We measured the optical transitions Er3+^{3+}3+ dopants to determine the previously unknown magnetic ordering of Gd2_{2}2​SiO5_{5}5​ -- a promising host for quantum applications of rare-earth dopants. By measuring the transitions' magnetic-field dependence we determined an antiferromagnetic ordering with spins oriented along or slightly canted from the crystal's a∗a^*a∗ axis. The optical transitions are narrower than the coupling to gadolinium spins revealing information about the coupling strengths. We further optically measured a Néel temperature of 1.86±0.01stat.±0.07syst.1.86\pm0.01_\mathrm{stat.}\pm0.07_\mathrm{syst.}1.86±0.01stat.​±0.07syst.​ K, and assembled a phase diagram in applied field and temperature showcasing a triple point where two gadolinium sites order semi-independently from each other. At high applied field the erbium dopants show long optical coherence times up to 0.4 ms at 3 T; at low fields these are probably limited by three low-frequency magnon modes below 10 GHz, observed directly. This study can be used to benchmark a method of magnetic structure determination.
We characterise optical transitions of neodymium ions (Nd3+) in antiferromagnetic neodymium gallate (NdGaO3) with applied fields up to 3 T. The magnetic phase of this material has not previously been studied with the field along its magnetisation axis. The measured optical spectra indicate three magnetic phases -- antiferromagnetic, intermediate, and paramagnetic -- where the intermediate phase likely forms a different magnetic structure from typical spin-flop phases. The observed absorptions were classified into two distinct families of optical transitions: single-Nd and two-Nd absorptions. We demonstrate that the optical transitions in the antiferromagnetic and paramagnetic phases can be modelled using a standard single-ion crystal-field Hamiltonian that interacts with a mean magnetisation from the rest of the lattice, and we expand that model to encompass pairs of ions, explaining the origins of the two-Nd transitions. This study offers a deeper understanding of the optical transitions in rare-earth antiferromagnetic crystals, which have been recently attracting significant interest for microwave-to-optical quantum transduction, despite being relatively unexplored to date.
Microwave and optical transitions of rare-earth ions enable microwave-to-optical frequency transduction. This transduction is a coherent process; therefore, the narrow linewidths and long coherence times of rare-earth ions are crucial for achieving efficient frequency conversion. Particularly long coherence times can be achieved with small-spin materials, as unpaired electronic and nuclear spins introduce magnetic noise, serving as a decoherent source of the transitions. However, complete spin-free rare-earth materials cannot exist without charge compensation. Consequently, residual spins in existing rare-earth materials act as a bottleneck, limiting both their spin and optical coherence times. Rather than focusing on nearly spin-free materials, this thesis investigates the microwave and optical transitions of rare-earth ions in materials that are fully concentrated with electronic spins. Recent studies on rare-earth magnetic materials have demonstrated narrow optical linewidths resulting from magnetic ordering and a particularly strong coupling between microwave cavity modes and the collective excitations of rare-earth ions. Although these recent studies are noteworthy, the energy-level transitions, especially optical transitions, of rare-earth ions in magnetic materials remain largely unexamined. In this thesis, various spectroscopic studies are employed to characterise their transition properties and to develop a model of energy levels. The model presented is expected to be applicable to other rare-earth magnetic materials, thereby opening avenues for further investigation in this class of systems. Two types of rare-earth magnetic materials are investigated: neodymium gallate with a stoichiometric concentration of neodymium ions, and gadolinium vanadate doped with a low (ppm) concentration of erbium ions. Microwave and optical transmission spectroscopy are employed under externally applied magnetic fields to characterise the energy-state transitions of the rare-earth ions in both materials. The magnetic phases and corresponding spin configurations influence the observed spectra, making conventional approaches to spectral simulation inadequate. To address this challenge, mean field and magnon-coupled crystal-field models are developed in this thesis to predict magnon and optical transition spectra. These simulations exhibit good agreement with experimental results, allowing for the characterisation of transition properties. Following the characterisation of the material, a new transduction approach is introduced, developed, and implemented using doped rare-earth ions in a magnetic material. In this scheme, coherent conversion between microwave and optical modes is achieved by exciting an optical transition of the doped ions.
We identify and analyze dephasing mechanisms that broaden the optical transitions of rare-earth ions in randomly oriented transparent ceramics. The study examines the narrow $^{7}F_{0}\phantom{\rule{4pt}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{4pt}{0ex}}^{5}D_{0}$ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ dopants in a series of Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ ceramic samples prepared under varying conditions. We characterize the temperature and magnetic field dependence of the homogeneous linewidth, as well as long-term spectral diffusion on time scales up to 1 s. The results highlight significant differences between samples with differing thermal treatments and Zr4+{\mathrm{Zr}}^{4+}Zr4+ additive concentrations. In particular, several distinct magnetic interactions from defect centers are observed, which are clearly distinguished from the broadening due to interactions with two-level systems and phonons. By minimizing the broadening due to the different defect centers, linewidths of the order of 4 kHz are achieved for all samples. The linewidths are limited by temperature-dependent interactions and by an interaction that is yet to be identified. Although the homogeneous linewidth can be narrowed further in these ceramic samples, the broadening is now comparable to the linewidths achieved in rare-earth-ion--doped single crystals. Thus, this work emphasizes the usefulness of studying ceramics to gain insights into dephasing mechanisms relevant to single crystals and suggests that ceramics may be an interesting alternative for applications in classical and quantum information processing.
Understanding decoherence in cryogenically cooled rare-earth-ion doped glass fibers is of fundamental interest and a prerequisite for applications of these material in quantum information applications. Here we study the coherence properties in a weakly doped erbium silica glass fiber motivated by our recent observation of efficient and long-lived Zeeman sublevel storage in this material and by its potential for applications at telecommunication wavelengths. We analyze photon echo decays as well as the potential mechanisms of spectral diffusion that can be caused by coupling with dynamic disorder modes that are characteristic for glassy hosts, and by the magnetic dipole-dipole interactions between Er3+{\mathrm{Er}}^{3+}Er3+ ions. We also investigate the effective linewidth as a function of magnetic field, temperature, and time, and then present a model that describes these experimental observations. We highlight that the operating conditions (0.6 K and 0.05 T) at which we previously observed efficient spectral hole burning coincide with those for narrow linewidths (1 MHz)---an important property for applications that has not been reported before for a rare-earth-ion doped glass.