Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

AVS Quantum Science

Non-Markovian fluorescence dynamics in rare-earth systems

Humberto Triviño, F. Mesa

Published Apr 2, 2026• 0 citations
Publisher

Abstract

We investigate the fluorescence dynamics of the rare-earth ions europium, terbium, and gadolinium, with particular emphasis on quantifying non-Markovian behavior. By employing fluorescence as a probe, we characterize deviations from memoryless dynamics and identify clear distinctions between Markovian and non-Markovian regimes. Our analysis demonstrates how these profiles manifest in optical spectroscopy, providing direct insight into system–environment interactions. Beyond their fundamental implications, these insights may support the rational design of rare-earth-doped materials for applications in multicolor phosphors, hybrid optoelectronic architectures, and emerging quantum sensing technologies.

DOI
10.1116/5.0322941

Related papers

Spin dynamics in rare-earth-ion-doped crystals for optical quantum memories

Emmanuel Zambrini Cruzeiro

Spin dynamics are investigated in several rare-earth-ion-doped crystals, both for so-called Kramers ions and non-Kramers ions. I have studied two illustrative examples of such systems, Neodymium (Kramers) and Europium (non-Kramers). The main motivation behind these studies is the search for long relaxation and coherence times in solid state atomic ensembles. To this end I employ spectroscopic techniques to probe different kinds of interactions and relaxation mechanisms taking place in the samples. I perform spectroscopy of Neodymium (Kramers) in two different crystal lattices, yttrium orthosilicate and yttrium orthovanadate. I propose new methods to improve the relaxation lifetimes, and make precise characterizations of the interactions taking place within the atomic ensemble. In particular we achieve the most precise measurement of a kind of interaction which has received considerable attention recently in other areas of physics, the Dzyaloshinskii-Moriya interaction. These spectroscopic studies are of course of fundamental interest, but they can also be applied to quantum communication and computation. In this context, we were able to increase the efficiency of a quantum memory based on a Kramers ion (Nd) to be on par with the best non-Kramers (Eu,Pr) memories. Using Neodymium ions, I have certified that multi-dimensional entanglement can be stored in a quantum memory. The second part of this thesis concerns the study of Europium (non-Kramers), starting with a characterization of the Zeeman and quadrupole interactions. I believe these studies will pave the way for long duration (100 ms or more) quantum storage in a rare-earth-ion-doped crystal.

•Jan 1, 2017•0 citations

Decay times of radiative and non-radiative transitions in rare-earth ions

E. F. Kustov, Victor B. Loschenov, Irina Basieva

We present a theoretical method for evaluation of decay times of both radiative and non-radiative transitions in rare-earth ions in crystals and glasses. Relying on one experimentally known lifetime and known parameters of electrostatic and spin–orbit interaction, the fluorescence spectra can be modelled for various pumping wavelengths providing new insights into dynamical processes of fluorescence.

Physica Scripta•Dec 1, 2014•3 citations

Recent Progress on the Spectroscopy of Rare Earth Ions in Core–Shells, Nanowires, Nanotubes, and Other Novel Nanostructures

Xueyuan Chen, Liqin Liu, Guokui Liu

Research and development of nanoscale luminescent and laser materials are part of the rapidly advancing nanoscience and nanotechnology. Because of unique spectroscopic properties and luminescent dynamics of f-electron states, doping luminescent rare earth ions into nano-hosts has been demonstrated as an optimistic approach to developing highly efficient and stable nanophosphors for various applications. In this article, we review the most recent progress in spectroscopic measurements of rare earth ion-activated low-dimensional nanostructures including nanolayers, core-shells, nanowires, nanotubes, and nanodisks. Among a large volume of work reported in the literature on many members of the rare earth series including Ce3+, Pr3+, Nd3+, Eu3+, and Er3+, we focus on recent findings in the spectroscopic and luminescence properties of Eu3+ doped nanolayers, core-shells, and nanotubes, because Eu3+ ions have been extensively studied and widely used as an ideal probe for fundamental understanding of nano-phenomena. Specifically, the dependence of the optical properties of rare earth ions on nanostructures is discussed in detail.

Journal of Nanoscience and Nanotechnology•Mar 1, 2008•32 citations

Quantum Information, Laser Frequency Stabilization, and Optical Signal Processing with Rare-Earth Doped Materials

R. L. Cone, Charles W. Thiel, Yongchen Sun +2 more

Rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms. We design and characterize rare-earth-doped crystals for applications requiring long optical decoherence times (4.2 ms) and ultranarrow spectral holes (75 Hz).

Frontiers in Optics•Jan 1, 2013•2 citations

Spectroscopy of single rare earth solid-state qubits

Kangwei Xia

Light-matter interaction at single quantum object level is a long-lived challenge and dream of physicists. From the 1970s, the development of single ion spectroscopy and the observation of single photon states pave a way to a new era of detecting, and coherently manipulating quantum objects with electromagnetic field at single-ion levels. Later on, the invention of single molecular spectroscopy offers a new approach to investigate single quantum objects in condensed matter, where the sophisticated trapping systems like in ions and cold atoms are not needed, resulting in the discovery of various of single photon emitters embedded in solids. Among all, single quantum dots and single negatively charged nitrogen-vacancy centers in diamond attract most attentions, since their single spins can be coherently manipulated and entangled by the light field giving rise to numerous applications from nanoscale sensing to quantum computing. They are intensively studied as the most promising candidates for the realization of solid-state quantum bits. However, these systems coupled to a complex environment which can result in rapid loss of spin coherence or optical instability. Finding an alternative solid-state single system with remarkable optical and spin properties is the motivation of this dissertation. Rare earth ions doped in inorganic crystal hosts provide promises not only by the high quality factor 4f-4f optical transitions but also by the well preserved and long-lived spin states, with the applications from solid-state laser spectroscopy to quantum information processing. However, for almost three decades, not being able to identify single rare earth elements in solids is the obstacle to achieve their full potential functionality. We demonstrated the first direct optical detection of single rare earth ions (praseodymium) in solids in 2012. This research was covered in my Master Degree Thesis. This dissertation presents experimental progress in optically detecting other single rare earth species in crystals, understanding their fundamental spectroscopy properties and coherently controlling them, which is mainly focused on single trivalent cerium ions in different host materials. Following the optical detection of single cerium ions in yttrium aluminum garnet (YAG), the optical and spin properties of single Ce ions are investigated. Single Ce ions show good photostability under the pulsed laser excitation. Still, like in other solid emitters, photo-induced dynamics of single Ce ions is observed, however, in a counterintuitive way under the continuous laser irradiation. To understand this behavior, we proposed a charge dynamics model, and developed a novel method to suppress this undesired charge dynamics. With this approach, we obtain the photoluminescence excitation spectrum of single Ce ions in YAG under a CW laser excitation. Narrow (~80 MHz) and spectrally stable optical transitions between the lowest Kramers doublets of the ground and the excited states are observed. In comparison with the large inhomogeneous broadening (500 GHz), narrow resonant transitions provide the good selectivity in the spectral domain. Moreover, the single Ce ground spin state presents a spin 1/2 system with anisotropy g factor. It results in the optical selection rules dependent on the directions of the external magnetic field. Under parallel external magnetic field with respect to the quantization axis, only the spin-flip transitions are allowed with high transition contrast. It gives the opportunity to optically initialize the ground spin state of single Ce ions with 97.5% fidelity. The coherent spin properties of single Ce ions can be investigated, after the successful optical initialization. By scanning the microwave frequency, we obtain the electron spin resonance of single Ce spin transitions. We show the spin state has a coherence time of 290 ns, which is dominated by the surrounding aluminum nuclear spin bath and impurities induced electron spin bath. The coherence time can be extended to 2 ms through dynamical decoupling method, which approaches closely to the upper limit 4.5 ms due to spin-lattice relaxation. This result indicates single Ce electron spin can be a good solid-state qubit. With the combination of optical and spin manipulations of single Ce ions, a quantum interface between a single spin and a single photon is observed by monitoring the temporal behavior of circularly polarized emission photons from the ion. We obtain the Larmor precession of the excited spin state, indicating the direct mapping of the excited spin states of single Ce ions onto the polarization states of the fluorescence photons. Furthermore, with both optical and spin access, we all-optically demonstrate coherent population trapping of a single Ce spin qubit. To scale up the system for further applications, we present the nano-scale engineering of rare earth species in YAG crystal, with the acquirement of the production yield of Ce and Pr implantation (53 and 91% respectively). The optical and spin properties of single implanted Ce ions show fairly good performance, which paves the way towards coherent coupling of single rare earth qubits in a small volume. Besides the study of single Ce ions, the spectroscopy properties of single praseodymium ions in YAG crystal are investigated. We obtain the photoluminescence excitation spectrum and the hyperfine splitting of a single praseodymium ion. All-optical control of a single praseodymium ion is achieved. In this dissertation, we solve the key problem of optically detecting, spectrally studying and coherently manipulating single rare earth ions in solids. The developed methods including optical detection, initialization, readout, coherent control and nanoscale production of single rare earth elements in crystals offer novel and powerful tools for understanding and exploring the fundamental spectroscopy properties of single rare earth elements in solids. It paves a way towards constructing scalable quantum network based on single rare earth solid-state qubits.

•Jan 1, 2016•1 citation

PHOTONIC MATERIALS AND DEVICES Progress in relating rare-earth ion 4f and 5d energy levels to host bands in optical materials for hole burning, quantum information and phosphors

Charles W. Thiel, Yazhou Sun, R. L. Cone

Rare-earth ions play an important role in modern technology as optically active elements in solid-state luminescent materials. In many of these materials, interactions between the electronic band states of the host crystal and the rare-earth ion's localized 4f N and 4f N−1 5d states influence the material's optical properties. The importance of these interactions is discussed for material applications in photon-gated hole burning, quantum information and phosphors. Material dependent trends in the relative binding energies of the 4f N states and the host bands have been observed and are summarized. An empirical model for the ion dependence of the 4f electron binding energies is formulated in terms of atomic number and compared with previous models. These models are extended to describe the 4f N−1 5d states with one additional parameter. Improved estimates for the free-ion ionization potentials used in the model are also presented and discussed.

Journal of Modern Optics•Nov 1, 2002•67 citations
We investigate the fluorescence dynamics of the rare-earth ions europium, terbium, and gadolinium, with particular emphasis on quantifying non-Markovian behavior. By employing fluorescence as a probe, we characterize deviations from memoryless dynamics and identify clear distinctions between Markovian and non-Markovian regimes. Our analysis demonstrates how these profiles manifest in optical spectroscopy, providing direct insight into system–environment interactions. Beyond their fundamental implications, these insights may support the rational design of rare-earth-doped materials for applications in multicolor phosphors, hybrid optoelectronic architectures, and emerging quantum sensing technologies.
Spin dynamics are investigated in several rare-earth-ion-doped crystals, both for so-called Kramers ions and non-Kramers ions. I have studied two illustrative examples of such systems, Neodymium (Kramers) and Europium (non-Kramers). The main motivation behind these studies is the search for long relaxation and coherence times in solid state atomic ensembles. To this end I employ spectroscopic techniques to probe different kinds of interactions and relaxation mechanisms taking place in the samples. I perform spectroscopy of Neodymium (Kramers) in two different crystal lattices, yttrium orthosilicate and yttrium orthovanadate. I propose new methods to improve the relaxation lifetimes, and make precise characterizations of the interactions taking place within the atomic ensemble. In particular we achieve the most precise measurement of a kind of interaction which has received considerable attention recently in other areas of physics, the Dzyaloshinskii-Moriya interaction. These spectroscopic studies are of course of fundamental interest, but they can also be applied to quantum communication and computation. In this context, we were able to increase the efficiency of a quantum memory based on a Kramers ion (Nd) to be on par with the best non-Kramers (Eu,Pr) memories. Using Neodymium ions, I have certified that multi-dimensional entanglement can be stored in a quantum memory. The second part of this thesis concerns the study of Europium (non-Kramers), starting with a characterization of the Zeeman and quadrupole interactions. I believe these studies will pave the way for long duration (100 ms or more) quantum storage in a rare-earth-ion-doped crystal.
Research and development of nanoscale luminescent and laser materials are part of the rapidly advancing nanoscience and nanotechnology. Because of unique spectroscopic properties and luminescent dynamics of f-electron states, doping luminescent rare earth ions into nano-hosts has been demonstrated as an optimistic approach to developing highly efficient and stable nanophosphors for various applications. In this article, we review the most recent progress in spectroscopic measurements of rare earth ion-activated low-dimensional nanostructures including nanolayers, core-shells, nanowires, nanotubes, and nanodisks. Among a large volume of work reported in the literature on many members of the rare earth series including Ce3+, Pr3+, Nd3+, Eu3+, and Er3+, we focus on recent findings in the spectroscopic and luminescence properties of Eu3+ doped nanolayers, core-shells, and nanotubes, because Eu3+ ions have been extensively studied and widely used as an ideal probe for fundamental understanding of nano-phenomena. Specifically, the dependence of the optical properties of rare earth ions on nanostructures is discussed in detail.
Light-matter interaction at single quantum object level is a long-lived challenge and dream of physicists. From the 1970s, the development of single ion spectroscopy and the observation of single photon states pave a way to a new era of detecting, and coherently manipulating quantum objects with electromagnetic field at single-ion levels. Later on, the invention of single molecular spectroscopy offers a new approach to investigate single quantum objects in condensed matter, where the sophisticated trapping systems like in ions and cold atoms are not needed, resulting in the discovery of various of single photon emitters embedded in solids. Among all, single quantum dots and single negatively charged nitrogen-vacancy centers in diamond attract most attentions, since their single spins can be coherently manipulated and entangled by the light field giving rise to numerous applications from nanoscale sensing to quantum computing. They are intensively studied as the most promising candidates for the realization of solid-state quantum bits. However, these systems coupled to a complex environment which can result in rapid loss of spin coherence or optical instability. Finding an alternative solid-state single system with remarkable optical and spin properties is the motivation of this dissertation. Rare earth ions doped in inorganic crystal hosts provide promises not only by the high quality factor 4f-4f optical transitions but also by the well preserved and long-lived spin states, with the applications from solid-state laser spectroscopy to quantum information processing. However, for almost three decades, not being able to identify single rare earth elements in solids is the obstacle to achieve their full potential functionality. We demonstrated the first direct optical detection of single rare earth ions (praseodymium) in solids in 2012. This research was covered in my Master Degree Thesis. This dissertation presents experimental progress in optically detecting other single rare earth species in crystals, understanding their fundamental spectroscopy properties and coherently controlling them, which is mainly focused on single trivalent cerium ions in different host materials. Following the optical detection of single cerium ions in yttrium aluminum garnet (YAG), the optical and spin properties of single Ce ions are investigated. Single Ce ions show good photostability under the pulsed laser excitation. Still, like in other solid emitters, photo-induced dynamics of single Ce ions is observed, however, in a counterintuitive way under the continuous laser irradiation. To understand this behavior, we proposed a charge dynamics model, and developed a novel method to suppress this undesired charge dynamics. With this approach, we obtain the photoluminescence excitation spectrum of single Ce ions in YAG under a CW laser excitation. Narrow (~80 MHz) and spectrally stable optical transitions between the lowest Kramers doublets of the ground and the excited states are observed. In comparison with the large inhomogeneous broadening (500 GHz), narrow resonant transitions provide the good selectivity in the spectral domain. Moreover, the single Ce ground spin state presents a spin 1/2 system with anisotropy g factor. It results in the optical selection rules dependent on the directions of the external magnetic field. Under parallel external magnetic field with respect to the quantization axis, only the spin-flip transitions are allowed with high transition contrast. It gives the opportunity to optically initialize the ground spin state of single Ce ions with 97.5% fidelity. The coherent spin properties of single Ce ions can be investigated, after the successful optical initialization. By scanning the microwave frequency, we obtain the electron spin resonance of single Ce spin transitions. We show the spin state has a coherence time of 290 ns, which is dominated by the surrounding aluminum nuclear spin bath and impurities induced electron spin bath. The coherence time can be extended to 2 ms through dynamical decoupling method, which approaches closely to the upper limit 4.5 ms due to spin-lattice relaxation. This result indicates single Ce electron spin can be a good solid-state qubit. With the combination of optical and spin manipulations of single Ce ions, a quantum interface between a single spin and a single photon is observed by monitoring the temporal behavior of circularly polarized emission photons from the ion. We obtain the Larmor precession of the excited spin state, indicating the direct mapping of the excited spin states of single Ce ions onto the polarization states of the fluorescence photons. Furthermore, with both optical and spin access, we all-optically demonstrate coherent population trapping of a single Ce spin qubit. To scale up the system for further applications, we present the nano-scale engineering of rare earth species in YAG crystal, with the acquirement of the production yield of Ce and Pr implantation (53 and 91% respectively). The optical and spin properties of single implanted Ce ions show fairly good performance, which paves the way towards coherent coupling of single rare earth qubits in a small volume. Besides the study of single Ce ions, the spectroscopy properties of single praseodymium ions in YAG crystal are investigated. We obtain the photoluminescence excitation spectrum and the hyperfine splitting of a single praseodymium ion. All-optical control of a single praseodymium ion is achieved. In this dissertation, we solve the key problem of optically detecting, spectrally studying and coherently manipulating single rare earth ions in solids. The developed methods including optical detection, initialization, readout, coherent control and nanoscale production of single rare earth elements in crystals offer novel and powerful tools for understanding and exploring the fundamental spectroscopy properties of single rare earth elements in solids. It paves a way towards constructing scalable quantum network based on single rare earth solid-state qubits.
Rare-earth ions play an important role in modern technology as optically active elements in solid-state luminescent materials. In many of these materials, interactions between the electronic band states of the host crystal and the rare-earth ion's localized 4f N and 4f N−1 5d states influence the material's optical properties. The importance of these interactions is discussed for material applications in photon-gated hole burning, quantum information and phosphors. Material dependent trends in the relative binding energies of the 4f N states and the host bands have been observed and are summarized. An empirical model for the ion dependence of the 4f electron binding energies is formulated in terms of atomic number and compared with previous models. These models are extended to describe the 4f N−1 5d states with one additional parameter. Improved estimates for the free-ion ionization potentials used in the model are also presented and discussed.