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arXiv:2507.15051

Polarisation and Temperature Dependence of Er$^{3+}$:CaWO$_4$ -- Towards a Solid-State Rare-Earth Ion-Doped Quantum Memory

Mikhael Sayat, Lee, Trevor R., Suchit Negi, Naoya Iwahara, In Cheol Seo, Yung Chuen Tan, Ping Koy Lam, Young‐Wook Cho, Jian-Rui Soh

Published Jul 20, 2025• 0 citations
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Abstract

In the endeavour of developing quantum memories, Er$^{3+}$:CaWO$_4$ has emerged as a promising rare-earth ion-doped (REID) crystal platform due to its long optical coherence times and compatibility with the 1550 nm telecommunications band. This work investigates the effects of polarisation and temperature on the absorption strength, central wavelength, and linewidth of the $Z_1\to Y_1$ and $Z_1\to Y_2$ optical transitions, with light incident along the crystal $a$ and $c$ axes. It is found that the $Z_1\to Y_1$ transition at 1532.6 nm with the incident laser along the $c$-axis at cryogenic temperatures ($\sim$3 K) is particularly favourable. The transition exhibits a stable central wavelength, narrower linewidth, polarisation independence, larger absorption cross-section, and lies within the C-band -- attributes that make it highly suitable for quantum memory applications.

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Polarisation and temperature dependence of Er 3+ :CaWO 4 —towards a solid-state rare-earth ion-doped quantum memory

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Abstract In the development of high-performance optical quantum memories, Er 3+ :CaWO 4 has emerged as a compelling rare-earth ion-doped solid-state platform owing to its long optical coherence times and compatibility with the 1550nm telecommunications band. In this work, we systematically investigate how optical polarisation and temperature influence the absorption strength, central wavelength, and linewidth of the Z 1 → Y 1 and Z 1 → Y 2 transitions, with light incident along the crystal a and c axes. We identify the Z 1 → Y 1 transition at 1532.6 nm with the incident laser propagating along the c -axis at cryogenic temperatures (∼3 K) as particularly advantageous for memory operation. Under these conditions, the transition exhibits a stable central wavelength, narrower linewidth, polarisation-independent absorption, and an enhanced absorption cross-section, while residing within the telecommunication C-band. These combined attributes position the Z 1 → Y 1 line as a robust and suitable point for Er 3+ :CaWO 4 based quantum memories.

Physica Scripta•Jan 27, 2026•1 citation

A solid-state source for non-classical photon pairs with controllable delay

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Quantum memories for light are important resources as quantum interfaces between light and matter in future quantum information networks. In particular, solid state optical memories based on rare earth ion doped (REID) crystals are of great interest due to their unique physical properties. They provide large number of atoms naturally trapped in a solid with narrow optical and spin transitions. They indeed have excellent optical and spin state coherence times at cryogenic temperatures. Among the various rare-earth doped materials, Pr3+ :Y 2 SiO 5 crystals have shown excellent properties for light storage and exhibit a level scheme suitable for long lived storage in spin states.

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Isotopically enriched epitaxial CaWO$_{4}$ thin films for Er$^{3+}$ spin-photon quantum interfaces

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Rare earth ion (REI)-doped oxide thin films are attractive for the application of quantum interconnects due to their stable optical levels and scalability$^{1-3}$. Among them, Er$^{3+}$ doped CaWO$_{4}$ is promising because it possesses narrow optical linewidth transitions and a long spin coherence time$^{4-6}$. The electron spin coherence is limited at high temperatures by paramagnetic impurities and by the presence of the 14.3% $^{183}$W nuclear spin. To further increase the spin coherence time at millikelvin temperatures, where the paramagnetic impurities are frozen out, our approach is to synthesize chemically and isotopically purified thin films as a host material. We first grow non-isotopically enriched Er$^{3+}$ doped CaWO$_{4}$ thin films, which exhibit a 214(13) MHz photoluminescence (PL) inhomogeneous linewidth, indicating the thin film has high crystalline quality. We then grow isotopically enriched CaWO$_{4}$ thin films using an isotopically purified $^{186}$WO$_{3}$ source. Time of flight secondary ion mass spectrometry (ToF-SIMS) was used to measure the relative concentration of W isotopes. $^{183}$W, the only W isotope that has a net nuclear spin and is the major cause of spin decoherence, was at a relative abundance of 1.2%, a factor of 10 lower than natural abundance. We also observed PL emission from single ions after integrating nano-photonic devices with the thin film. These results establish isotopically engineered CaWO$_{4}$ thin films as a promising platform for future studies of nuclear-spin-limited coherence and for scalable rare-earth-ion-based quantum nanophotonic devices.

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Optical and microstructural characterization of Er3+ doped epitaxial cerium oxide on silicon

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Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies, such as quantum memories, due to the intrinsic spin–photon interface of the rare-earth ion combined with the integration methods available in the solid state. Erbium-doped cerium oxide (Er:CeO2) is a particularly promising host material platform for such a quantum memory, as it combines the telecom-wavelength (∼1.5μm) 4f–4f transition of erbium, a predicted long electron spin coherence time when embedded in CeO2, and a small lattice mismatch with silicon. In this work, we report on the epitaxial growth of Er:CeO2 thin films on silicon using molecular beam epitaxy, with controlled erbium concentration between 2 and 130 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO2 host structure and characterize the spin and optical properties of the embedded Er3+ ions as a function of doping density. In as-grown Er:CeO2 in the 2–3 ppm regime, we identify an EPR linewidth of 245(1) MHz, an optical inhomogeneous linewidth of 9.5(2) GHz, an optical excited state lifetime of 3.5(1) ms, and a spectral diffusion-limited homogeneous linewidth as narrow as 4.8(3) MHz. We test the annealing of Er:CeO2 films up to 900 °C, which yields narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%.

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Quantum memory development and new slow light applications in rare-earth-ion-doped crystals

Qian Li

When doped into solid state transparent crystals, rare-earth ions can have optically excited states with milliseconds coherence time and up to six hours coherence time for hyperfine levels after being cooled down to liquid helium temperature. This long coherence property makes them unique as solid state material and attractive for quantum information applications.The rare-earth ions have narrow homogeneous linewidths on the order of ~ kHz. When doped into a crystal, the lattice structure is slightly distorted due to the size mismatch between the dopant and the host ions, resulting in slight differences in the local crystal fields at the dopant sites. Therefore, the resonance frequencies of the rare-earth ions are shifted relatively, resulting in an inhomogeneously broadened absorption profile, typically on the order of a few GHz. This provides the possibility of addressing each group of ions individually and engineering the absorption profile for different purposes by optical pumping using a narrow linewidth laser, and makes rare-earth-ion-doped crystals suitable for ensemble based quantum memories.Quantum memories are vital components for developing longdistance quantum communication. Part of this thesis project focused on making quantum memories with high efficiency and long storage time, especially using materials with low optical depth. To achieve this goal, a low finesse, unsymmetrical cavity was employed and experiments were carried out at (or close to) the impedance matched condition. Atomic frequency comb (AFC) protocol proposed for such an inhomogeneously broadened system was used to store coherent light for a certain time. 56% overall efficiency was achieved, and the main limiting factor for reaching even higher efficiency was the inefficient coupling between incoming light and the cavity mode. Other possible loss mechanisms were analyzed as well.Long-time, on-demand, quantum memory experiments were conducted with the help of two efficient radio-frequency rephasing pulses. Storage time was extended from microseconds to milliseconds after compensating (most of) the residual earth magnetic field in the lab. The opportunities and challenges of combing the cavity assistant quantum memory and the long time, on demand quantum memory were analyzed and possible solutions were proposed. Another part of the thesis project involves slow light-based applications in rare-earth-ion-doped crystals. The strong slow light effect at the presence a spectral hole is due to the fact that the light interacts with the absorbing ions outside the spectral hole off-resonantly, and most of the light energy is stored inside the ions as a polarization. For example, with a group velocity of 300 km/s, 99.9% of the pulse energy is stored in the ions when the pulse propagates inside the crystal. The slower the light propagates, the more energy is stored inside the medium. Based on this, a frequency shifter that is capable of shifting the light frequency of ± 4 MHz was demonstrated, and frequency shift up to GHz was proposed. Group velocity control by a factor of 20 and pulse compression in time by a factor of 2 were also demonstrated. The frequency shift and group velocity of the light are solely controlled by the external electric field, which makes them ideal for weak light situation. The unique property of such a frequency shifter and group velocity controller is that they could be made to accept light from an arbitrary incoming angle and polarization, for example, scattered light.

•Jan 1, 2018•0 citations

Optical coherence properties of Kramers' rare-earth ions at the nanoscale for quantum applications

Mohammed K. Alqedra, Chetan Deshmukh, Shuping Liu +12 more

Rare Earth (RE) ion doped nanomaterials are promising candidates for a range of quantum technology applications. Among RE ions, the so-called Kramers' ions possess spin transitions in the GHz range at low magnetic fields, which allows for high-bandwidth multimode quantum storage, fast qubit operations as well as interfacing with superconducting circuits. They also present relevant optical transitions in the infrared. In particular, ${\mathrm{Er}}^{3+}$ has an optical transition in the telecom band, while ${\mathrm{Nd}}^{3+}$ presents a high-emission-rate transition close to 890 nm. In this paper, we measure spectroscopic properties that are of relevance to using these materials in quantum technology applications. We find the inhomogeneous linewidth to be 10.7 GHz for ${\mathrm{Er}}^{3+}$ and 8.2 GHz for ${\mathrm{Nd}}^{3+}$, and the excited state lifetime ${T}_{1}$ to be 13.68 ms for ${\mathrm{Er}}^{3+}$ and $540\phantom{\rule{0.16em}{0ex}}\textmu{}\mathrm{s}$ for ${\mathrm{Nd}}^{3+}$. We study the dependence of homogeneous linewidth on temperature for both samples, with the narrowest linewidth being 379 kHz (${T}_{2}=839$ ns) for ${\mathrm{Er}}^{3+}$ measured at 3 K, and 62 kHz (${T}_{2}=5.14\phantom{\rule{4pt}{0ex}}\textmu{}\mathrm{s}$) for ${\mathrm{Nd}}^{3+}$ measured at 1.6 K. Further, we investigate time-dependent homogeneous linewidth broadening due to spectral diffusion and the dependence of the homogeneous linewidth on magnetic field to get additional clarity of mechanisms that can influence the coherence time. In light of our results, we discuss two applications: single qubit-state readout and a Fourier-limited single photon source.

arXiv:2303.02054•Physical review. B./Physical review. B•Aug 3, 2023•20 citations
Polarisation and Temperature Dependence of Er3+^{3+}3+:CaWO4_44​ -- Towards a Solid-State Rare-Earth Ion-Doped Quantum Memory
In the endeavour of developing quantum memories, Er3+^{3+}3+:CaWO4_44​ has emerged as a promising rare-earth ion-doped (REID) crystal platform due to its long optical coherence times and compatibility with the 1550 nm telecommunications band. This work investigates the effects of polarisation and temperature on the absorption strength, central wavelength, and linewidth of the Z1→Y1Z_1\to Y_1Z1​→Y1​ and Z1→Y2Z_1\to Y_2Z1​→Y2​ optical transitions, with light incident along the crystal aaa and ccc axes. It is found that the Z1→Y1Z_1\to Y_1Z1​→Y1​ transition at 1532.6 nm with the incident laser along the ccc-axis at cryogenic temperatures (∼\sim∼3 K) is particularly favourable. The transition exhibits a stable central wavelength, narrower linewidth, polarisation independence, larger absorption cross-section, and lies within the C-band -- attributes that make it highly suitable for quantum memory applications.
Abstract In the development of high-performance optical quantum memories, Er 3+ :CaWO 4 has emerged as a compelling rare-earth ion-doped solid-state platform owing to its long optical coherence times and compatibility with the 1550nm telecommunications band. In this work, we systematically investigate how optical polarisation and temperature influence the absorption strength, central wavelength, and linewidth of the Z 1 → Y 1 and Z 1 → Y 2 transitions, with light incident along the crystal a and c axes. We identify the Z 1 → Y 1 transition at 1532.6 nm with the incident laser propagating along the c -axis at cryogenic temperatures (∼3 K) as particularly advantageous for memory operation. Under these conditions, the transition exhibits a stable central wavelength, narrower linewidth, polarisation-independent absorption, and an enhanced absorption cross-section, while residing within the telecommunication C-band. These combined attributes position the Z 1 → Y 1 line as a robust and suitable point for Er 3+ :CaWO 4 based quantum memories.
Quantum memories for light are important resources as quantum interfaces between light and matter in future quantum information networks. In particular, solid state optical memories based on rare earth ion doped (REID) crystals are of great interest due to their unique physical properties. They provide large number of atoms naturally trapped in a solid with narrow optical and spin transitions. They indeed have excellent optical and spin state coherence times at cryogenic temperatures. Among the various rare-earth doped materials, Pr3+ :Y 2 SiO 5 crystals have shown excellent properties for light storage and exhibit a level scheme suitable for long lived storage in spin states.
Isotopically enriched epitaxial CaWO4_{4}4​ thin films for Er3+^{3+}3+ spin-photon quantum interfaces
Rare earth ion (REI)-doped oxide thin films are attractive for the application of quantum interconnects due to their stable optical levels and scalability1−3^{1-3}1−3. Among them, Er3+^{3+}3+ doped CaWO4_{4}4​ is promising because it possesses narrow optical linewidth transitions and a long spin coherence time4−6^{4-6}4−6. The electron spin coherence is limited at high temperatures by paramagnetic impurities and by the presence of the 14.3% 183^{183}183W nuclear spin. To further increase the spin coherence time at millikelvin temperatures, where the paramagnetic impurities are frozen out, our approach is to synthesize chemically and isotopically purified thin films as a host material. We first grow non-isotopically enriched Er3+^{3+}3+ doped CaWO4_{4}4​ thin films, which exhibit a 214(13) MHz photoluminescence (PL) inhomogeneous linewidth, indicating the thin film has high crystalline quality. We then grow isotopically enriched CaWO4_{4}4​ thin films using an isotopically purified 186^{186}186WO3_{3}3​ source. Time of flight secondary ion mass spectrometry (ToF-SIMS) was used to measure the relative concentration of W isotopes. 183^{183}183W, the only W isotope that has a net nuclear spin and is the major cause of spin decoherence, was at a relative abundance of 1.2%, a factor of 10 lower than natural abundance. We also observed PL emission from single ions after integrating nano-photonic devices with the thin film. These results establish isotopically engineered CaWO4_{4}4​ thin films as a promising platform for future studies of nuclear-spin-limited coherence and for scalable rare-earth-ion-based quantum nanophotonic devices.
Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies, such as quantum memories, due to the intrinsic spin–photon interface of the rare-earth ion combined with the integration methods available in the solid state. Erbium-doped cerium oxide (Er:CeO2) is a particularly promising host material platform for such a quantum memory, as it combines the telecom-wavelength (∼1.5μm) 4f–4f transition of erbium, a predicted long electron spin coherence time when embedded in CeO2, and a small lattice mismatch with silicon. In this work, we report on the epitaxial growth of Er:CeO2 thin films on silicon using molecular beam epitaxy, with controlled erbium concentration between 2 and 130 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO2 host structure and characterize the spin and optical properties of the embedded Er3+ ions as a function of doping density. In as-grown Er:CeO2 in the 2–3 ppm regime, we identify an EPR linewidth of 245(1) MHz, an optical inhomogeneous linewidth of 9.5(2) GHz, an optical excited state lifetime of 3.5(1) ms, and a spectral diffusion-limited homogeneous linewidth as narrow as 4.8(3) MHz. We test the annealing of Er:CeO2 films up to 900 °C, which yields narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%.
When doped into solid state transparent crystals, rare-earth ions can have optically excited states with milliseconds coherence time and up to six hours coherence time for hyperfine levels after being cooled down to liquid helium temperature. This long coherence property makes them unique as solid state material and attractive for quantum information applications.The rare-earth ions have narrow homogeneous linewidths on the order of ~ kHz. When doped into a crystal, the lattice structure is slightly distorted due to the size mismatch between the dopant and the host ions, resulting in slight differences in the local crystal fields at the dopant sites. Therefore, the resonance frequencies of the rare-earth ions are shifted relatively, resulting in an inhomogeneously broadened absorption profile, typically on the order of a few GHz. This provides the possibility of addressing each group of ions individually and engineering the absorption profile for different purposes by optical pumping using a narrow linewidth laser, and makes rare-earth-ion-doped crystals suitable for ensemble based quantum memories.Quantum memories are vital components for developing longdistance quantum communication. Part of this thesis project focused on making quantum memories with high efficiency and long storage time, especially using materials with low optical depth. To achieve this goal, a low finesse, unsymmetrical cavity was employed and experiments were carried out at (or close to) the impedance matched condition. Atomic frequency comb (AFC) protocol proposed for such an inhomogeneously broadened system was used to store coherent light for a certain time. 56% overall efficiency was achieved, and the main limiting factor for reaching even higher efficiency was the inefficient coupling between incoming light and the cavity mode. Other possible loss mechanisms were analyzed as well.Long-time, on-demand, quantum memory experiments were conducted with the help of two efficient radio-frequency rephasing pulses. Storage time was extended from microseconds to milliseconds after compensating (most of) the residual earth magnetic field in the lab. The opportunities and challenges of combing the cavity assistant quantum memory and the long time, on demand quantum memory were analyzed and possible solutions were proposed. Another part of the thesis project involves slow light-based applications in rare-earth-ion-doped crystals. The strong slow light effect at the presence a spectral hole is due to the fact that the light interacts with the absorbing ions outside the spectral hole off-resonantly, and most of the light energy is stored inside the ions as a polarization. For example, with a group velocity of 300 km/s, 99.9% of the pulse energy is stored in the ions when the pulse propagates inside the crystal. The slower the light propagates, the more energy is stored inside the medium. Based on this, a frequency shifter that is capable of shifting the light frequency of ± 4 MHz was demonstrated, and frequency shift up to GHz was proposed. Group velocity control by a factor of 20 and pulse compression in time by a factor of 2 were also demonstrated. The frequency shift and group velocity of the light are solely controlled by the external electric field, which makes them ideal for weak light situation. The unique property of such a frequency shifter and group velocity controller is that they could be made to accept light from an arbitrary incoming angle and polarization, for example, scattered light.
Rare Earth (RE) ion doped nanomaterials are promising candidates for a range of quantum technology applications. Among RE ions, the so-called Kramers' ions possess spin transitions in the GHz range at low magnetic fields, which allows for high-bandwidth multimode quantum storage, fast qubit operations as well as interfacing with superconducting circuits. They also present relevant optical transitions in the infrared. In particular, Er3+{\mathrm{Er}}^{3+}Er3+ has an optical transition in the telecom band, while Nd3+{\mathrm{Nd}}^{3+}Nd3+ presents a high-emission-rate transition close to 890 nm. In this paper, we measure spectroscopic properties that are of relevance to using these materials in quantum technology applications. We find the inhomogeneous linewidth to be 10.7 GHz for Er3+{\mathrm{Er}}^{3+}Er3+ and 8.2 GHz for Nd3+{\mathrm{Nd}}^{3+}Nd3+, and the excited state lifetime T1{T}_{1}T1​ to be 13.68 ms for Er3+{\mathrm{Er}}^{3+}Er3+ and $540\phantom{\rule{0.16em}{0ex}}\textmu{}\mathrm{s}$ for Nd3+{\mathrm{Nd}}^{3+}Nd3+. We study the dependence of homogeneous linewidth on temperature for both samples, with the narrowest linewidth being 379 kHz (T2=839{T}_{2}=839T2​=839 ns) for Er3+{\mathrm{Er}}^{3+}Er3+ measured at 3 K, and 62 kHz (${T}_{2}=5.14\phantom{\rule{4pt}{0ex}}\textmu{}\mathrm{s}$) for Nd3+{\mathrm{Nd}}^{3+}Nd3+ measured at 1.6 K. Further, we investigate time-dependent homogeneous linewidth broadening due to spectral diffusion and the dependence of the homogeneous linewidth on magnetic field to get additional clarity of mechanisms that can influence the coherence time. In light of our results, we discuss two applications: single qubit-state readout and a Fourier-limited single photon source.