The influence of the anisotropic Zeeman effect on optical decoherence was studied for the 1.54 μm telecom transition in Er3+:Y2SiO5 using photon echo spectroscopy as a function of applied magnetic field orientation and strength. The decoherence strongly correlates with the Zeeman energy splittings described by the ground- and excited-state g factor variations for all inequivalent Er3+ sites, with the observed decoherence times arising from the combined effects of the magnetic dipole-dipole coupling strength and the ground- and excited-state spin-flip rates, along with the natural lifetime of the upper level. The decoherence time was maximized along a preferred magnetic field orientation that minimized the effects of spectral diffusion and that enabled the measurement of an exceptionally narrow optical resonance in a solid—demonstrating a homogeneous linewidth as narrow as 73 Hz.
The influence of the anisotropic Zeeman effect on optical decoherence was studied for the 1.54 μm telecom transition in Er3+:Y2SiO5 using photon echo spectroscopy as a function of applied magnetic field orientation and strength. The decoherence strongly correlates with the Zeeman energy splittings described by the ground- and excited-state g factor variations for all inequivalent Er3+ sites, with the observed decoherence times arising from the combined effects of the magnetic dipole-dipole coupling strength and the ground- and excited-state spin-flip rates, along with the natural lifetime of the upper level. The decoherence time was maximized along a preferred magnetic field orientation that minimized the effects of spectral diffusion and that enabled the measurement of an exceptionally narrow optical resonance in a solid—demonstrating a homogeneous linewidth as narrow as 73 Hz.
Erbium-doped solids are a promising platform for quantum technology due to the Er3+ 1.5-\textmu{}m optical transition in the telecom C band that can offer long coherence times. To characterize the intrinsic C2 site of Er3+ in Y2O3 for quantum information and photonic signal-processing applications, absorption and site-selective fluorescence spectroscopy were used to assign the Er3+4I15/2$\ensuremath{\leftrightarrow}$4I13/2 transitions. The lowest-to-lowest transition occurs at 1535.608 nm and laser absorption determined an inhomogeneous linewidth of 780 MHz in a 0.005%-doped crystal at 3.4 K. Time-resolved fluorescence established an upper limit for the excited-state lifetime of 8.5 ms. Angular-dependent Zeeman absorption was used to determine ground- and excited-state g tensors. The C2-site g tensor components for the ground state are gx=1.60, gy=4.71, and gz=11.93 with a tipping angle of \ensuremath{\alpha} = $2.{06}^{\ensuremath{\circ}}$, whereas for the excited state the components are gx=1.08, gy=4.36, and gz=10.07 with a tipping angle of \ensuremath{\alpha} = $\ensuremath{-}11.{7}^{\ensuremath{\circ}}$. Optical decoherence can be suppressed by the application of a magnetic field parallel to $\ensuremath{\langle}111\ensuremath{\rangle}$ crystal axes where all C2 sites become nearly magnetically equivalent with large g values so that spin flips of neighboring Er3+ ions can be simultaneously suppressed. Using this magnetic field direction, two-pulse photon echoes gave a homogeneous linewidth of 5 kHz for an applied magnetic field of 0.5 T, narrowing and saturating at 2.5 kHz at 3.5 T. Decoherence over intermediate magnetic fields was described by spectral diffusion due to $\mathrm{E}{\mathrm{r}}^{3+}\text{\ensuremath{-}}\mathrm{E}{\mathrm{r}}^{3+}$ magnetic dipole interactions driven by the direct phonon process. With Er3+:Y2O3 absorption at a convenient telecom laser wavelength and the ability to fabricate waveguides, our study suggests that this is a promising material system for quantum information and spectral hole-burning signal-processing applications.
The mechanisms and effects of spectral diffusion for optical transitions of paramagnetic ions have been explored using the inhomogeneously broadened 1536 nm $^{4}\mathrm{I}_{15∕2}\ensuremath{\rightarrow}^{4}\mathrm{I}_{13∕2}$ transition in Er3+:Y2SiO5. Using photon echo spectroscopy, spectral diffusion was measured by observing the evolution of the effective coherence lifetimes over time scales from $1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ to 20 ms for magnetic-field strengths from 0.3 to 6.0 T, temperatures from 1.6 to 6.5 K, and nominal Er3+ concentrations of 0.0015%, 0.005%, and 0.02%. To understand the effect of spectral diffusion on material decoherence for different environmental conditions and material compositions, data and models were compared to identify spectral diffusion mechanisms and microscopic spin dynamics. Observations were successfully modeled by ${\mathrm{Er}}^{3+}\ensuremath{-}{\mathrm{Er}}^{3+}$ magnetic dipole interactions and Er3+ electron spin flips driven by the one-phonon direct process. At temperatures of 4.2 K and higher, spectral diffusion due to 89Y nuclear spin flips was also observed. The success in describing our extensive experimental results using simple models provides an important capability for exploring larger parameter spaces, accelerating the design and optimization of materials for spatial-spectral holography, and spectral hole-burning devices. The broad insight into spectral diffusion mechanisms and dynamics is applicable to other paramagnetic materials, such as those containing Yb3+ or Nd3+.
Erbium ions (Er3+) provide a telecom-band optical transition with strong magnetic-dipole character, making them attractive for quantum communication and spin-photon interfaces. Identifying host environments that combine low decoherence with photonic compatibility, however, remains a central challenge. Here we investigate Er3+ emission in tungsten disulfide (WS2) flakes, a layered host offering low nuclear-spin density and narrow telecom emission. Using time- and polarization-resolved photoluminescence under modest magnetic fields (< 0.2 T), we observe pronounced dimming, lifetime extension, and rotation of the emission dipole when the field has an out-of-plane component, whereas in-plane fields produce little change. Effective model calculations of Er3+ in monolayer WS2 parametrized from density functional theory indicate that these effects arise primarily from Zeeman-induced mixing of near-degenerate crystal-field sublevels, which modifies the magnitude and orientation of the optical transition dipole moments. Comparative measurements in flakes of different thickness and numerical estimates of the local density of optical states further suggest a secondary contribution from dipole coupling to the anisotropic photonic environment of thin WS2 layers. These findings identify layered WS2 as a platform where magnetic fields can tune telecom emission through an interplay of crystal-field physics and anisotropic photonic coupling.
When introduced as dopants into Y2O3, Er3+ ions replace Y3+ ions at two crystallographic sites of C2 and C3i point symmetries. The C3i site is particularly interesting, given that the inversion symmetry prohibits static electric-dipole moments and electric-dipole transitions, resulting in 1.5 \textmu{}m optical transitions characterized by purely magnetic-dipole properties. Employing $\mathrm{E}{\mathrm{r}}^{3+}\phantom{\rule{4pt}{0ex}}^{4}I_{15/2}\ensuremath{\leftrightarrow}^{4}I_{13/2}$ transitions, we examined the inherent C3i site of Er3+ in Y2O3 for its potential in quantum information science and spectral hole burning applications. Our approach involved absorption and site-selective fluorescence spectroscopy to discern Er3+ energy levels and revealed an excited-state lifetime of 14.6 ms. High-resolution laser spectroscopy at 3.7 K indicated an inhomogeneous linewidth of 1.3 GHz in our sample. Orientation-dependent Zeeman laser absorption spectroscopy facilitated the determination of the full g tensors for both the ground and excited states, confirming the C3i site assignment. Furthermore, it identified a suitable magnetic field direction for mitigating decoherence, a finding corroborated through two-pulse photon echo spectroscopy. Our study presents photon echo coherent transient measurements related to magnetic-dipole-allowed rare-earth ion transitions at the C3i site. The observed decoherence, attributed to spectral diffusion arising from $\mathrm{E}{\mathrm{r}}^{3+}\text{\ensuremath{-}}\mathrm{E}{\mathrm{r}}^{3+}$ magnetic-dipole interactions, underscores the complex spin dynamics at play in systems with multiple inequivalent dopant sites. Coupled with the practicality of telecom laser wavelengths, our investigation highlights the promise of magnetic-dipole transitions in advancing quantum information science and spectral hole burning applications.
Spatial-spectral holography using spectral hole burning materials is a powerful technique for performing real-time, wide-bandwidth information storage and signal processing. For operation in the important 1.5 μm communication band, the material Er3+:Y2SiO5 enables applications such as laser frequency stabilization, all-optical correlators, analog signal processing, and data storage. Site-selective absorption and emission spectroscopy identified spectral hole burning transitions and excited state T1 lifetimes in the 1.5 μm spectral region. The effects of crystal temperature, Er3+-dopant concentration, magnetic field strength, and crystal orientation on spectral diffusion were explored using stimulated photon echo spectroscopy, which is the "prototype" interaction mechanism for device applications. The performance of Er3+:Y2SiO5 and related Er3+ materials has been dramatically enhanced by reducing the effect of spectral diffusion on the coherence lifetime T2 through fundamental material design coupled with the application of an external magnetic field oriented along specific directions. A preferred magnetic field orientation that maximized T2 by minimizing the effects of spectral diffusion was determined using the results of angle-dependent Zeeman spectroscopy. The observed linewidth broadening due to spectral diffusion was successfully modeled by considering the effect of one-phonon (direct) processes on Er3+ - Er3+ interactions. The reported studies improved our understanding of Er3+ materials, explored the range of conditions and material parameters required to optimize performance for specific applications, and enabled measurement of the narrowest optical resonance ever observed in a solid-with a homogeneous linewidth of 73 Hz. With the optimized materials and operating conditions, photon echoes were observed up to temperatures of 5 K, enabling 0.5 GHz bandwidth optical signal processing at 4.2 K and providing the possibility for operation with a closed-cycle cryocooler.
We report detailed studies of the optical decoherence and spectroscopic properties of the 1536-nm optical transition of the bandwidth-engineered material 0.02Er:1Eu:Y2SiO5. This work is motivated by the need for comprehensive understanding of new resonant optical materials for spatial-spectral holography and quantum information applications. The dependence of optical decoherence on excitation frequency, applied magnetic field strength and orientation, crystal temperature, measurement time scale, and optical excitation density was studied using stimulated photon echo spectroscopy and time-resolved spectral hole-burning techniques. The effects of weak disorder generated by the introduction of Eu3+ ions into the lattice was probed by comparing measurements across the static disorder-induced distribution of transition frequencies as well as by comparing with measurements on 0.02Er:Y2SiO5. The results reveal that the coherence properties of Er:Y2SiO5 are preserved in the disordered system; moreover, the increased inhomogeneity produced by the disorder acts to suppress optical decoherence by inhibiting the electronic spin diffusion process, improving material properties for low magnetic field strengths and at increased temperatures desirable for practical applications.