Applied Physics Letters

Room-temperature electron spin dynamics of Ce3+ ions in a YAG crystal

P. Liang, Rongrong Hu, C. Chen, V. V. Belykh, Tianqing Jia, Z. R. Sun, Donghai Feng, Dmitri R. Yakovlev, M. Bayer

Published May 29, 2017• 16 citations

Abstract

Circularly polarized optical excitation generates electron spin polarization in the lowest 5d state of rare-earth Ce3+ ions in a YAG crystal. The 5d electron spin dynamics is investigated in transverse and longitudinal magnetic fields by time-resolved pump-probe Faraday rotation. Long lived electron spin coherence with a dephasing time of 2.5 ns is found at room temperature. In a transverse magnetic field of 1 T, the electron spin coherence shows a distinct beating-like amplitude modulation due to several slightly different Larmor frequencies corresponding to different electron g factors of magnetically inequivalent positions of the Ce3+ ions in the crystal lattice. Hyperfine coupling between the 5d electron of Ce3+ ions and environmental nuclear spins dominates the spin relaxation, which can be efficiently suppressed by a longitudinal magnetic field as small as 10 mT. The dependence of electron spin relaxation on both the transverse and longitudinal magnetic fields agrees well with the one predicted theoretically for the hyperfine coupling mechanism.

DOI: 10.1063/1.4984232

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Applied Physics Letters

Room-temperature electron spin dynamics of Ce3+ ions in a YAG crystal

P. Liang, Rongrong Hu, C. Chen, V. V. Belykh, Tianqing Jia, Z. R. Sun, Donghai Feng, Dmitri R. Yakovlev, M. Bayer

Published May 29, 2017• 16 citations

Publisher

Abstract

DOI: 10.1063/1.4984232

Related papers

Electron spin dynamics of Ce3+ ions in YAG crystals studied by pulse-EPR and pump-probe Faraday rotation

Д. В. Азамат, V. V. Belykh, Dmitri R. Yakovlev +6 more

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cond-mat.mtrl-sciCross-listedarXiv:2601.20768Jan 29, 2026

The spin relaxation dynamics of

{\mathrm{Ce}}^{3+}

ions in heavily cerium-doped YAG crystals is studied using pulse-electron paramagnetic resonance and time-resolved pump-probe Faraday rotation. Both techniques address the

4f

ground state, while pump-probe Faraday rotation also provides access to the excited

5d

state. We measure a millisecond spin-lattice relaxation time

{T}_{1}

, a microsecond spin coherence time

{T}_{2}

, and a $\ensuremath{\sim}10$ ns inhomogeneous spin dephasing time

{T}_{2}^{*}

for the

{\mathrm{Ce}}^{3+}

ground state at low temperatures. The spin-lattice relaxation of

{\mathrm{Ce}}^{3+}

ions is due to modified Raman processes involving the optical phonon mode at $\ensuremath{\sim}\phantom{\rule{0.16em}{0ex}}125\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. The relaxation at higher temperature goes through a first excited level of the

^{2}\mathrm{F}_{\frac{5}{2}}

term at about $\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\approx}228\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. Effects provided by the hyperfine interaction of the

{\mathrm{Ce}}^{3+}

with the

^{27}\mathrm{Al}

nuclei are observed.

{}^{3+}

:YAG and for spin transitions in Er

{}^{3+}

{}_{2}

SiO

{}_{5}

. The long coherence times that ZEFOZ can enable would make Pr

{}^{3+}

:YAG a strong candidate for achieving the strong-coupling regime of cavity QED, and would be an important step forward in creating long-lived telecommunications wavelength quantum memories in Er

{}^{3+}

{}_{2}

SiO

{}_{5}

. This work relies mostly on published spin-Hamiltonian parameters, but Raman heterodyne spectroscopy was performed on Pr

{}^{3+}

:YAG to measure the parameters for the excited state.

{}^{171}

Yb (spin-1/2) and

{}^{173}

Yb (spin-5/2) isotopes. The results demonstrate long coherence times for both the electron and nuclear spins (~1 ms). Employing a range of pulsed electron spin resonance measurements as well as comparison with relevant theory, the study elucidates a number of spin relaxation and decoherence mechanisms at work.

T_2

of the order of 1 ms, measured for a bulk FA

_{0.95}

_{0.05}

PbI

_3

lead halide perovskite crystal. Using periodic laser pulses, we synchronize the electron spin Larmor precession about an external magnetic field in an inhomogeneous ensemble, the effect known as spin mode locking. It appears as a decay of the optically created ensemble spin polarization within the dephasing time

T_2^*

of up to 20 ns and its revival during the spin coherence time

T_2

reaching the millisecond range. This exceptionally long spin coherence time in a bulk crystal is complemented by millisecond-long longitudinal spin relaxation times

T_1

for electrons and holes, measured by optically-detected magnetic resonance. These long-lasting spin dynamics highlight perovskites as promising platform for the quantum devices with all-optical control.