Spectroscopy and Coherence of an Excited-State Transition in Tm$^{3+}$:YAlO$_3$ at Telecommunication Wavelength

TL;DR

This study characterizes the spectroscopic and coherence properties of an excited-state transition in Tm$^{3+}$:YAlO$_3$ at cryogenic temperatures, revealing potential for quantum technology applications.

Contribution

First demonstration of coherence in an excited-state transition in a rare-earth crystal, with detailed spectroscopic and coherence measurements at telecommunication wavelengths.

Findings

Measured maximum optical coherence time of 4.75 microseconds at 2 Tesla.

Characterized inhomogeneous broadening and hyperfine interactions in Tm$^{3+}$:YAlO$_3$.

Demonstrated potential for quantum technology using excited-state transitions.

Abstract

We characterize spectroscopic and coherence properties of the 1451.37 nm excited-state zero-phonon line (ZPL) between the $^{3}F_{4}$ and the $^{3}H_{4}$ manifolds of a thulium-doped yttrium aluminum perovskite (Tm$^{3+}$:YAlO$_3$) crystal at temperatures around 1.5 K. We measure the absorption spectrum between the $^{3}H_{6}$ - $^{3}F_{4}$ and $^{3}F_{4}$ - $^{3}H_{4}$ manifolds, the inhomogeneous broadening of the $^{3}F_{4}$ - $^{3}H_{4}$ (excited-state) ZPL, and the lifetimes of the higher-lying and lower-lying excited states. We also investigate level shifts caused by the quadratic Zeeman interaction as well as spectral hole-burning spectra with varying magnetic fields, providing insights into hyperfine interactions. Using again spectral holes but also optical free induction decays (FIDs), we assess optical coherence times, finding a maximum of $4.75 \pm 0.07~\mu s$ at B=2T and low ion concentration in the $^{3}F_{4}$ level. Our results -- the first to demonstrate coherence of an excited-state transition in a rare-earth crystal -- suggest the possibility of exploiting such transitions for quantum technology.