The zero-phonon line (ZPL) between the two excited-state manifolds 3F4 and 3H4 of the trivalent thulium ion in yttrium aluminum perovskite (Tm3+:YAlO3) lies within the telecom E-band at around 1451 nm and exhibits an optical coherence time of a few μs at cryogenic temperatures. To improve this time in view of potential applications, e.g. single-photon sources and optical quantum memory, we characterized the magnetic properties of the lowest Stark levels of these two manifolds. Varying the external magnetic field amplitude and orientation, we measured the enhanced nuclear Zeeman splitting by probing the field-dependent frequency detuning of side holes created by means of spectral hole burning, and we characterized the inhomogeneous line shift caused by the quadratic Zeeman interaction. Together, this allowed us to establish the spin Hamiltonians for the lowest Stark level of the 3F4 and 3H4 manifolds, and to predict optical clock transitions for particular orientations and magnitudes of the magnetic field
The zero-phonon line (ZPL) between the two excited-state manifolds 3F4 and 3H4 of the trivalent thulium ion in yttrium aluminum perovskite (Tm3+:YAlO3) lies within the telecom E-band at around 1451 nm and exhibits an optical coherence time of a few μs at cryogenic temperatures. To improve this time in view of potential applications, e.g. single-photon sources and optical quantum memory, we characterized the magnetic properties of the lowest Stark levels of these two manifolds. Varying the external magnetic field amplitude and orientation, we measured the enhanced nuclear Zeeman splitting by probing the field-dependent frequency detuning of side holes created by means of spectral hole burning, and we characterized the inhomogeneous line shift caused by the quadratic Zeeman interaction. Together, this allowed us to establish the spin Hamiltonians for the lowest Stark level of the 3F4 and 3H4 manifolds, and to predict optical clock transitions for particular orientations and magnitudes of the magnetic field
Spectroscopy and Coherence of an Excited-State Transition in Tm3+:YAlO3 at Telecommunication Wavelength
We characterize spectroscopic and coherence properties of the 1451.37 nm excited-state zero-phonon line (ZPL) between the 3F4 and the 3H4 manifolds of a thulium-doped yttrium aluminum perovskite (Tm3+:YAlO3) crystal at temperatures around 1.5 K. We measure the absorption spectrum between the 3H6 - 3F4 and 3F4 - 3H4 manifolds, the inhomogeneous broadening of the 3F4 - 3H4 (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±0.07μs at B=2T and low ion concentration in the 3F4 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.
Rare-earth-doped crystals have been used for optical signal processing and storage applications. In this dissertation, their potential for quantum computing applications is explored. In one quantum computing scheme, information is stored in nuclear spin states and this information is then processed by using optical pulses through the coupling of these nuclear spin states to a common electronic level. To implement this scheme, nuclear spin states and coupling of these nuclear spin states to a common electronic level is required. Preliminary work in rare-earth materials like Pr3+ and Eu3+ has shown promising results regarding their suitability for quantum computing applications. One particular problem with these materials is that their transition wavelengths are only accessible with dye lasers. These lasers are inherently unstable, and currently few available systems exhibit the stability required for quantum computing applications. An alternative choice was to investigate other rare-earth ions like thulium. Thulium has a transition wavelength that can be accessed with diode lasers, which are commercially available, easy to stabilize, and compact. This dissertation is based on our investigations of Tm3+:YAG for quantum computing applications. Investigations involved a detailed characterization of the material. Nuclear spin states, in Tm3+:YAG, were obtained by applying an external magnetic field to the sample. First, interaction of an external magnetic field with the thulium ions at various sites in the crystal was analyzed. This analysis was used to measure the magnetic anisotropy in the material. These results show that it is possible, with the suitable choice of the magnetic orientation and the site in the crystal, to build a working 3-level quantum system. In the demonstration of single qubit operations in Tm3+:YAG, we first theoretically studied the effect of Gaussian spatial beam on the single qubit operations. Later on, we experimentally prepared a single isolated ensemble of ions in the inhomogeneously broadened absorption profile of the medium. This single isolated ensemble of ions was used as a test-bed to implement the single qubit operations. We also isolated two ensembles of ions in the inhomogeneous absorption profile of the medium. The interaction between these two isolated ensembles of ions was also studied.
High resolution, absolute excited-state absorption (ESA) spectra, at room temperature, from the long-lived 3F4 energy level of several crystals doped with trivalent thulium (Tm3+) ions have been measured employing high-brightness narrowband (FWHM <30 nm) light emitting diodes (LEDs) as a probe wavelength. The aim of this investigation was to determine the strength of ESA channels at wavelengths addressable by commercially available semiconductor laser diodes operating around 630-680 nm. The favourable lifetime of the 3F4 manifold and negligible ground-state absorption (GSA) for the red-wavelength second-step excitation, ensures a direct and efficient route for a dual-wavelength pumping scheme of the thulium ion, which will enable blue-green laser emission from its 1G4 upper-laser level.
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.
Photon-echo measurements are reported for the trivalent thulium ion, which differs from all other rare-earth ions in having a single isotope of nuclear spin 1/2. Echo decays on the 3H6(1) ↔ 3H4(1) transition of LaF3:Tm3+ and YAG:Tm3+ were magnetic-field dependent at 1.5 K, showing that the dephasing originates from spin fluctuations of nuclei in the host crystals. Coherence times in the range of 7 to 100 μs were measured, corresponding to homogeneous linewidths of tens of kilohertz. The echo decays were nonexponential, providing evidence for spectral diffusion that is due to a distribution of 19F and 27A1 nuclear spin-flip times in the respective hosts.
The $^{2}F_{7/2}\ensuremath{\leftrightarrow}^{2}F_{5/2}$ optical transitions of Yb3+ doped into Y3Al5O12 (YAG) were studied for potential quantum information and photonic signal processing applications. Absorption and fluorescence spectroscopy located the energy levels of the ground 2F7/2 and excited 2F5/2 manifolds, allowing inconsistencies between previous assignments of crystal field splittings in the literature to be resolved. These measurements reveal an unusually large splitting between the first and second levels in both the ground and excited multiplets, potentially providing for reduced sensitivity to thermally induced decoherence and spin-lattice relaxation. Spectral hole burning through two-level saturation was observed, determining the excited state lifetime to be 860 \ensuremath{\mu}s and resolving ambiguities in previous fluorescence measurements that were caused by the large radiation trapping effects in this material. Optical decoherence measurements using two-pulse photon echoes gave a homogeneous linewidth of 18 kHz for an applied magnetic field of 1 T, narrowing to 5 kHz at 2.5 T. The observed decoherence was described by spectral diffusion attributed to $\mathrm{Y}{\mathrm{b}}^{3+}\mathrm{\ensuremath{-}}\mathrm{Y}{\mathrm{b}}^{3+}$ magnetic dipole interactions. Laser absorption determined an inhomogeneous linewidth of 3.6 GHz for this transition in this 0.05%-doped crystal, which is narrower than for any other rare-earth-ion transition previously studied in the YAG host. The temperature dependence of the transition energy and linewidth of the lowest 2F7/2 to lowest 2F5/2 transition centered at 968.571 nm measured from 4 K to 300 K was well described by phonon scattering at higher temperatures, with an additional anomalous linear temperature-dependent broadening at temperatures below 80 K. Two magnetically inequivalent subgroups of Yb3+ ions were identified when a magnetic field was applied along the $\ensuremath{\langle}111\ensuremath{\rangle}$ axis, as expected for the D2 sites in the cubic symmetry crystal, with ground and excited state effective g-values of gg=3.40 (3.34) and ge=1.04 (2.01), respectively. Together with the convenient diode laser wavelength of this transition, our study suggests that Yb3+:YAG is a promising material system for spectral hole burning and quantum information applications.