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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Excited-state absorption measurements of Tm3+-doped crystals

Jakub W. Szela, Jacob I. Mackenzie

Published May 14, 2012• 3 citations
Publisher

Abstract

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.

DOI
10.1117/12.922673

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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.
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 possibility of using stimulated emission to improve the optical pumping of Tm3+ ions embedded in Tm3+:YAG to the 3F4 level is explored. The oscillator strengths and the frequencies of the transitions between the ground crystal field level of 3H4 to the different crystal field levels of 3F4 are measured at low temperature. Stimulated emission measurements at 1461 nm are performed to evaluate the optical pumping efficiency. Application to the spectral tailoring of Tm3+:YAG for quantum information applications is discussed.
New ways are proposed of increasing broadband-lamp pumping effectiveness of laser crystals with trivalent lanthanides. The method is based on the broadening of lasing-ion absorption spectrum by the remove (excitation) of their considerable part from the ground state into one (some) of the upper states with the help of additional resonant bleaching laser add-pumping Advantages of the new pumping schemes are illustrated by the results, obtained during quantitative analysis of the necessary conditions of stimulated-emission excitation for four laser crystals (LaF3, LiYF4, BaY2F8, and YA103) with Pr3+ ions, which can lase at 3Po → 3F4,3,2, 3H6,5 channels at 300 K with lamp pumping. The method proposed is also suitable for laser effectiveness increase in crystals with other lanthanides activators.
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.