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Optical Materials

Anti-Stokes fluorescence of Cr3+ ions doped crystals excited in one-phonon vibronic sidebands

S.P. Feofilov, A.B. Kulinkin

Published May 30, 2019• 8 citations
Publisher
DOI
10.1016/j.optmat.2019.05.044

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A vibronic model of laser cooling for crystals doped with Yb3+ ions is proposed. The model involves the stimulated Raman adiabatic passage pumping through dipole-allowed 4f–5d transitions, electron transitions between Stark-split sublevels due to vibronic interaction, and anti-Stokes fluorescence from the excited ion state. Dynamics of the cooling process are described by the density matrix formalism. It is shown that the cooling power in the case of vibronic interaction is higher at least by a factor of 3.4 compared to the case of electron–phonon interaction. In the proposed model, an increase in the cooling power yields deeper and faster refrigeration of a crystal doped with Yb3+ ions. Estimations show that, on cooling by the stimulated Raman adiabatic passage pumping, the temperature of a crystal with an irradiated volume of 2.12×10−4 cm3 can reach 64 K in a time of 2 s. In the proposed model, the cooling temperature is 30 K lower and the cooling process is 100 times faster compared to the traditional model of direct pumping. The estimates are applicable to present-day materials of technologically attainable purity.

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Chapter 8 Bulk Cooling Efficiency Measurements of Yb-Doped Fluoride Single Crystals and Energy Transfer–Assisted Anti-Stokes Cooling in Co-Doped Fluorides

Azzurra Volpi, Alberto Di Lieto, M. Tonelli

To overcome the ETU-induced heating and realize efficient and enhanced laser cooling in Ho3+-doped solids, in Section 4.3, we will provide a modified excitation scheme based on ground-state absorption (GSA) of 5I8 Æ 5I7 at around 2.07 μm and ESA of 5I5 Æ 5F5 at around 2.28 μm. Compared with the conventional pumping scheme, the co-pumping scheme ameliorates the cooling performance significantly through alleviating the upconversion-quenching-induced heat [12], that is, the heat-producing 5I5 Ho3+ions are pumped to the 5F5 state by the laser at 2.28 μm. Fortunately, the 5F5 Ho3+ ions barely transit to the lower nearby state and tend to decay radiatively. Therefore, major heat produced in the conventional laser cooling of Ho3+-doped solids is avoided, and both cooling efficiency and cooling power density can be improved. In Section 4.4, we broaden the research domain of optical refrigeration to rare earth ion co-doped systems. Specifically, when Ho3+–Tm3+ co-doped YLiF4 crystals are pumped at around 2.07 μm, Ho3+ ions will populate at the 5I7 manifold. Meanwhile, Tm3+ ions will also be sensitized by absorbing energy transferred from 5I7 Ho3+ ions. Since the average energy of fluorescence photons generated by Tm3+3F4 Æ 3H6 radiative transitions is higher than that generated by Ho3+5I7 Æ 5I8 radiative transitions, energy transfer (ET) from Ho3+ to Tm3+ ions will induce annihilation of host phonons, and bring enhancement in both the cooling efficiency and the cooling power. Therefore, this cooling mechanism is referred next as energy transfer-enhanced laser cooling (ETLC) of solids [11]. 4.2 Conventional Laser Cooling of Holmium- The main upconversion process and the anti-Stokes fluorescence cooling (ASFC) processes of Ho3+-doped fluoride crystals are illustrated in Fig. 4.1. The ground-state (5I8) Ho3+ ions are pumped to the first excited state (5I7) with laser excitations of energy hν (solid red arrow on the left) and then relax thermally among the Stark levels in a timescale of picoseconds with host phonon absorption. Part of the Ho3+5I7 ions de-excite by emitting fluorescence photons of mean energy hν10 (solid blue arrow, ν10 > ν), which accounts for the ASFC process. The rest of the 5I7 Ho3+ ions de-excited and transfer their energy to the neighboring 5I7 Ho3+ ions, causing population accumulation at the third excited state (5I5) with host phonon absorption (solid green arrows). Comparison between the energy mismatch and the host phonon energy (for YLiF4 crystal host, ħω ≈ 450 cm-1) indicates that about two host phonons are annihilated for each ETU process (see Table 4.1).

Pan Stanford Publishing eBooks•Aug 31, 2016•0 citations
A vibronic model of laser cooling for crystals doped with Yb3+ ions is proposed. The model involves the stimulated Raman adiabatic passage pumping through dipole-allowed 4f–5d transitions, electron transitions between Stark-split sublevels due to vibronic interaction, and anti-Stokes fluorescence from the excited ion state. Dynamics of the cooling process are described by the density matrix formalism. It is shown that the cooling power in the case of vibronic interaction is higher at least by a factor of 3.4 compared to the case of electron–phonon interaction. In the proposed model, an increase in the cooling power yields deeper and faster refrigeration of a crystal doped with Yb3+ ions. Estimations show that, on cooling by the stimulated Raman adiabatic passage pumping, the temperature of a crystal with an irradiated volume of 2.12×10−4 cm3 can reach 64 K in a time of 2 s. In the proposed model, the cooling temperature is 30 K lower and the cooling process is 100 times faster compared to the traditional model of direct pumping. The estimates are applicable to present-day materials of technologically attainable purity.
To overcome the ETU-induced heating and realize efficient and enhanced laser cooling in Ho3+-doped solids, in Section 4.3, we will provide a modified excitation scheme based on ground-state absorption (GSA) of 5I8 Æ 5I7 at around 2.07 μm and ESA of 5I5 Æ 5F5 at around 2.28 μm. Compared with the conventional pumping scheme, the co-pumping scheme ameliorates the cooling performance significantly through alleviating the upconversion-quenching-induced heat [12], that is, the heat-producing 5I5 Ho3+ions are pumped to the 5F5 state by the laser at 2.28 μm. Fortunately, the 5F5 Ho3+ ions barely transit to the lower nearby state and tend to decay radiatively. Therefore, major heat produced in the conventional laser cooling of Ho3+-doped solids is avoided, and both cooling efficiency and cooling power density can be improved. In Section 4.4, we broaden the research domain of optical refrigeration to rare earth ion co-doped systems. Specifically, when Ho3+–Tm3+ co-doped YLiF4 crystals are pumped at around 2.07 μm, Ho3+ ions will populate at the 5I7 manifold. Meanwhile, Tm3+ ions will also be sensitized by absorbing energy transferred from 5I7 Ho3+ ions. Since the average energy of fluorescence photons generated by Tm3+3F4 Æ 3H6 radiative transitions is higher than that generated by Ho3+5I7 Æ 5I8 radiative transitions, energy transfer (ET) from Ho3+ to Tm3+ ions will induce annihilation of host phonons, and bring enhancement in both the cooling efficiency and the cooling power. Therefore, this cooling mechanism is referred next as energy transfer-enhanced laser cooling (ETLC) of solids [11]. 4.2 Conventional Laser Cooling of Holmium- The main upconversion process and the anti-Stokes fluorescence cooling (ASFC) processes of Ho3+-doped fluoride crystals are illustrated in Fig. 4.1. The ground-state (5I8) Ho3+ ions are pumped to the first excited state (5I7) with laser excitations of energy hν (solid red arrow on the left) and then relax thermally among the Stark levels in a timescale of picoseconds with host phonon absorption. Part of the Ho3+5I7 ions de-excite by emitting fluorescence photons of mean energy hν10 (solid blue arrow, ν10 > ν), which accounts for the ASFC process. The rest of the 5I7 Ho3+ ions de-excited and transfer their energy to the neighboring 5I7 Ho3+ ions, causing population accumulation at the third excited state (5I5) with host phonon absorption (solid green arrows). Comparison between the energy mismatch and the host phonon energy (for YLiF4 crystal host, ħω ≈ 450 cm-1) indicates that about two host phonons are annihilated for each ETU process (see Table 4.1).