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Phonon sidebands, electron-phonon coupling and vibronic lasing in Tm$^{3+}$:Lu$_2$O$_3$ sesquioxide

Pavel A. Loiko, Kirill Eremeev, Christian Kränkel, Alain Braud, Patrice Camy

Published Jul 1, 2024• 1 citation
OpenAlex

Abstract

A vibronic Tm:Lu$_2$O$_3$ laser generated 654 mW at 2238-2309 nm with a slope efficiency of 68.9% exceeding the Stokes limit. Tm:Lu2O3 features a strong electron-phonon interaction resulting in a profound long-wave phonon sideband for the $^3$F$_4$ → $^3$H$_6$ electronic transition extending up to at least 2.4 μm supporting vibronic laser operation.

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Phonon sidebands, electron-phonon coupling and vibronic lasing in Tm3+^{3+}3+:Lu2_22​O3_33​ sesquioxide
A vibronic Tm:Lu2_22​O3_33​ laser generated 654 mW at 2238-2309 nm with a slope efficiency of 68.9% exceeding the Stokes limit. Tm:Lu2O3 features a strong electron-phonon interaction resulting in a profound long-wave phonon sideband for the 3^33F4_44​ → 3^33H6_66​ electronic transition extending up to at least 2.4 μm supporting vibronic laser operation.
A compact Tm:GdVO4_44​ laser pumped by a 794 nm laser diode generated 6.09 W at 2.29 μm ( 3^33H4_44​ → 3^33H5_55​ Tm3+^{3+}3+ transition) with a high slope efficiency of 30.8% and linear laser polarization (π). The polarized spectroscopic properties of Tm3+^{3+}3+ in GdVO4_44​ were also revised. The peak stimulated-emission cross-section of Tm3+^{3+}3+ is 2.97 × 10−20^{-20}−20 cm2^22 at 2280 nm corresponding to an emission bandwidth of 42 nm for π-polarized light.
The Mollow triplet is the definitive spectral signature of an optically dressed quantum emitter. We predict that for emitters coupled to localized phonons, this signature is not confined to the zero-phonon line. Under a strong resonant drive, we show that Mollow triplets are strikingly replicated on the associated phonon sidebands -a surprising result, given that phonon sidebands are typically viewed as incoherent, inelastic scattering pathways. These vibronic Mollow triplets are a direct fingerprint of dynamically generated dressed states that hybridize the emitter's electronic, photonic, and vibrational degrees of freedom. We develop a scalable analytical formalism to model this effect in complex, multi-mode molecular systems, such as dibenzoterrylene. Our work provides the precise driving conditions for observing these novel spectral features, establishing a new signature of coherence in vibronically coupled systems.
Coupling between electronic motions and the lattice vibrations, phonons could broaden the spectral bandwidth of the fluorescence spectroscopy by the energy transferring, which was recognized from the beginning of last century and successfully applied in many vibronic lasers. However, the laser performances under electron-phonon coupling were mainly prejudged by the experimental spectroscopy. The multiphonon participated lasing mechanism is still elusive and should be in-depth investigated. Here, a direct quantitative relationship between the laser performance and phonon participating dynamic process was derived in theory. With a transition metal doped alexandrite (Cr 3+ :BeAl 2 O 4 ) crystal, the multiphonon coupled laser performance was manifested in experiments. Associated with the Huang-Rhys factor calculations and hypothesis, the multiphonon participated lasing mechanism with phonon numbers from 2 to 5 was discovered and identified. This work provides not only a credible model for understanding the multiphonon participated lasing, but should also boost the study of laser physics in the electron-phonon-photon coupled systems.