“…The generated SRS emission lines cover the broad region from ≈0.2 to ≈2 μm and result from SRSactive vibration modes with energies that range between ≈50 DOI: 10.1002/crat.202100055 and ≈3400 cm −1 . The Raman shifts of these SRS-active Raman modes, however, are not distributed equally within the so far realized energy range and there are only few materials, e.g., 𝛼quartz (𝜔 SRS ≈ 465 cm −1 [2] ) and 𝛼-Al 2 O 3 (𝜔 SRS ≈ 419 cm −1 [3,4] ), that possess SRSpromoting vibration modes of around 450 cm −1 . Here, 𝛼-AlOOH, which shows a strong, sharp, and isolated vibration mode at 446 cm −1 in its spontaneous Raman spectra, [5] appears to be a promising further material which could complement the set of SRS materials in this region.…”