Given the ubiquity of glass formulations that are functionalized with silver compounds, the electronic interaction between isolated silver cations and the glass network deserves more attention. Here, we report the structural origin of the optical properties that result from silver doping in fluorophosphate (PF) and sulfophosphate (PS) glasses. To achieve this, solid-state nuclear magnetic resonance (NMR) spectroscopy and density functional theory (DFT) are combined with optical spectroscopic analysis and physical property measurements. Comparing the 31 P NMR, 27 Al 1d NMR, and 27 Al multi-quantum magic-angle spinning NMR of doped glasses and glasses with large amounts of Ag + added, we deduce silver's bonding preference in these mixed-anion aluminophosphate glasses. We show that such understanding provides an explanation for the large Stokes shift observed for Ag + in PF and PS glasses, which is related to absorption by the ionic Ag + ••• − O−P species and transfer of the excitation energy within more covalently bonded Ag 2 O-like clusters. This is corroborated by DFT calculations, which show that the Ag + ••• − O−P and Ag + ••• − O−S bonds in corresponding crystals are mostly ionic. The introduction of more silver ions into the crystal structure results in more covalent bonding between Ag + and the phosphate matrix.
Ultrasound‐induced mechanoluminescence (USML) of Erbium‐doped CaZnOS is reported. Using the fluorescence intensity ratio of the
2
H
11/2
,
4
S
3/2
→
4
I
15/2
transitions of Er
3+
allows for simultaneous temperature mapping at an absolute sensitivity of 0.003 K
−1
in the physiological regime. The combination of USML, local heating, and remote read‐out enables a feedback and response loop for highly controlled stimulation. It is found that ML is a result of direct energy transfer from the host material to Er
3+
, giving room for adapted spectral characteristics through bandgap modulation. ML saturation at high acoustic power enables independent control of local light emission and ultrasonic heating. Such USML materials may have profound implications for optogenetics, photodynamic therapy and other areas requiring local illumination, heating, and thermometry simultaneously.
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