Abstract
AbstractMolecular compounds of the general formula [(RT)4E6] (R=organic or organometallic substituent; T=C, Si, Ge, Sn; E=CH2, S, Se), hence adamantane derivatives and inorganic‐organic hybrid compounds based on a heteroadamantane structure exhibit a non‐linear optical response upon radiation with a continuous‐wave near‐infrared laser. The effect depends on the compounds’ habitus, which itself depends on the elemental composition of the cluster core, and on the nature of the organic substituents. A combination of these parameters that cause the material to be intrinsically amorphous leads to supercontinuum generation and thus to the emission of a broad spectrum, potentially appearing as white light. Notably, the emission essentially retains the driving laser's directionality. For crystalline samples, second harmonic generation is observed instead, which points to a close relationship of the optical properties and the intermolecular order. Variation of R, T, and E allows further fine‐tuning of the emitted spectra. We present all studies made in regards to these effects and our overarching conclusions derived from them.
Highlights
Molecular compounds of the general formula [(RT)4E6] (R = organic or organometallic substituent; T = C, Si, Ge, Sn; E = CH2, S, Se), adamantane derivatives and inorganic-organic hybrid compounds based on a heteroadamantane structure exhibit a non-linear optical response upon radiation with a continuous-wave near-infrared laser
The fact that the transition was not observed in 1 at the investigated pump powers was explained by the lower band gap of the inorganic compounds relative to the organic structure, which leads to an enhancement of nonlinear optical effects by the fundamental transition dipole moment associated with the cluster core, as the detuning of the driving laser is smaller in this case
Nonlinear optical properties have been observed for inorganic heteroadamantane-based compounds and for purely organic adamantane derivatives, one being strong second harmonic generation (SHG) and the other one being a more extreme nonlinear effect that causes the generation of a supercontinuum, which in most cases covers the visible spectrum, and is referred to as white-light generation (WLG)
Summary
We will give a chronological overview of the research done in this specific area of WLG and SHG generation with the compounds under consideration This includes the syntheses and crystal structure determinations, the investigation of linear and nonlinear optical absorption properties, exploration of morphology and molecular aggregation in amorphous samples, and quantum chemical investigations of geometric and electronic structures of the clusters as well as solid materials based on them. Decomposition Nearly insoluble material[34] Amorphization upon laser irradiation Amorphization upon laser irradiation WLG hindered by re-absorption www.chemphotochem.org
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