Photon Upconversion through a Cascade Process of Two-Photon Absorption in CsPbBr₃ and Triplet–Triplet Annihilation in Porphyrin/Diphenylanthracene

Abstract

Photon upconversion constitutes an exceptionally rich area of research in photonics and electronics, where low-energy light is converted to high-energy light through nonlinear processes represented by two-photon absorption (TPA) and triplet−triplet annihilation (TTA). Here, we report a cascade process of TPA in inorganic perovskite quantum dots (PQDs) of CsPbBr 3 and TTA in an organic molecule (9,10-diphenylanthracene) mediated by an octaethylporphyrinatoplatinum(II) (PtOEP) sensitizer. This sequential energy transfer enables upconversion from four photons from a near-infrared femtosecond laser at 800 nm to one photon at 430 nm with a large anti-Stokes shift of ∼1.3 eV. We characterize the energy transfer from PQDs to PtOEP by picosecond lifetime spectroscopy and a Stern−Volmer plot of the steady-state photoluminescence while considering dynamic and static quenching as well as trivial absorption and Forster (fluorescence) resonance energy transfer. The serial connection of TPA and TTA achieved in a simple system opens up an attractive avenue in nonlinear photonics and harvesting of low-energy photons.

Unraveling Reversible Quenching Processes of O2, N2, Ar, and H2O in Metal Halide Perovskites at Moderate Photon Flux Densities

“…This is a standard technique most commonly used in organic chemistry to study the diffusive nature and charge transfer kinetics from a fluorescent emitter to a mobile quencher. [78,79] Although this technique is generally employed to describe the quenching effect of molecules in solution, [80][81][82][83][84] it has also been successfully used in the soft-matter and solid state. In many of these cases, emitters are distributed and immobilized in a gas permeable thin film.…”

Nonlinear Photonics Using Low‐Dimensional Metal‐Halide Perovskites: Recent Advances and Future Challenges

“…Excellent 2PA capability of CsPbBr 3 was quantified utilizing the OA Z‐scan method with fs pulsed laser excitation at 800 nm, and giant σ 2 value of ≈1.2 × 10 5 GM and ≈4.2 × 10 5 GM before and after the local field effect correction was revealed. Following this intriguing report, so far more than 34 other research works [ 92–96,99,101–111,138,189,234–248 ] on the 2PA response of NCs of 3D metal‐halide perovskites have been carried out and published. 2PA performance from NCs of 3D organic–inorganic MAPbX 3 and all‐inorganic CsPbX 3 (X = Cl, Br, I, or mixed halide) was the research focus in most of the published articles.…”

“…The inherent σ 2 values of MAPbX 3 and CsPbX 3 NCs were determined to be in the range of ≈(10 5 to 10 7 ) GM across the visible–NIR excitation wavelength range of ≈(600–1250) nm. [ 92–96,99,101–111,138,189,234–237,239–248 ] The variation of σ 2 values can be attributed to one or some of the following factors: different sample compositions (e.g., different A + or X − in AMX 3 ), assorted sample sizes, various sample shapes, diverse sample quality, different excitation wavelengths, discrepant excitation pulsed lasers. On the other hand, Jiang et al.…”

Ratiometric Nanoparticle Probe Based on FRET‐Amplified Phosphorescence for Oxygen Sensing with Minimal Phototoxicity

“…This result indicates that the observed PtOEP emission corresponds to phosphorescence, which is in line with the observed long acceptor emission lifetimes on the time scale of microseconds ( Figure 5D) and the literature data for PtOEP. [37] Observation of phosphoresce at room temperature is remarkable phenomenon that attracted strong attention recently. [38] In our NPs, it was observed for two reasons.…”