Giant two-photon absorption of anatase TiO2 in Au/TiO2 core-shell nanoparticles

We report on deep-to-near-UV transient absorption spectra of core-shell Au/SiO2 and Au/TiO2 nanoparticles (NPs) excited at the surface plasmon resonance of the Au core, and of UV-excited bare anatase TiO2 NPs. The bleaching of the first excitonic transition of anatase TiO2 at -3.8 eV is a signature of the presence of electrons/ holes in the conduction band (CB)/valence band (VB) of the material. We find that while in bare anatase TiO2 NPs, two-photon excitation does not occur up to the highest used fluences (1.34 mJ/cm2), it takes place in the TiO2 shell at moderate fluences (0.18 mJ/cm2) in Au/TiO2 core-shell NPs, as a result of an enhancement due to the plasmon resonance. We estimate the enhancement factor to be of the order of -108-109. Remarkably, we observe that the bleach of the 3.8 eV band of TiO2 lives significantly longer than in bare TiO2, suggesting that the excess electrons/holes in the conduction/valence band are stored longer in this material.& COPY; 2023 Chinese Laser Press

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Majed Chergui, Malte Oppermann, Lijie Wang
2023
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https://infoscience.epfl.ch/record/304141?ln=en

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Valence and conduction bands

In solid-state physics, the valence band and conduction band are the bands closest to the Fermi level, and thus determine the electrical conductivity of the solid. In nonmetals, the valence band is the highest range of electron energies in which electrons are normally present at absolute zero temperature, while the conduction band is the lowest range of vacant electronic states. On a graph of the electronic band structure of a semiconducting material, the valence band is located below the Fermi level, while the conduction band is located above it.

Electron hole

In physics, chemistry, and electronic engineering, an electron hole (often simply called a hole) is a quasiparticle denoting the lack of an electron at a position where one could exist in an atom or atomic lattice. Since in a normal atom or crystal lattice the negative charge of the electrons is balanced by the positive charge of the atomic nuclei, the absence of an electron leaves a net positive charge at the hole's location. Holes in a metal or semiconductor crystal lattice can move through the lattice as electrons can, and act similarly to positively-charged particles.

Surface plasmon resonance

Surface plasmon resonance (SPR) is a phenomenon that occurs where electrons in a thin metal sheet become excited by light that is directed to the sheet with a particular angle of incidence, and then travel parallel to the sheet. Assuming a constant light source wavelength and that the metal sheet is thin, the angle of incidence that triggers SPR is related to the refractive index of the material and even a small change in the refractive index will cause SPR to not be observed.

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