Dynamical evolution of the Schottky barrier as a determinant contribution to electron–hole pair stabilization and photocatalysis of plasmon-induced hot carriers

Abstract

The harnessing of plasmon-induced hot carriers promises to open new avenues for the development of clean energies and chemical catalysis. The extraction of carriers before thermalization and recombination is of...

Plasmon-Induced Hot Carriers: An Atomistic Perspective of the First Tens of Femtoseconds

“…The second important feature that can be observed from Figure b is that this huge charge injection is stable even for the pulse excitation (in ref we show that this is the case up to 250 fs with and without nuclear motion). This result is in tune with the charge separation liftimes of ps and ns observed experimentally.…”

“…To study the photoinjection and subsequent catalysis, we employed CO molecules bonded to the TiO 2 NP ([Au-TiO 2 -CO]). The details of the Hamiltonian parametrization and the building of the model can be found in ref ; the resulting structure is shown in the inset of Figure a together with its absorption spectrum. In ref , the correct description of the Au and TiO 2 NP spectra is assessed in terms of experimental and other theoretical reports.…”

“…The details of the Hamiltonian parametrization and the building of the model can be found in ref ; the resulting structure is shown in the inset of Figure a together with its absorption spectrum. In ref , the correct description of the Au and TiO 2 NP spectra is assessed in terms of experimental and other theoretical reports. The whole [Au-TiO 2 -CO] structure presents an LSPR peak band at 2.4 eV and a broad absorption at higher energies produced by the interband absorption of Au and TiO 2 .…”

“…The fact that this does not happen clearly points to the development of a new source of charge stabilization. We have characterized this feature as a new contribution to the point contact potential or Schottky barrier, that we called “Dynamical Contribution to the Schottky Barrier” (DSB) . In Figure d, a profile of the electrostatic potential modification at the end of the simulation (Δ V ) in the interparticle axis is presented.…”

Benchmarking DFTB+ on the first singlet vertical excitation energy of small organic molecules

“…In other words, the approximations of DFTB bring quantum mechanics to systems that otherwise would be treated with classical force fields. As a result, DFTB is being widely employed in pure and hybrid QM-schemes for the simulation of the spectroscopic properties of nanostructures [8], photoactive materials [9] and complex biological systems [10] of many thousands of atoms.…”