arXiv subjects

Adriel Dominguez

Publications and source records attributed to Adriel Dominguez.

6 recordsLinked to original sources

arXiv2020

Giant exciton Mott density in anatase TiO2

Elucidating the carrier density at which strongly bound excitons dissociate into a plasma of uncorrelated electron-hole pairs is a central topic in the many-body physics of semiconductors. However, there is a lack of information on the high-density response of excitons absorbing in the near-to-mid ultraviolet, due to the absence of suitable experimental probes in this elusive spectral range. Here, we present a unique combination of many-body perturbation theory and state-of-the-art ultrafast broadband ultraviolet spectroscopy to unveil the interplay between the ultraviolet-absorbing two-dimensional excitons of anatase TiO$_2$ and a sea of electron-hole pairs. We discover that the critical density for the exciton Mott transition in this material is the highest ever reported in semiconductors. These results deepen our knowledge of the exciton Mott transition and pave the route toward the investigation of the exciton phase diagram in a variety of wide-gap insulators.

cond-mat.mtrl-sci↗

arXiv2018

Phonon-Driven Selective Modulation of Exciton Oscillator Strengths in Anatase TiO2 Nanoparticles

The way nuclear motion affects electronic responses has become a very hot topic in materials science. Coherent acoustic phonons can dynamically modify optical, magnetic and mechanical properties at ultrasonic frequencies, with promising applications as sensors and transducers. Here, by means of ultrafast broadband deep-ultraviolet spectroscopy, we demonstrate that coherent acoustic phonons confined in anatase TiO$_2$ nanoparticles can selectively modulate the oscillator strength of the two-dimensional bound excitons supported by the material. We use many-body perturbation-theory calculations to reveal that the deformation potential is the mechanism behind the generation of the observed coherent acoustic wavepackets. Our results offer a route to manipulate and dynamically tune the properties of excitons in the deep-ultraviolet at room temperature.

cond-mat.mes-hall↗

arXiv2018

Exciton Control in a Room-Temperature Bulk Semiconductor with Coherent Strain Pulses

The coherent manipulation of excitons in bulk semiconductors via the lattice degrees of freedom is key to the development of acousto-optic and acousto-excitonic devices. Wide-bandgap transition metal oxides exhibit strongly bound excitons that are interesting for applications in the deep-ultraviolet, but their properties have remained elusive due to the lack of efficient generation and detection schemes in this spectral range. Here, we perform ultrafast broadband deep-ultraviolet spectroscopy on anatase TiO$_2$ single crystals at room temperature, and reveal a dramatic modulation of the exciton peak amplitude due to coherent acoustic phonons. This modulation is comparable to those of nanostructures where exciton-phonon coupling is enhanced by quantum confinement, and is accompanied by a giant exciton shift of 30-50 meV. We model these results by many-body perturbation theory and show that the deformation potential coupling within the nonlinear regime is the main mechanism for the generation and detection of the coherent acoustic phonons. Our findings pave the way to the design of exciton control schemes in the deep-ultraviolet with propagating strain pulses.

cond-mat.mtrl-sci↗

arXiv2017

Strongly bound excitons in anatase TiO2 single crystals and nanoparticles

Anatase TiO$_2$ is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over the continuum of indirect interband transitions. This exciton possesses an intermediate character between the Wannier-Mott and Frenkel regimes and displays a peculiar two-dimensional wavefunction in the three-dimensional lattice. The nature of the higher-energy excitations is also identified. The universal validity of our results is confirmed up to room temperature by observing the same elementary excitations in defect-rich samples (doped single crystals and nanoparticles) via ultrafast two-dimensional deep-ultraviolet spectroscopy.

cond-mat.mtrl-sci↗

arXiv2017

Anomalous Anisotropic Exciton Temperature Dependence in Rutile TiO2

Elucidating the details of the electron-phonon coupling in semiconductors and insulators is a topic of pivotal interest, as it governs the transport mechanisms and is responsible for various phenomena such as spectral-weight transfers to phonon sidebands and self-trapping. Here, we investigate the influence of the electron-phonon interaction on the excitonic peaks of rutile TiO$_2$, revealing a strong anisotropic polarization dependence with increasing temperature, namely an anomalous blueshift for light polarized along the a-axis and a conventional redshift for light polarized along the c-axis. By employing many-body perturbation theory, we identify two terms in the electron-phonon interaction Hamiltonian that contribute to the anomalous blueshift of the a-axis exciton. Our approach paves the way to a complete ab initio treatment of the electron-phonon interaction and of its influence on the optical spectra of polar materials.

cond-mat.mtrl-sci↗

arXiv2008

Exact-Diagonalization Studies of Inelastic Light Scattering in Self-Assembled Quantum Dots

We report exact diagonalization studies of inelastic light scattering in few-electron quantum dots under the strong confinement regime characteristic of self-assembled dots. We apply the orthodox (second-order) theory for scattering due to electronic excitations, leaving for the future the consideration of higher-order effects in the formalism (phonons, for example), which seem relevant in the theoretical description of available experiments. Our numerical results stress the dominance of monopole peaks in Raman spectra and the breakdown of selection rules in open-shell dots. The dependence of these spectra on the number of electrons in the dot and the incident photon energy is explicitly shown. Qualitative comparisons are made with recent experimental results.

cond-mat.mes-hall↗