Meghdad Yazdi-Rizi

Strongly bound excitons in anatase TiO2 single crystals and nanoparticles

Anatase TiO2 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.Here the authors combine steady-state angle-resolved photoemission spectroscopy, ellipsometry and ultrafast two-dimensional ultraviolet spectroscopy to examine the role of many-body correlations in anatase TiO2, revealing the existence of strongly bound excitons in single crystals and nanoparticles.

Terahertz ellipsometry study of the soft mode behavior in ultrathin SrTiO3 films

We present a combined study with conventional far-infrared and time-domain terahertz ellipsometry of the temperature dependent optical response of SrTiO3 thin films (85 and 8.5 nm) that are grown by pulsed-laser deposition on LSAT substrates. We demonstrate that terahertz ellipsometry is very sensitive to the optical response of these thin films, in particular, to the soft mode of SrTiO3. We show that for the 85 nm film the eigenfrequency of the soft mode is strongly reduced by annealing at 1200 C, whereas for the 8.5 nm film it is hardy affected. For the latter, after annealing the mode remains at 125 cm-1 at 300 K and exhibits only a weak softening to about 90 cm-1 at 10 K. This suggests that this ultrathin film undergoes hardly any relaxation of the compressive strain due to the LSAT substrate.

Optical probe of ferroelectric order in bulk and thin-film perovskite titanates

We have measured the temperature dependence of the direct band gap Eg in SrTiO3 and BaTiO3 and related materials with quantum-paraelectric and ferroelectric properties using optical spectroscopy. We show that Eg exhibits an anomalous temperature dependence with pronounced changes in the vicinity of the ferroelectric transition that can be accounted for in terms of the Frohlich electron-phonon interaction with an optical phonon mode, the so-called soft mode. In addition, we demonstrate that these characteristic changes of Eg can be readily detected even in very thin films of SrTiO3 with a strain-induced ferroelectric order. Optical spectroscopy thus can be used as a rather sensitive probe of ferroelectric order in very thin films of these titanates and probably also in subsequent multilayers and devices.

Infrared Study of the Spin Reorientation Transition and Its Reversal in the Superconducting State in Underdoped Ba(1-x)K(x)Fe(2)As(2).

With infrared spectroscopy we investigated the spin-reorientation transition from an orthorhombic antiferromagnetic (o-AF) to a tetragonal AF (t-AF) phase and the reentrance of the o-AF phase in the superconducting state of underdoped Ba(1-x)K(x)Fe(2)As(2). In agreement with the predicted transition from a single-Q to a double-Q AF structure, we found that a distinct spin density wave develops in the t-AF phase. The pair breaking peak of this spin density wave acquires much more low-energy spectral weight than the one in the o-AF state which indicates that it competes more strongly with superconductivity. We also observed additional phonon modes in the t-AF phase which likely arise from a Brillouin-zone folding that is induced by the double-Q magnetic structure with two Fe sublattices exhibiting different magnitudes of the magnetic moment.

Low-energy interband transitions in the infrared response of Ba(Fe1-xCox)2As2

We studied the doping and temperature (T) dependence of the infrared (IR) response of Ba(Fe1_xCox)2As2 single crystals. We show that a weak band around 1000 cm_1, that was previously interpreted in terms of interaction of the charge carriers with magnetic excitations or of a pseudogap, is rather related to low energy interband transitions. Specifically, we show that this band exhibits a similar doping and T dependence as the hole pockets seen by angle resolved photoemission spectroscopy (ARPES). Notably, we find that it vanishes as a function of doping near the critical point where superconductivity is suppressed in the overdoped regime. Our IR data thus provide bulk specific information (complementary to the surface sensitive ARPES) for a Lifshitz transition. Our IR data also reveal a second low-energy band around 2300 cm_1 which further emphasizes the necessity to consider the multiband nature of these iron arsenides in the analysis of the optical response.

Infrared ellipsometry study of photogenerated charge carriers at the (001) and (110) surfaces of SrTiO3 crystals and at the interface of the corresponding LaAlO3/SrTiO3 heterostructures

The work at the University of Fribourg was supported by the Schweizerische Nationalfonds (SNF) through Grant No. 200020-153660. B.P.P.M. wishes to acknowledge support from the Marsden Fund of New Zealand. The work at MUNI was financially supported by the Ministry of education youth and sports of the Czech Republic, under the project CEITEC 2020 (LQ1601). M.S., F.S., and G.H. acknowledge the support by the Spanish Government through Project No. MAT2014-56063-C2-1-R, the Severo Ochoa Grant No. SEV-2015-0496, and the Generalitat de Catalunya (Project No. 2014SGR 734). J. Mannhart is acknowledged for providing the LAO/STO (001) sample and J. Foncuberta for scientific discussion.

Infrared ellipsometry study of the confined electrons in a high-mobility γ-Al2O3/SrTiO3 heterostructure

With infrared ellipsometry we studied the response of the confined electrons in gamma-Al2O3/SrTiO3 (GAO/STO) heterostructures in which they originate predominantly from oxygen vacancies. From the analysis of a so-called Berreman mode, that develops near the highest longitudinal optical phonon mode of SrTiO3, we derive the sheet carrier density, N-s, the mobility, mu, and the depth profile of the carrier concentration. Notably, we find that N-s and the shape of the depth profile are similar as in LaAlO3/SrTiO3 (LAO/STO) heterostructures for which the itinerant carriers are believed to arise from a polar discontinuity. Despite an order of magnitude higher mobility in GAO/STO, as obtained from transport measurements, the derived mobility in the infrared range exhibits only a twofold increase. We interpret this finding in terms of the polaronic nature of the confined charge carriers in GAO/STO and LAO/STO which leads to a strong, frequency-dependent interaction with the STO phonons. Copyright (C) EPLA, 2016

Anisotropy of infrared-active phonon modes in the monodomain state of tetragonal SrTiO3 (110)

With infrared and terahertz ellipsometry we investigated the anisotropy of the infrared active phonon modes in SrTiO3 (110) single crystals in the tetragonal state below the so-called antiferrodistortive transition at T* = 105 K. In particular, we show that the anisotropy of the oscillator strength of the so-called R-mode, which becomes weakly infrared active below T*, is a valuable indicator for the orientation of the structural domains. Our results reveal that a mono-domain state with the tetragonal axis (c-axis) parallel to the [001] direction can be created by applying a moderate uniaxial stress of about 2.3 MPa along the [1-10] direction (with a mechanical clamp). The resulting, intrinsic splitting of the infrared-active phonon modes is reported.

Anomalous anisotropic exciton temperature dependence in rutile TiO2

Elucidating the details of 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 TiO2, revealing a strong anisotropic polarization dependence with increasing temperature, namely, an anomalous blue shift for light polarized along the a axis and a conventional red shift 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 blue shift 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.

X-ray absorption study of the ferromagnetic Cu moment at the YBa2Cu3O7/La2/3Ca1/3MnO3 interface and variation of its exchange interaction with the Mn moment

With x-ray absorption spectroscopy and polarized neutron reflectometry we studied how the magnetic proximity effect at the interface between the cuprate high-TC superconductor YBa2Cu3O7 (YBCO) and the ferromagnet La2/3Ca1/3MnO3 (LCMO) is related to the electronic and magnetic properties of the LCMO layers. In particular, we explored how the magnitude of the ferromagnetic Cu moment on the YBCO side depends on the strength of the antiferromagnetic (AF) exchange coupling with the Mn moment on the LCMO side. We found that the Cu moment remains sizable if the AF coupling with the Mn moments is strongly reduced or even entirely suppressed. The ferromagnetic order of the Cu moments thus seems to be intrinsic to the interfacial CuO2 planes and related to a weakly ferromagnetic intraplanar exchange interaction. The latter is discussed in terms of the partial occupation of the Cu 3d3z2 - r2 orbitals, which occurs in the context of the so-called orbital reconstruction of the interfacial Cu ions.