Soon Jae Moon

Electronic structures of hexagonal R Mn O 3 ( R = Gd , Tb, Dy, and Ho) thin films: Optical spectroscopy and first-principles calculations

We investigated the electronic structure of multiferroic hexagonal RMnO3 (R = Gd, Tb, Dy, and Ho) thin films using both optical spectroscopy and first-principles calculations. Using artificially stabilized hexagonal RMnO3, we extended the optical spectroscopic studies on the hexagonal multiferroic manganite system. We observed two optical transitions located near 1.7 eV and 2.3 eV, in addition to the predominant absorption above 5 eV. With the help of first-principles calculations, we attribute the low-lying optical absorption peaks to inter-site transitions from the oxygen states hybridized strongly with different Mn orbital symmetries to the Mn 3d3z2-r2 state. As the ionic radius of the rare earth ion increased, the lowest peak showed a systematic increase in its peak position. We explained this systematic change in terms of a flattening of the MnO5 triangular bipyramid.

Effects of oxygen-reducing atmosphere annealing on LaMnO3 epitaxial thin films

We investigated the effects of annealing on LaMnO3 epitaxial thin films grown by pulsed laser deposition (PLD) and propose an efficient method of characterizing their stoichiometry. Structural, magnetic and optical properties coherently indicate non-stoichiometric ferromagnetic and semiconducting phases for as-grown LaMnO3 films. By annealing in an oxygen-reducing atmosphere, we recovered the antiferromagnetic and insulating phases of bulk-like stoichiometric LaMnO3. We show that non-destructive optical spectroscopy at room temperature is one of the most convenient tools for identifying the phases of LaMnO3 films. Our results serve as a prerequisite for studying LaMnO3 based heterostructures grown by PLD.

Dimensional crossover of polaron dynamics in Nb:SrTiO3/SrTiO3 superlattices: Possible mechanism of thermopower enhancement

Using optical spectroscopy, we investigated the electrodynamic properties of Nb:SrTiO3/SrTiO3 superlattices. In these superlattices, a large enhancement of the Seebeck coefficient (S) has been reported with decreasing Nb:SrTiO3 layer thickness [refer to H. Ohta et al., Nature Mater. 6, 129 (2007)]. By analyzing the optical spectra, we found that the polaron plays an important role in determining the electrodynamic properties of the superlattices. With decreasing Nb:SrTiO3 layer thickness from eleven to one unit cell, we observed a threefold enhancement of the polaron effective mass and relaxation time. Such increases were attributed to a dimensional crossover of polaron from 3D to quasi-2D. Moreover, the modified nature of the polaron at low dimensions enhanced the thermoelectric properties of the oxide superlattice, by simultaneously increasing S and preventing the decrease of carrier mobility. Our results indicate that strong electron-phonon coupling can provide an alternative pathway in searching efficient thermoelectric materials.

Temperature evolution of itinerant ferromagnetism in SrRuO3 probed by optical spectroscopy.

The temperature (T) dependence of the optical conductivity spectra σ(ω) of a single crystal SrRuO(3) thin film is studied over a T range from 5 to 450 K. We observed significant T dependence of the spectral weights of the charge transfer and interband d-d transitions across the ferromagnetic Curie temperature (T(c) ∼ 150 K). Such T dependence was attributed to the increase in the Ru spin moment, which is consistent with the results of density functional theory calculations. T scans of σ(Ω,T) at fixed frequencies Ω reveal a clear T(2) dependence below T(c), demonstrating that the Stoner mechanism is involved in the evolution of the electronic structure. In addition, σ(Ω,T) continues to evolve at temperatures above T(c), indicating that the local spin moment persists in the paramagnetic state. This suggests that SrRuO(3) is an intriguing oxide system with itinerant ferromagnetism.

Dimensionality Control of d-orbital Occupation in Oxide Superlattices

Manipulating the orbital state in a strongly correlated electron system is of fundamental and technological importance for exploring and developing novel electronic phases. Here, we report an unambiguous demonstration of orbital occupancy control between t2g and eg multiplets in quasi-two-dimensional transition metal oxide superlattices (SLs) composed of a Mott insulator LaCoO3 and a band insulator LaAlO3. As the LaCoO3 sublayer thickness approaches its fundamental limit (i.e. one unit-cell-thick), the electronic state of the SLs changed from a Mott insulator, in which both t2g and eg orbitals are partially filled, to a band insulator by completely filling (emptying) the t2g (eg) orbitals. We found the reduction of dimensionality has a profound effect on the electronic structure evolution, which is, whereas, insensitive to the epitaxial strain. The remarkable orbital controllability shown here offers a promising pathway for novel applications such as catalysis and photovoltaics, where the energy of d level is an essential parameter.