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- Bielecki, Johan, 1982
(författare)
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Optical Spectroscopy on Correlated Electron Materials
- 2010
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Licentiatavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Strongly correlated materials poses a great challenge to our microscopic understanding of matter, mainly due to the inability of perturbative methods to predict the properties of such materials. This inability stems from strong correlations between electronic, lattice and spin degrees of freedom, leading to a variety of complex and exotic phenomena such as (unconventional) superconductivity, metal-insulator transitions, non-Fermi liquid behavior and colossal magnetoresistance.In this thesis, optical spectroscopy investigations on two kinds of strongly correlated matter is presented: materials exhibiting colossal magnetoresistance (manganites) and superconductivity (iron-pnictides). The research has been done from a fundamental point of view, with the goal to advance our understanding of the fascinating interplay between electrons, phonons and spin fluctuation that is encountered in these materials. The electron-phonon coupling in the newly discovered iron-pnictide class of high temperature superconductors have been studied using Raman spectroscopy assisted by theoretical calculations with the goal to elucidate the role of phonons as the mediating boson between electrons in a Cooper-pair. Our results indicate that the phononic spectra can, to good accuracy, be explained by neglecting completely the electron-phonon coupling. This provides further credentials to the widespread opinion that magnetic fluctuations constitute the attractive force responsible for the destabilization of the Fermi-sea leading to the condensation into superconducting Cooper-pairs. Further analysis shows that, through F doping on the O site, ejecting electrons into the quasi-two dimensional Fe-As plane actually leads to hole-doping at the Fe site, in accord with previous first principle calculations.The fundamental dynamics between the electrons, lattice and spins in two manganite samples have been studied using sub-picosecond time resolved pump-probe reflectance spectroscopy: The parent compound LaMnO3 and the doped La0.7Ca0.3MnO3 exhibiting colossal magnetoresistance. Even though LaMnO3 is a semiconductor and La0.7Ca0.3MnO3 is a double-exchange metal at low temperatures, the observed femtosecond dynamics are very similar. We introduce a phenomenological model that can explain all observed features in both samples using a combination of thermal (>1ps) and non-thermal (
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| 2. |
- Bielecki, Johan, 1982
(författare)
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Structure and Dynamics in Transition Metal Perovskites — An Optical Spectroscopy Study
- 2012
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Transition metal oxides with the perovskite structure exhibit a vast number of exotic properties due to the large number of competing degrees of freedom at the Fermi surface. Together with couplings between and correlations within these degrees of freedom, this class of materials is of high interest from both a practical and theoretical point of view. In this thesis, the properties of four different perovskite systems and their relation to structure and dynamics is investigated: La1-x CaxMnO3, exhibiting the colossal magnetoresistance effect; LaCoO3, undergoing spin-state transitions influenced by complicated electron-lattice interactions; BiFeO3 that is of the only known room-temperature multiferroic materials; and the proton conductor BaInO3H.Two kinds of optical spectroscopy methods have been used to investigate the structure and dynamics of these transition metal perovskites. Raman spectroscopy measures low-energy excitations and is, in combination with group theoretical selection rules, a sensitive probe of electronic, atomic, and magnetic structure. Ultrafast time-resolved spectroscopy is used to study, in real time, fundamental dynamics and interaction mechanisms on the femtosecond timescale.Utilizing time resolved pump-probe reflectance spectroscopy, thermal and lattice contributions to the spin-state transition are temporarily decouple, and the first explicit observation of the high-spin repulsion in LaCoO3, first conjectured by Goodenough in the 1950's, is presented. This opens up a novel avenue for investigating the spin-state transition in LaCoO3. With the same experimental technique, the electron-lattice, lattice-spin, and electron-spin dynamics are investigated in La1-xCaxMnO3. Incorporating a two-component heat diffusion mechanism it is shown that the rate-equation based model captures all essentials of the >1 ps dynamics.Raman spectroscopy is used to investigate the structural phase-diagram of isovalently substituted BiFeO3. The vibrational frequencies as a function of substitution provides unique input into the controversial phonon assignments of BiFeO3 and the pronounced second-order scattering is explained in terms of LO-modes activated by the Fröhlich interaction. Further, the first phonon assignment is presented and the structural transition during dehydration is investigated for BaInO3H.Complementing the studies on perovskites, the electron-phonon interactions are investigated in a iron-pnictide high temperature superconductor by combining Raman spectroscopy and phonon-phonon calculations. Our results point towards weak electron-phonon couplings and supports the view that a non-phononic glue is responsible for the Cooper pair condensation in iron-pnictides.
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| 3. |
- Bielecki, Johan, 1982, et al.
(författare)
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Two-component heat diffusion observed in LaMnO3 and La0.7Ca0.3MnO3
- 2010
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Ingår i: Physical Review B Condensed Matter. - : Americal Physical Society. - 0163-1829 .- 1095-3795. ; 81:6, s. art. no. 064434-
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Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- We investigate the low-temperature electron, lattice, and spin dynamics of LaMnO3 (LMO) and La0.7Ca0.3MnO3 (LCMO) by resonant pump-probe reflectance spectroscopy. Probing the high-spin d-d transition as a function of time delay and probe energy, we compare the responses of the Mott insulator and the double-exchange metal to the photoexcitation. Attempts have previously been made to describe the subpicosecond dynamics of colossal magnetoresistance manganites in terms of a phenomenological three-temperature model describing the energy transfer between the electron, lattice, and spin subsystems followed by a comparatively slow exponential decay back to the ground state. However, conflicting results have been reported. Here we first show clear evidence of an additional component in the long-term relaxation due to film-to-substrate heat diffusion and then develop a modified three-temperature model that gives a consistent account for this feature. We confirm our interpretation by using it to deduce the band gap in LMO. In addition, we also model the nonthermal subpicosecond dynamics, giving a full account of all observed transient features both in the insulating LMO and the metallic LCMO.
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