arXiv subjects

P. E. Blöchl

Publications and source records attributed to P. E. Blöchl.

5 recordsLinked to original sources

arXiv2025

Elementary Steps of Energy Conversion in Strongly Correlated Systems: Beyond Single Quasiparticles and Rigid Bands

Energy conversion in materials can be considered as a sequence of elementary steps initiated by a primary excitation. While these steps are quite well understood in classical semiconductors in terms of quasiparticle (QP) excitations and interactions, their understanding in strongly correlated materials is still elusive. Here, we review the progress which has been achieved over recent years by studies of manganite perovskite oxides as a model system for materials with strong correlations. They show a subtle interplay of different types of correlations, i.e., electron-phonon, electron-electron and spin-spin, resulting in rich physical phenomena due to competition between different ground states accompanied by temperature- and field-induced phase transitions. They strongly impact various types of energy conversion and transport processes including friction at surfaces, thermal transport, time-, energy- and power-dependent optical excitations as well as photovoltaic energy conversion. The underlying microscopic processes can be broken down to the behavior of the low-energy thermal and high-energy optical excitations, their interactions, transport and conversion which are theoretically analyzed by using models of interacting and tunable QPs: Their nature and interactions can change during excitation, transport and phase transitions, thus modifying electronic structure. At sufficiently high stimulation, QP excitations can even induce or actuate phase transitions. As a result, we obtained a comprehensive understanding of energy conversion steps going far beyond single QP pictures and rigid band approximations well-known for conventional semiconductors.

cond-mat.str-el↗

arXiv2024

Characteristic THz-emissions induced by optically excited collective orbital modes

We study the generation of collective orbital modes, their evolution, and the characteristic nonlinear optical response induced by them in a photoinduced orbital-ordered correlated oxide using real-time simulations based on an interacting multiband tight-binding (TB) model. The d-d optical transitions under femtoseconds light-pulse in an orbital-ordered state excite collective orbital modes, also known as "orbitons". Consistently incorporating electronic interactions and the interplay between charge, spin, and lattice degrees of freedom in the TB-model provides a clearer understanding of how these factors influence the generation and evolution of collective orbital modes. The dynamics of Jahn-Teller vibrational modes in the photoinduced state modify the intersite orbital interaction, which further amplifies these orbital modes. In the presence of weak ferroelectricity, the excitation of collective orbital modes induces a strong THz oscillatory photocurrent, which is long-lived. This suggests an alternative way to experimentally detect low-energy collective modes through THz-emission studies in the photoinduced state. Our study also elucidates that quasiparticle dynamics in improper ferroelectric oxides can be exploited to achieve highly interesting and non-trivial optoelectronic properties.

cond-mat.str-el↗

arXiv2020

Orbital order phase transition in $Pr_{1-x}Ca_xMnO_3$ probed by photovoltaics

The phase diagram of $Pr_{1-x}Ca_xMnO_3$ is modified x $\le$ 0.3, which suggests a reevaluation of the phase diagram of other manganites in that doping region. Rather than an orbital ordered phase reaching up to high temperatures of approximately 800-1100 K, we propose a loss of spontaneous orbital order already near room temperature. Above this temperature, the phase is characterized by a finite orbital polarization and octahedral tilt pattern. The tilt pattern couples to the Jahn-Teller distortion and thus induces a remaining orbital order, which persists up to high temperatures, where the tilt order is lost as well. This explains the experimental observation of orbital order up to high temperatures. The reevaluation of the orbital order transition is based on observed anomalies of various physical properties at a temperatures of 220-260 K in epitaxial thin films of $Pr_{1-x}Ca_xMnO_3$ x=0.1, i.e.in the photovoltaic effect, electric transport, magnetization, optical and ultrafast transient pump probe studies. Finite-temperature simulations based on a tight-binding model with carefully adjusted parameters from first-principles calculations exhibit an orbital order phase transition at $T_{OO} \approx$ 300 K for x=0.1. This is consistent with the experimental observation of a temperature dependent change in lattice parameter for bulk samples of the same doping at 300 K for x=0.1 and 350 K for x=0, typical for a second order phase transition. Since our reassignment of the orbital order phase transition towards lower temperatures challenges a well-established and long-accepted picture, we provide results of multiple complementary measurements as well as a detailed discussion.

cond-mat.str-el↗

arXiv2020

Ultrafast spin-nematic and ferroelectric phase transitions induced by femto-second light pulses

Optically-induced phase transitions of the manganite $\rm Pr_{1/3}Ca_{2/3}MnO_3$ have been simulated using a model Hamiltonian, that captures the dynamics of strongly correlated charge, orbital, lattice, and spin degrees of freedom. Its parameters have been extracted from first-principles calculations. Beyond a critical intensity of a femto-second light pulse, the material undergoes ultra-fast and non-thermal magnetic phase transition from a non-collinear to collinear antiferromagnetic phases. The light-pulse excites selectively either a spin-nematic or a ferroelectric phase depending on the light-polarization. The behavior can be traced to an optically induced ferromagnetic coupling between Mn-trimers, i.e. polarons which are delocalized over three Mn-sites. The polarization guides the polymerization of the polaronic crystal into distinct patterns of ferromagnetic chains determining the target phase.

cond-mat.str-el↗

arXiv2020

Surface resonance of the (2$\times$1) reconstructed lanthanum hexaboride (001)-cleavage plane: a combined STM and DFT study

We performed a combined study of the (001)-cleavage plane of lanthanum hexaboride (LaB$_\text{6}$) using scanning tunneling microscopy (STM) and density functional theory (DFT). Experimentally, we found a (2$\times$1) reconstructed surface on a local scale. The reconstruction is only short-range ordered and tends to order perpendicularly to step edges. At larger distances from surface steps, the reconstruction evolves to a labyrinth-like pattern. These findings are supported by low-energy electron diffraction (LEED) experiments. Slab calculations within the framework of DFT shows that the atomic structure consists of parallel lanthanum chains on top of boron octahedra. Scanning tunneling spectroscopy (STS) shows a prominent spectral feature at -0.6 eV. Using DFT, we identify this structure as a surface resonance of the (2$\times$1) reconstructed LaB$_\text{6}$ (100)-surface which is dominated by boron dangling bond-states and lanthanum d-states.

cond-mat.mes-hall↗