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arXiv:1407.6779 · Physical Review B

Model of nonadiabatic-to-adiabatic dynamical quantum phase transition in photoexcited systems

Jun Chang, Ilya Eremin, Jize Zhao

Published Sep 18, 2014• 2 citations
arXivHTMLPDF

Abstract

We study the ultrafast dynamic process in photoexcited systems and find that the Franck-Condon or Landau-Zener tunneling between the photoexcited state and the ground state is abruptly blocked with increasing the state coupling from nonadiabatic to adiabatic limits. The blockage of the tunneling inhibits the photoexcited state from decaying into the thermalized state and results in an emergence of a metastable state, which represents an entanglement of electronic states with different electron-phonon coupling strengths. Applying this model to the investigation of photoexcited half-doped manganites, we show that the quantum critical transition is responsible for more than a three-order-of-magnitude difference in the ground-state recovery times following photoirradiation. This model also explains some elusive experimental results, such as photoinduced rearrangement of orbital order by the structural rather than electronic process and the structural bottleneck of a one-quarter period of the Jahn-Teller mode. We demonstrate that in the spin-boson model there exist unexplored regions not covered in the conventional phase diagram.

DOI
10.1103/physrevb.90.104305

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We study the ultrafast dynamic process in photoexcited systems and find that the Franck-Condon or Landau-Zener tunneling between the photoexcited state and the ground state is abruptly blocked with increasing the state coupling from nonadiabatic to adiabatic limits. The blockage of the tunneling inhibits the photoexcited state from decaying into the thermalized state and results in an emergence of a metastable state, which represents an entanglement of electronic states with different electron-phonon coupling strengths. Applying this model to the investigation of photoexcited half-doped manganites, we show that the quantum critical transition is responsible for more than a three-order-of-magnitude difference in the ground-state recovery times following photoirradiation. This model also explains some elusive experimental results, such as photoinduced rearrangement of orbital order by the structural rather than electronic process and the structural bottleneck of a one-quarter period of the Jahn-Teller mode. We demonstrate that in the spin-boson model there exist unexplored regions not covered in the conventional phase diagram.
We investigate the evolution of a photoexcitation in correlated materials over a wide range of time scales. The system studied is a one-dimensional model of a manganite with correlated electron, spin, orbital, and lattice degrees of freedom, which we relate to the three-dimensional material ${\mathrm{Pr}}_{1\ensuremath{-}x}{\mathrm{Ca}}_{x}{\mathrm{MnO}}_{3}$. The ground-state phases for the entire composition range are determined and rationalized by a coarse-grained polaron model. At half doping a pattern of antiferromagnetically coupled Zener polarons is realized. Using time-dependent density-matrix renormalization group (tDMRG), we treat the electronic quantum dynamics following the excitation. The emergence of quasiparticles is addressed, and the relaxation of the nonequilibrium quasiparticle distribution is investigated via a linearized quantum-Boltzmann equation. Our approach shows that the magnetic microstructure caused by the Zener polarons leads to an increase of the relaxation times of the excitation.
We investigate the behavior of 1D correlated systems following a photo-excitation by combining ab-initio methods, time-dependent matrix product state (MPS) approaches, analytical insights from quantum Boltzmann equations, and molecular dynamics (MD) simulations to describe the dynamics on different time scales ranging from femtoseconds up to nanoseconds. This is done for manganite systems in the material class Pr1−xCaxMnO3. We derive one-dimensional ab-initio model Hamiltonians for which we compute the ground states at different values of the doping using MD simulations. At half doping, we obtain a magnetic microstructure of alternating dimers which we use as a starting point to formulate a one-dimensional Hubbard-type model. In this strongly correlated 1D system we address the formation of quasiparticles after photoexcitations. We introduce a quasiclassical model for the absorption process of light which takes into account the backaction of the electrons to the electromagnetic field and compare the results with the ones obtained with a Peierls substitution ansatz in which we neglect the backaction. Taking this effect into account leads to a stronger response since the emitted radiation can be re-absorbed by neighboring particles. We use the resulting state as starting point for the short-time dynamics which we obtain from 'numerically exact' MPS calculations. The dynamics is analyzed concerning the formation and lifetime of quasi-particles which form a starting point for the description of the relaxation process via a linearized quantum Boltzmann equation. In this way, our work constitutes a first step to building a unifying theoretical framework for the description of photoexcitations in strongly correlated materials over a wide range of time scales, capable of making predictions for ongoing experiments investigating pump-probe situations and unconventional photovoltaics.
Motivated by the experimental observation of resonant tunneling in systems of half-integer spin, such as V15 and Mn4, we study the mechanism of the adiabatic change of the magnetization in systems with time-reversal symmetry. Although tunneling between the degenerate ground states is suppressed in a simple Kramers doublet, some types of perturbational interactions cause an avoided level crossing structure in the energy level structures when the system possesses additional degeneracy of the ground state. We show that a nonadiabatic transition governed by the Landau-Zener-Stückelberg mechanism occurs in many cases, and also find more general cases of adiabatic change of the magnetization in which LZS mechanism cannot be applied directly.
The photoexcited state in a correlated electron system with a spin-state degree of freedom is studied. We start from the two-orbital extended Hubbard model where the energy difference between the two orbitals is introduced. The photoexcited metastable state is examined based on the effective model Hamiltonian derived using the two-orbital Hubbard model. Spin-state change is induced by photoirradiation in the low-spin band insulator near the phase boundary, and it is found that a high-spin state is stabilized by creating a ferromagnetic bound state with photodoped hole carriers. An optical absorption occurs between the bonding and antibonding orbitals inside the bound state. The time evolution of photoexcited states is simulated in the time-dependent mean-field scheme. It is found that pair annihilations of photodoped electrons and holes generate the high-spin state in a low-spin band insulator. We propose that this process is directly observed by the time-resolved photoemission experiments.
Competition between ordered phases, and their associated phase transitions, are significant in the study of strongly correlated systems. Here, we examine one aspect, the nonequilibrium dynamics of a photoexcited Mott-Peierls system, using an effective Peierls-Hubbard model and exact diagonalization. Near a transition where spin and charge become strongly intertwined, we observe antiphase dynamics and a coupling-strength-dependent suppression or enhancement in the static structure factors. The renormalized bosonic excitations coupled to a particular photoexcited electron can be extracted, which provides an approach for characterizing the underlying bosonic modes. The results from this analysis for different electronic momenta show an uneven softening due to a stronger coupling near k_{F}. This behavior reflects the strong link between the fermionic momenta, the coupling vertices, and ultimately, the bosonic susceptibilities when multiple phases compete for the ground state of the system.
Photo-induced hidden phases are often observed in materials with intertwined orders. Understanding the formation of these non-thermal phases is challenging and requires a resolution of the cooperative interplay between different orders on the ultra-short timescale. In this work, we demonstrate that non-equilibrium photo-excitations can induce a state with spin-orbital orders entirely different from the equilibrium state in the three-quarter-filled two-band Hubbard model. We identify a general mechanism governing the transition to the hidden state, which relies on a non-thermal partial melting of the intertwined orders mediated by photoinduced charge excitations in the presence of strong spin-orbital exchange interactions. Our study theoretically confirms the crucial role played by orbital degrees of freedom in the light-induced dynamics of strongly correlated materials and it shows that the switching to hidden states can be controlled already on the fs timescale of the electron dynamics.