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Register a new userStrong spin-phonon coupling unveiled by coherent phonon oscillations in Ca2RuO4
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We utilize near-infrared femtosecond pulses to investigate coherent phonon oscillations of Ca2RuO4. The coherent Ag phonon mode of the lowest frequency changes abruptly not only its amplitude but also the oscillation-phase as the spin order develops. In addition, the phonon mode shows a redshift entering the magnetically ordered state, which indicates a spin-phonon coupling in the system. Density functional theory calculations reveal that the Ag oscillations result in octahedral tilting distortions, which are exactly in sync with the lattice deformation driven by the magnetic ordering. We suggest that the structural distortions by the spin-phonon coupling can induce the unusual oscillation-phase shift between impulsive and displacive type oscillations.
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We investigate the antiadiabatic limit of an antiferromagnetic S=1/2 Heisenberg chain coupled to Einstein phonons via a bond coupling. The flow equation method is used to decouple the spin and the phonon part of the Hamiltonian. In the effective spin model longer range spin-spin interactions are generated. The effective spin chain is frustrated. The resulting temperature dependent couplings are used to determine the magnetic susceptibility and to determine the phase transition from a gapless state to a dimerized gapped phase. The susceptibilities and the phase diagram obtained via the effective couplings are compared with independently calculated quantum Monte Carlo results.
The coupling of the manganite stripe phase to the lattice and to strain has been investigated via transmission electron microscopy studies of polycrystalline and thin film manganites. In polycrystalline PCMOfiftwo a lockin to $q/a^*=0.5$ in a sample with $x>0.5$ has been observed for the first time. Such a lockin has been predicted as a key part of the Landau CDW theory of the stripe phase. Thus it is possible to constrain the size of the electron-phonon coupling in the CDW Landau theory to between 0.04% and 0.05% of the electron-electron coupling term. In the thin film samples, films of the same thickness grown on two different substrates exhibited different wavevectors. The different strains present in the films on the two substrates can be related to the wavevector observed via Landau theory. It is demonstrated that the the elastic term which favours an incommensurate modulation has a similar size to the coupling between the strain and the wavevector, meaning that the coupling of strain to the superlattice is unexpectedly strong.
Antiferromagnetism (AF) such as Neel ordering is often closely related to Coulomb interactions such as Hubbard repulsion in two-dimensional (2D) systems. Whether Neel AF ordering in 2D can be dominantly induced by electron-phonon couplings (EPC) has not been completely understood. Here, by employing numerically-exact sign-problem-free quantum Monte Carlo (QMC) simulations, we show that optical Su-Schrieffer-Heeger (SSH) phonons with frequency $omega$ and EPC constant $lambda$ can induce AF ordering for a wide range of phonon frequency $omega>omega_c$. For $omega<omega_c$, a valence-bond-solid (VBS) order appears and there is a direct quantum phase transition between VBS and AF phases at $omega_c$. The phonon mechanism of the AF ordering is related to the fact that SSH phonons directly couple to electron hopping whose second-order process can induce an effective AF spin exchange. Our results shall shed new lights to understanding AF ordering in correlated quantum materials.
We employ an optical pump-probe technique to study coherent phonon oscillations in Ca$_2$RuO$_4$. We find that oscillation-amplitude of an $A_g$ symmetric phonon mode is strongly suppressed at 260 K, a putative transition point of orbital ordering. The oscillation also shows a gradual but huge change in its $phase$, such that the oscillation even flips over with a 180$^{circ}$ change across the temperature. Density functional theory calculations indicate that the $A_g$ phonon has an eigenmode of octahedral distortion with conventional tilting along the $a$-axis and antipolar distortion of apical oxygen. Careful inspection of the lattice captures an unusually large antipolar distortion in low-temperature structures, which may play a crucial role for the phase transition at 260 K.
Enhanced coupling of material properties offers new fundamental insights and routes to multifunctional devices. In this context 5d oxides provide new paradigms of cooperative interactions driving novel emergent behavior. This is exemplified in 5d osmates that host a metal-insulator transition (MIT) driven by magnetic order. Here we consider the most robust case, the 5d perovskite NaOsO3, and reveal a giant coupling between spin and phonon through a frequency shift of {Delta}{omega}=40 cm-1, the largest measured in any material. We identify the dominant octahedral breathing mode and show isosymmetry with spin ordering which induces dynamic charge disproportionation that sheds new light on the MIT. The occurrence of the dramatic spin-phonon-electronic coupling in NaOsO3 is due to a property common to all 5d materials: the large spatial extent of the 5d ion. This allows magnetism to couple to phonons on an unprecedented scale and consequently offers multiple new routes to enhanced coupled phenomena.
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