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Peter M. Gehring

Publications and source records attributed to Peter M. Gehring.

10 recordsLinked to original sources

Magnetoelastic honeycomb fragmentation in VI$_{3}$

The discovery of ordered magnetism in two-dimensional van der Waals materials at the monolayer limit challenges the Mermin-Wagner theorem, which forbids spontaneous breaking of continuous symmetries in two dimensions at finite temperatures. The persistence of static magnetism in low-dimensions is fundamentally influenced by magnetic anisotropy and the local single-ion crystalline electric field. Crucially, spin-orbit coupling connects the structural properties with spin degrees of freedom. We investigate the magnetic single-ion properties in the van der Waals magnet VI$_3$. Utilizing neutron and x-ray diffraction, we map out the symmetry breaking phase transitions and argue for a single structural transition at T$_S \sim$ 80 K, driven by an orbital degeneracy, followed by a ferromagnetic transition at a lower temperature, T$_C \sim$ 50 K. Through a comparative analysis of samples prepared under varying conditions, we suggest that lower temperature transitions reported near $\sim$ 30 K are not intrinsic to VI$_{3}$. A group theoretical analysis suggests a structural transition from rhombohedral $R\overline{3}$ to triclinic $P\overline{1}$ or $P1$. This transition is significant as it suggests the formation of two distinct crystallographyically inequivalent V$^{3+}$ sites, each with distinct spin-orbital properties. Neutron spectroscopy provides evidence for dominant magnetic exchange coupling only between symmetry-equivalent sites in the triclinc unit cell. We suggest this breaks up the low-temperature honeycomb VI$_3$ lattice into two interpenetrating approximately hexagonal planes resulting in a fragmentated honeycomb. Our findings highlight the critical role of magnetoelastic coupling in determining the magnetic and structural phases in two-dimensional van der Waals magnets.

cond-mat.mtrl-sci

Anisotropic Band-Split Magnetism in Magnetostrictive CoFe$_2$O$_4$

Single crystal spinel CoFe$_2$O$_4$ exhibits the largest room-temperature saturation magnetostriction among non-rare-earth compounds and a high Curie temperature ($T_c \sim 780$ K), properties that are critical to a wide range of industrial and medical applications. Neutron spectroscopy reveals a large band splitting ($\sim$ 60 meV) between two ferrimagnetic magnon branches, which is driven by site mixing between Co$^{2+}$ and Fe$^{3+}$ cations, and a significantly weaker magnetocrystalline anisotropy ($\sim$ 3 meV). Central to this behavior is the competition between extremely large mismatched molecular fields on the tetrahedral $A$-site and octahedral $B$-site sublattices and the single-ion anisotropy on the $B$-site. This creates a strong energetic anisotropy that locks the magnetic moment within each structural domain in place. As a result of these differing energy scales, switching structural domains is energetically favored over a global spin reorientation under applied magnetic fields, and this is what amplifies the magnetostrictive nature of CoFe$_2$O$_4$.

cond-mat.mtrl-sci

On the question of dynamic domains and critical scattering in cubic methylammonium lead triiodide

We investigate the hypothesis of dynamic tetragonal domains occuring in cubic CH$_3$NH$_3$PbI$_3$ using high-resolution neutron spectroscopy to study a fully deuterated single crystal. The $\textit{R}$-point scattering above the 327.5 K tetragonal-cubic phase transition is always resolution-limited in energy and therefore inconsistent with dynamic domain predictions. This behavior is instead consistent with the central peak phenomenon observed in other perovskites. The scattering may originate from small, static, tetragonal-phase domains nucleating about crystal defects, and the temperature dependence demonstrates the transition is first-order.

cond-mat.mtrl-sci

Electric field effect on short-range polar orders in a relaxor ferroelectric system

Short-range polar orders in the relaxor ferroelectric material PbMg$_{1/3}$Nb$_{2/3}$O$_3$-$28\%$PbTiO$_3$ (PMN-28PT) have been studied using neutron diffuse scattering. An external electric field along [110] direction can affect the diffuse scattering in the low temperature rhombohedral/monoclinic phase. Diffuse scattering intensities associated with [110] short-range polarizations are partially suppressed, while those arising from [1$\bar{1}$0] polarizations are enhanced. On the other hand, short-range polar orders along other equivalent $\langle110\rangle$ directions, i.e. [101],[10$\bar{1}$], [011], and [01$\bar{1}$] directions, are virtually unaffected by the field. Our results, combined with previous work, strongly suggest that most part of short-range polar orders in PMN-$x$PT relaxor systems are robust in the low temperature phase, where they couple strongly to ferroelectric polarizations of the surrounding ferroelectric domains, and would only respond to an external field indirectly through ferroelectric domain rotation.

cond-mat.mtrl-sci

Acoustic Phonon Lifetimes Limit Thermal Transport in Methylammonium Lead Iodide

Hybrid organic-inorganic perovskites (HOIPs) have become an important class of semiconductors for solar cells and other optoelectronic applications. Electron-phonon coupling plays a critical role in all optoelectronic devices, and although the lattice dynamics and phonon frequencies of HOIPs have been well studied, little attention has been given to phonon lifetimes. We report the first high-precision measurements of acoustic phonon lifetimes in the hybrid perovskite methylammonium lead iodide (MAPI), using inelastic neutron spectroscopy to provide high energy resolution and fully deuterated single crystals to reduce incoherent scattering from hydrogen. Our measurements reveal extremely short lifetimes on the order of picoseconds, corresponding to nanometer mean free paths and demonstrating that acoustic phonons are unable to dissipate heat efficiently. Lattice-dynamics calculations using ab-initio third-order perturbation theory indicate that the short lifetimes stem from strong three-phonon interactions and a high density of low-energy optical phonon modes related to the degrees of freedom of the organic cation. Such short lifetimes have significant implications for electron-phonon coupling in MAPI and other HOIPs, with direct impacts on optoelectronic devices both in the cooling of hot carriers and in the transport and recombination of band edge carriers. These findings illustrate a fundamental difference between HOIPs and conventional photovoltaic semiconductors and demonstrate the importance of understanding lattice dynamics in the effort to develop metal halide perovskite optoelectronic devices.

cond-mat.mtrl-sci

Spin-wave induced phonon resonance in multiferroic BiFeO$_3$

We report the direct observation of a "resonance" mode in the lowest-energy optic phonon very near the zone center around (111) in the multiferroic BiFeO$_3$ using neutron scattering methods. The phonon scattering intensity is enhanced when antiferromagnetic (AFM) order sets in at T$_N = 640$~K, and it increases on cooling. This "resonance" is confined to a very narrow region in energy-momentum space where no spin-wave excitation intensity is expected, and it can be modified by an external magnetic field. Our results suggest the existence of a novel coupling between the lattice and spin fluctuations in this multiferroic system in which the spin-wave excitations are mapped onto the lattice vibrations via the Dzyaloshinskii-Moriya (DM) interaction.

cond-mat.mtrl-sci

Thermal evolution of the full three-dimensional magnetic excitations in the multiferroic BiFeO3

The idea of embedding and transmitting information within the fluctuations of the magnetic moments of spins (spin waves) has been recently proposed and experimentally tested. The coherence of spin waves, which describes how well defined these excitations are, is of course vital to this process, and themost significant factor that affects the spin-wave coherence is temperature. Here we present neutron inelastic scattering measurements of the full threedimensional spin-wave dispersion in BiFeO3, which is one of the most promising functional multiferroic material, for temperatures from 5K to 700K. Despite the presence of strong electromagnetic coupling, the magnetic excitations behave like conventional magnons over all parts of the Brillouin zone. At low temperature the spin-waves are well-defined coherent modes, described by a classical model for a G-type antiferromagnet. A spin-wave velocity softening is already present at room temperature, and more pronounced damping occurs as the magnetic ordering temperature TN \sim 640K is approached. In addition, a strong hybridization of the Fe 3d and O 2p states is found to modify the distribution of the spin-wave spectral weight significantly, which implies that the spins are not restricted to the Fe atomic sites as previously believed.

cond-mat.mtrl-sci

Dynamic origin of the morphotropic phase boundary - Soft modes and phase instability in 0.68Pb(Mg1/3Nb2/3O3)-0.32PbTiO3

We report neutron inelastic scattering on single crystal 0.68Pb(Mg1/3Nb2/3O3)-0.32PbTiO3 (PMN-0.32PT), a relaxor ferroelectric material that lies within the compositional range of the morphotropic phase boundary (MPB). Data were obtained between 100 K and 600 K under zero and non-zero electric field applied along the cubic [001] direction. The lowest energy, zone-center, transverse optic phonon is strongly damped and softens slowly at high temperature; however the square of the soft mode energy begins to increase linearly with temperature as in a conventional ferroelectric, which we term the soft mode "recovery," upon cooling into the tetragonal phase at TC. Our data show that the soft mode in PMN-0.32PT behaves almost identically to that in pure PMN, exhibiting the same temperature dependence and recovery temperature even though PMN exhibits no well-defined structural transition (no TC). The temperature dependence of the soft mode in PMN-0.32PT is also similar to that in PMN-0.60PT; however in PMN-0.60PT the recovery temperature equals TC. These results suggest that the temperature dependence and the energy scale of the soft mode dynamics in PMN-xPT are independent of concentration on the Ti-poor side of the MPB, but scale with TC for Ti-rich compositions. Thus the MPB may be defined in lattice dynamical terms as the concentration where TC first matches the recovery temperature of the soft mode. High-resolution x-ray studies show that the cubic-to-ferroelectric phase boundary shifts to higher temperatures by an abnormal amount within the MPB region in the presence of an electric field. This suggests that an unusual instability exists within the apparently cubic phase at the MPB.

cond-mat.mtrl-sci

Neutron scattering study of soft phonons and diffuse scattering in insulating La$_{1.95}$Sr$_{0.05}$CuO$_{4}$

Soft phonons and diffuse scattering in insulating La$_{2-x}$Sr$_{x}$CuO$_4$ ($x=0.05$) have been studied by the neutron scattering technique. The X-point phonon softens from high temperature towards the structural transition temperature $T_{s}=410$ K, and the Z-point phonon softens again below 200 K. The Z-point phonon softening persists to low temperature, in contrast to the behavior observed in the superconducting $x=0.15$ compound, in which the Z-point phonon hardens below $T_c$. The diffuse scattering associated with the structural phase transition at 410 K appears at commensurate positions. These results highlight interesting differences between superconducting and insulating samples.

cond-mat.supr-con

Neutron Diffraction Study of the Irreversible R-MA-MC Phase Transition in Single Crystal Pb[(Zn1/3Nb2/3)1-xTix]O3

Single crystals of the relaxor PZN-xPT display an enormously strong piezoelectric character. Recent x-ray scattering studies have revealed novel electric-field induced phase transitions in PZN-8%PT. As-grown crystals exhibit a rhombohedral structure that, under application of an electric field oriented along [001], transforms into a monoclinic (MA) phase, and then irreversibly to another monoclinic (MC) phase with increasing field strength. Since the latter phase change is very unusual, its transition sequence has been investigated by using triple-axis neutron scattering techniques so that the ``skin effect'' observed by x-ray scattering can be avoided, and the entire crystal bulk is probed. Contour maps of the elastic scattering have been mapped out in each phase in the (HOL) zone with high q-resolution. Increasing the field strength within the MC phase induces a sharp c-axis jump around 15 kV/cm. This jump was observed easily with x-rays in previous studies, but it was not observed in 5 different crystals examined with neutrons. A subsequent high-energy x-ray study of the same crystals showed that the c-axis jump is distributed within the crystal volume, thereby washing out the jump. The observed R-MA-MC transformational path is in perfect accord with very recent first principles calculations by Bellaiche, Garcia, and Vanderbilt in the PZT system.

cond-mat.str-el