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Michael Fechner

Publications and source records attributed to Michael Fechner.

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Parametric resonance of Josephson plasma waves: A theory for optically amplified interlayer superconductivity in YBa$_2$Cu$_3$O$_{6+x}$

Non-linear interactions between collective modes play a definitive role in far out of equilibrium dynamics of strongly correlated electron systems. Understanding and utilizing these interactions is crucial to photo-control of quantum many-body states. One of the most surprising examples of strong mode coupling is the interaction between apical oxygen phonons and Josephson plasmons in bilayer YBa$_2$Cu$_3$O$_{6+x}$ superconductors. Experiments by Hu et al (2014). and Kaiser et al. (2014) showed that below Tc, photo-excitation of phonons leads to enhancement and frequency shifts of Josephson plasmon edges, while aboveTc, photo-excited phonons induce plasmon edges even when there are no discernible features in the equilibrium reflectivity spectrum. Recent experiments by Van Hoegen et al. (2019) also observed parametric generation of Josephson plasmons from photo-excited phonons both below Tc and in the pseudogap phase. In this paper we present a theoretical model of phonon-plasmon three wave interaction arising from coupling between the oxygen motion and the in-plane superfluid stiffness. Analysis of the parametric instability of plasmons based on this model gives frequencies of the most unstable plasmons that are in agreement with experimental observations. We also discuss how strong parametric excitation of Josephson plasmons can explain pump induced changes in the TeraHertz reflectivity of YBa$_2$Cu$_3$O$_{6+x}$ in the superconducting state, including frequency shifts and sharpening of Josephson plasmon edges, as well as appearance of a new peak around 2THz. An interesting feature of this model is that overdamped Josephson plasmons do not give any discernible features in reflectivity in equilibrium, but can develop plasmon edges when parametrically excited. We suggest that this mechanism explains photo-induced plasmon edges in the pseudogap phase of YBa$_2$Cu$_3$O$_{6+x}$.

cond-mat.supr-con

Polarizing an antiferromagnet by optical engineering of the crystal field

Strain engineering is widely used to manipulate the electronic and magnetic properties of complex materials. An attractive route to control magnetism with strain is provided by the piezomagnetic effect, whereby the staggered spin structure of an antiferromagnet is decompensated by breaking the crystal field symmetry, which induces a ferrimagnetic polarization. Piezomagnetism is especially attractive because unlike magnetostriction it couples strain and magnetization at linear order, and allows for bi-directional control suitable for memory and spintronics applications. However, its use in functional devices has so far been hindered by the slow speed and large uniaxial strains required. Here, we show that the essential features of piezomagnetism can be reproduced with optical phonons alone, which can be driven by light to large amplitudes without changing the volume and hence beyond the elastic limits of the material. We exploit nonlinear, three-phonon mixing to induce the desired crystal field distortions in the antiferromagnet CoF$_2$. Through this effect, we generate a ferrimagnetic moment of 0.2 $μ_B$ per unit cell, nearly three orders of magnitude larger than achieved with mechanical strain.

cond-mat.mtrl-sci

Metastable ferroelectricity in optically strained $SrTiO_3$

Fluctuating orders in solids are generally considered high-temperature precursors of broken symmetry phases. However, in some cases these fluctuations persist to zero temperature and prevent the emergence of long-range order, as for example observed in quantum spin and dipolar liquids. $SrTiO_3$ is a quantum paraelectric in which dipolar fluctuations grow when the material is cooled, although a long-range ferroelectric order never sets in. We show that the nonlinear excitation of lattice vibrations with mid-infrared optical pulses can induce polar order in $SrTiO_3$ up to temperatures in excess of 290 K. This metastable phase, which persists for hours after the optical pump is interrupted, is evidenced by the appearance of a large second-order optical nonlinearity that is absent in equilibrium. Hardening of a low-frequency mode indicates that the polar order may be associated with a photo-induced ferroelectric phase transition. The spatial distribution of the optically induced polar domains suggests that a new type of photo-flexoelectric coupling triggers this effect.

cond-mat.mtrl-sci

Terahertz-Driven Phonon Upconversion in SrTiO3

Direct manipulation of the atomic lattice using intense long-wavelength laser pulses has become a viable approach to create new states of matter in complex materials. Conventionally, a high frequency vibrational mode is driven resonantly by a mid-infrared laser pulse and the lattice structure is modified through indirect coupling of this infrared-active phonon to other, lower frequency lattice modulations. Here, we drive the lowest frequency optical phonon in the prototypical transition metal oxide SrTiO3 well into the anharmonic regime with an intense terahertz field. We show that it is possible to transfer energy to higher frequency phonon modes through nonlinear coupling. Our observations are carried out by directly mapping the lattice response to the coherent drive field with femtosecond x-ray pulses, enabling direct visualization of the atomic displacements.

cond-mat.mtrl-sci

Probing optically silent superfluid stripes in cuprates

Unconventional superconductivity in the cuprates emerges from, or coexists with, other types of electronic order. However, these orders are sometimes invisible because of their symmetry. For example, the possible existence of superfluid charge stripes in the normal state of single layer cuprates cannot be validated with infrared optics, because interlayer tunneling fluctuations vanish on average. Similarly, it is not easy to establish if charge orders are responsible for dynamical decoupling of the superconducting layers over broad ranges of doping and temperatures. Here, we show that TeraHertz pulses can excite nonlinear tunneling currents between linearly de-coupled charge-ordered planes. A giant TeraHertz third harmonic signal is observed in La1.885Ba0.115CuO4 far above Tc=13 K and up to the charge ordering temperature TCO = 55 K. We model these results by considering large order-parameter-phase oscillations in a pair density wave condensate, and show how nonlinear mixing of optically silent tunneling modes can drive large dipole-carrying super-current oscillations. Our results provide compelling experimental support for the presence of hidden superfluid order in the normal state of cuprates. These experiments also underscore the power of nonlinear TeraHertz optics as a sensitive probe of frustrated excitations in quantum solids.

cond-mat.supr-con

Correlated local dipoles in PbTe

We present a combined single-crystal x-ray diffuse scattering and ab-initio molecular dynamics study of lead telluride, PbTe. Well-known for its thermoelectric and narrow-gap semiconducting properties, PbTe recently achieved further notoriety following the report of an unusual off-centering of the lead atoms, accompanied by a local symmetry breaking, on heating. This observation, which was named emphanisis, ignited considerable controversy regarding the details of the underlying local structure and the appropriate interpretation of the total scattering experiments. In this study, we demonstrate close agreement between our diffuse scattering measurements and our calculations, which allows us to analyze features such as higher-order correlations that are accessible in the simulations but not experimentally. This allowed us to discover an unusual correlated local dipole formation extending over several unit cells with an associated local reduction of the cubic symmetry in both our x-ray diffuse scattering measurements and our molecular dynamics simulations. Importantly, when averaged spatially or temporally, the most probable positions for the ions are at the centers of their coordination polyhedra. Our results therefore clarify the nature of the local symmetry breaking, and reveal the source of the earlier controversy regarding the existence or absence of off-centering. Finally, we provide an interpretation of the behavior in terms of coupled soft optical and acoustic modes, which is linked also to the high thermoelectric performance of PbTe.

cond-mat.mtrl-sci

Parametric amplification of optical phonons

Amplification of light through stimulated emission or nonlinear optical interactions has had a transformative impact on modern science and technology. The amplification of other bosonic excitations, like phonons in solids, is likely to open up new remarkable physical phenomena. Here, we report on an experimental demonstration of optical phonon amplification. A coherent mid-infrared optical field is used to drive large amplitude oscillations of the Si-C stretching mode in silicon carbide. Upon nonlinear phonon excitation, a second probe pulse experiences parametric optical gain at all wavelengths throughout the reststrahlen band, which reflects the amplification of optical-phonon fluctuations. Starting from first principle calculations, we show that the high-frequency dielectric permittivity and the phonon oscillator strength depend quadratically on the lattice coordinate. In the experimental conditions explored here, these oscillate then at twice the frequency of the optical field and provide a parametric drive for lattice fluctuations. Parametric gain in phononic four wave mixing is a generic mechanism that can be extended to all polar modes of solids, as a new means to control the kinetics of phase transitions, to amplify many body interactions or to control phonon-polariton waves.

cond-mat.mtrl-sci

Probing the Interatomic Potential of Solids by Strong-Field Nonlinear Phononics

Femtosecond optical pulses at mid-infrared frequencies have opened up the nonlinear control of lattice vibrations in solids. So far, all applications have relied on second order phonon nonlinearities, which are dominant at field strengths near 1 MVcm-1. In this regime, nonlinear phononics can transiently change the average lattice structure, and with it the functionality of a material. Here, we achieve an order-of-magnitude increase in field strength, and explore higher-order lattice nonlinearities. We drive up to five phonon harmonics of the A1 mode in LiNbO3. Phase-sensitive measurements of atomic trajectories in this regime are used to experimentally reconstruct the interatomic potential and to benchmark ab-initio calculations for this material. Tomography of the Free Energy surface by high-order nonlinear phononics will impact many aspects of materials research, including the study of classical and quantum phase transitions.

cond-mat.mtrl-sci

Dynamical Multiferroicity

An appealing mechanism for inducing multiferroicity in materials is the generation of electric polarization by a spatially varying magnetization that is coupled to the lattice through the spin-orbit interaction. Here we describe the reciprocal effect, in which a time-dependent electric polarization induces magnetization even in materials with no existing spin structure. We develop a formalism for this dynamical multiferroic effect in the case for which the polarization derives from optical phonons, and compute the strength of the phonon Zeeman effect, which is the solid-state equivalent of the well-established vibrational Zeeman effect in molecules, using density functional theory. We further show that a recently observed behavior -- the resonant excitation of a magnon by optically driven phonons -- is described by the formalism. Finally, we discuss examples of scenarios that are not driven by lattice dynamics and interpret the excitation of Dzyaloshinskii-Moriya-type electromagnons and the inverse Faraday effect from the viewpoint of dynamical multiferroicity.

cond-mat.mtrl-sci

Effects of intense optical phonon pumping on the structure and electronic properties of yttrium barium copper oxide

We investigate the structural modulations induced by optical excitation of a polar phonon mode in YBa$_2$Cu$_3$O$_7$, using first-principles calculations based on density functional theory. We focus on the intense-excitation regime in which we expect that fourth-order phonon-phonon coupling terms dominate, and model the structural modulations induced by pulses of such intensity. Our calculations of the phonon-phonon anharmonicities confirm that the cubic coupling between modes, shown in earlier work to cause a quasi-static change in the apical O - Cu distance and a buckling of the CuO$_2$ planes, is the leading contribution at moderate pump strengths. At higher pump strengths ($\sim$10 MV/cm) the previously neglected quartic couplings become relevant and produce an additional shearing of the CuO$_2$ planes. Finally, we analyze the changes in the electronic and magnetic properties associated with the induced structural changes.

cond-mat.supr-con

Ultrafast Structure Switching through Nonlinear Phononics

We describe an ultrafast coherent control of the transient structural distortion arising from nonlinear phononics in ErFeO$_3$. Using density functional theory, we calculate the structural properties as input to an anharmonic phonon model that describes the response of the system to a pulsed optical excitation. We find that the trilinear coupling of two orthogonal infrared-active phonons to a Raman-active phonon causes a transient distortion of the lattice. The direction of the distortion is determined by the polarization of the exciting light, suggesting a route to nonlinear phononic lattice control and switching. Since the occurrence of the coupling is determined by the symmetry of the system we propose that it is a universal feature of orthorhombic and tetragonal perovskites.

cond-mat.mtrl-sci

First-principles calculation of the bulk magnetoelectric monopolization: Berry phase and Wannier function approaches

We present a formalism to calculate the macroscopic magnetoelectric monopolization from first principles within the density functional theory framework. An expression for the monopolization in the case of insulating collinear magnetism is derived first in terms of spin-polarized Wannier functions then recast as a Berry phase. We propose an extension to the general, non-collinear case which we implement computationally in the Wannier function form and use to calculate the magnetoelectric monopolizations of LiMnPO$_4$ and Cr$_2$O$_3$. We find that, while the former is well approximated by a summation over the formal local spin moments, the latter shows significant deviations from this approximation. We suggest that equating the Berry phase value with a sum over local moments provides an unambiguous route to defining the size of the local magnetic moment in magnetoelectric antiferromagnets containing only one type of magnetic ion.

cond-mat.mtrl-sci

The magnetic field generated by a charge in a uniaxial magnetoelectric material

We revisit the description of the magnetic field around antiferromagnetic magnetoelectrics in the context of recent developments regarding magnetoelectric monopoles. Using Maxwell's equations, we calculate the magnetic and electric fields associated with a free charge in a bulk uniaxial magnetoelectric, as well as in a finite sphere of magnetoelectric material. We show that a charge in the prototypical magnetoelectric Cr$_2$O$_3$, which is uniaxial with a diagonal magnetoelectric response, induces an internal magnetic field with both monopolar and quadrupolar components, but that only the quadrupolar contribution extends beyond the sample surface. We discuss the behavior of the external quadrupolar field and compare its magnitude to those of magnetic fields from other sources.

cond-mat.mtrl-sci

The macroscopic monopolization in diagonal magnetoelectrics

We develop the formalism of the macroscopic monopolization -- that is the monopole moment per unit volume -- in periodic solids, and discuss its relationship to the diagonal magnetoelectric effect. For the series of lithium transition metal phosphate compounds we use first-principles density functional theory to calculate the contributions to the macroscopic monopolization from the global distribution of magnetic moments within the unit cell, as well as from the distribution of magnetization around the atomic sites. We find one example within the series (LiMnPO$_4$) that shows a macroscopic monopolization corresponding to a ferromonopolar ordering consistent with its diagonal magnetoelectric response. The other members of the series (LiMPO$_4$, with M = Co, Fe and Ni) have zero net monopolization but have antiferromonopolar orderings that should lead to $q$-dependent diagonal magnetoelectric effects

cond-mat.str-el

Linear Magnetoelectric Effect by Orbital Magnetism

We use symmetry analysis and first principles calculations to show that the linear magnetoelectric effect can originate from the response of orbital magnetic moments to the polar distortions induced by an applied electric field. Using LiFePO4 as a model compound we show that spin-orbit coupling partially lifts the quenching of the 3d orbitals and causes small orbital magnetic moments ($μ_{(L)}\approx 0.3 μ_B$) parallel to the spins of the Fe$^{2+}$ ions. An applied electric field $\mathbf{E}$ modifies the size of these orbital magnetic moments inducing a net magnetization linear in $\mathbf{E}$.

cond-mat.mtrl-sci

Effect of interfacial Cr on magnetoelectricity of Fe2/CrO2/BaTiO3(001)

On the basis of first-principles calculations we study the effect of interfacial Cr on the magnetoelectric properties of a composite multiferroic Fe_L/BaTiO_3(001), with the Fe thickness L=1,2 monolayers. The use of the CrO_2-terminated interface instead of TiO_2 may significantly enhance magnetoelectricity in the system, showing an unexpected change in magnetization induced by the electric polarization reversal. In the case of L=2, for instance, the magnetic order of the Fe bilayer can be switched from nearly zero ferrimagnetic to ferromagnetic upon polarization reversal.

cond-mat.mtrl-sci