arXiv subjects

G. Ingold

Publications and source records attributed to G. Ingold.

At least 19 recordsLinked to original sources

arXiv2020

Nonequilibrium Charge-Density-Wave Order Beyond the Thermal Limit

The interaction of many-body systems with intense light pulses may lead to novel emergent phenomena far from equilibrium. Recent discoveries, such as the optical enhancement of the critical temperature in certain superconductors and the photo-stabilization of hidden phases, have turned this field into an important research frontier. Here, we demonstrate nonthermal charge-density-wave (CDW) order at electronic temperatures far greater than the thermodynamic transition temperature. Using time- and angle-resolved photoemission spectroscopy and time-resolved X-ray diffraction, we investigate the electronic and structural order parameters of an ultrafast photoinduced CDW-to-metal transition. Tracking the dynamical CDW recovery as a function of electronic temperature reveals a behaviour markedly different from equilibrium, which we attribute to the suppression of lattice fluctuations in the transient nonthermal phonon distribution. A complete description of the system's coherent and incoherent order-parameter dynamics is given by a time-dependent Ginzburg-Landau framework, providing access to the transient potential energy surfaces.

cond-mat.mtrl-sci↗

arXiv2020

Strain Wave Pathway to Semiconductor-to-Metal Transition revealed by time resolved X-ray powder diffraction

Thanks to the remarkable developments of ultrafast science, one of today's challenges is to modify material state by controlling with a light pulse the coherent motions that connect two different phases. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a macroscopic transformation pathway for the semiconducting-to-metal transition with large volume change in bistable Ti$_3$O$_5$ nanocrystals. Femtosecond powder X-ray diffraction allowed us to quantify the structural deformations associated with the photoinduced phase transition on relevant time scales. We monitored the early intra-cell distortions around absorbing metal dimers, but also long range crystalline deformations dynamically governed by acoustic waves launched at the laser-exposed Ti$_3$O$_5$ surface. We rationalize these observations with a simplified elastic model, demonstrating that a macroscopic transformation occurs concomitantly with the propagating acoustic wavefront on the picosecond timescale, several decades earlier than the subsequent thermal processes governed by heat diffusion.

cond-mat.mtrl-sci↗

arXiv2019

Optical control of vibrational coherence triggered by an ultrafast phase transition

Femtosecond time-resolved x-ray diffraction is employed to study the dynamics of the periodic lattice distortion (PLD) associated with the charge-density-wave (CDW) in K0.3MoO3. Using a multi-pulse scheme we show the ability to extend the lifetime of coherent oscillations of the PLD about the undistorted structure through re-excitation of the electronic states. This suggests that it is possible to enter a regime where the symmetry of the potential energy landscape corresponds to the high symmetry phase but the scattering pathways that lead to the damping of coherent dynamics are still controllable by altering the electronic state population. The demonstrated control over the coherence time offers new routes for manipulation of coherent lattice states.

cond-mat.str-el↗

arXiv2018

Disentangling charge and structural contributions during coherent atomic motions studied by ultrafast resonant x-ray diffraction

We report on the ultrafast dynamics of charge order and structural response during the photoinduced suppression of charge and orbital order in a mixed-valence manganite. Employing femtosecond time-resolved resonant x-ray diffraction below and at the Mn K absorption edge, we present a method to disentangle the transient charge order and structural dynamics in thin films of Pr0.5Ca0.5MnO3. Based on the static resonant scattering spectra, we extract the dispersion correction of charge ordered Mn3+ and Mn4+ ions, allowing us to separate the transient contributions of purely charge order from structural contributions to the scattering amplitude after optical excitation. Our finding of a coherent structural mode at around 2.3 THz, which primarily modulates the lattice, but does not strongly affect the charge order, confirms the picture of the charge order being the driving force of the combined charge, orbital and structural transition.

cond-mat.str-el↗

arXiv2018

Ultrafast relaxation dynamics of the antiferrodistortive phase in Ca doped SrTiO3

The ultrafast dynamics of the octahedral rotation in Ca:SrTiO3 is studied by time resolved x-ray diffraction after photo excitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO3, we observe a ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperaure despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on a slower picosecond timescale is attributed to thermal effects. Time-dependent density-functional-theory calculations show that the fast response can be ascribed to an ultrafast displacive modification of the soft-mode potential towards the normal state, induced by holes created in the oxygen 2p states.

cond-mat.mtrl-sci↗

arXiv2017

The photoinduced transition in magnetoresistive manganites: a comprehensive view

We use femtosecond x-ray diffraction to study the structural response of charge and orbitally ordered Pr$_{1-x}$Ca$_x$MnO$_3$ thin films across a phase transition induced by 800 nm laser pulses. By investigating the dynamics of both superlattice reflections and regular Bragg peaks, we disentangle the different structural contributions and analyze their relevant time-scales. The dynamics of the structural and charge order response are qualitatively different when excited above and below a critical fluence $f_c$. For excitations below $f_c$ the charge order and the superlattice is only partially suppressed and the ground state recovers within a few tens of nanosecond via diffusive cooling. When exciting above the critical fluence the superlattice vanishes within approximately half a picosecond followed by a change of the unit cell parameters on a 10 picoseconds time-scale. At this point all memory from the symmetry breaking is lost and the recovery time increases by many order of magnitudes due to the first order character of the structural phase transition.

cond-mat.str-el↗

arXiv2017

Coupling between a charge density wave and magnetism in an Heusler material

The Prototypical magnetic memory shape alloy Ni$_2$MnGa undergoes various phase transitions as a function of temperature, pressure, and doping. In the low-temperature phases below 260 K, an incommensurate structural modulation occurs along the [110] direction which is thought to arise from softening of a phonon mode. It is not at present clear how this phenomenon is related, if at all, to the magnetic memory effect. Here we report time-resolved measurements which track both the structural and magnetic components of the phase transition from the modulated cubic phase as it is brought into the high-symmetry phase. The results suggest that the photoinduced demagnetization modifies the Fermi surface in regions that couple strongly to the periodicity of the structural modulation through the nesting vector. The amplitude of the periodic lattice distortion, however, appears to be less affected by the demagnetizaton.

cond-mat.str-el↗

arXiv2017

Watching the birth of a charge density wave order: diffraction study on nanometer-and picosecond-scales

Femtosecond time-resolved X-ray diffraction is used to study a photo-induced phase transition between two charge density wave (CDW) states in 1T-TaS$_2$, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photo-induced I-CDW phase then develops through a nucleation/growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a non-conservative order parameter.

cond-mat.str-el↗

arXiv2016

Ultrafast x-ray diffraction of a ferroelectric soft mode driven by broadband terahertz pulses

Intense, few-cycle pulses in the terahertz frequency range have strong potential for schemes of control over vibrational modes in solid-state materials in the electronic ground-state. Here we report an experiment using single cycle terahertz pulses to directly excite lattice vibrations in the ferroelectric material $\mathrm{Sn_2P_2S_6}$ and ultrafast x-ray diffraction to quantify the resulting structural dynamics. A model of a damped harmonic oscillator driven by the transient electric field of the terahertz pulses describes well the movement of the Sn$^{2+}$ ion along the ferroelectric soft mode. Finally, we describe an anharmonic extension of this model which predicts coherent switching of domains at peak THz-frequency fields of 790 kV/cm.

cond-mat.mtrl-sci↗

arXiv2015

Ultrafast Laser-Induced Melting of Long-Range Magnetic Order in Multiferroic TbMnO3

We performed ultrafast time-resolved near-infrared pump, resonant soft X-ray diffraction probe measurements to investigate the coupling between the photoexcited electronic system and the spin cycloid magnetic order in multiferroic TbMnO3 at low temperatures. We observe melting of the long range antiferromagnetic order at low excitation fluences with a decay time constant of 22.3 +- 1.1 ps, which is much slower than the ~1 ps melting times previously observed in other systems. To explain the data we propose a simple model of the melting process where the pump laser pulse directly excites the electronic system, which then leads to an increase in the effective temperature of the spin system via a slower relaxation mechanism. Despite this apparent increase in the effective spin temperature, we do not observe changes in the wavevector q of the antiferromagnetic spin order that would typically correlate with an increase in temperature under equilibrium conditions. We suggest that this behavior results from the extremely low magnon group velocity that hinders a change in the spin-spiral wavevector on these time scales.

cond-mat.str-el↗

arXiv2014

Ultrafast structural dynamics of the Fe-pnictide parent compound BaFe2As2

Using femtosecond time-resolved x-ray diffraction we investigate the structural dynamics of the coherently excited A1g phonon mode in the Fe-pnictide parent compound BaFe2As2. The fluence dependent intensity oscillations of two specific Bragg reflections with distinctly different sensitivity to the pnictogen height in the compound allow us to quantify the coherent modifications of the Fe-As tetrahedra, indicating a transient increase of the Fe magnetic moments. By a comparison with time-resolved photoemission data we derive the electron-phonon deformation potential for this particular mode. The value of Delta mu/Delta z = -(1.0 - 1.5) eV/A is comparable with theoretical predictions and demonstrates the importance of this degree of freedom for the electron-phonon coupling in the Fe pnictides.

cond-mat.supr-con↗

arXiv2014

Structural and Magnetic Dynamics in the Magnetic Shape Memory Alloy Ni$_2$MnGa

Magnetic shape memory Heusler alloys are multiferroics stabilized by the correlations between electronic, magnetic and structural order. To study these correlations we use time resolved x-ray diffraction and magneto-optical Kerr effect experiments to measure the laser induced dynamics in a Heusler alloy Ni$_2$MnGa film and reveal a set of timescales intrinsic to the system. We observe a coherent phonon which we identify as the amplitudon of the modulated structure and an ultrafast phase transition leading to a quenching of the incommensurate modulation within 300~fs with a recovery time of a few ps. The thermally driven martensitic transition to the high temperature cubic phase proceeds via nucleation within a few ps and domain growth limited by the speed of sound. The demagnetization time is 320~fs, which is comparable to the quenching of the structural modulation.

cond-mat.mtrl-sci↗

arXiv2014

Temperature-dependent electron-phonon coupling in La$_{2-x}$Sr$_x$CuO$_4$ probed by femtosecond X-ray diffraction

The strength of the electron-phonon coupling parameter and its evolution throughout a solid's phase diagram often determines phenomena such as superconductivity, charge- and spin-density waves. Its experimental determination relies on the ability to distinguish thermally activated phonons from those emitted by conduction band electrons, which can be achieved in an elegant way by ultrafast techniques. Separating the electronic from the out-of-equilibrium lattice subsystems, we probed their re-equilibration by monitoring the transient lattice temperature through femtosecond X-ray diffraction in La$_{2-x}$Sr$_x$CuO$_4$ single crystals with $x$=0.1 and 0.21. The temperature dependence of the electron-phonon coupling is obtained experimentally and shows similar trends to what is expected from the \textit{ab-initio} calculated shape of the electronic density-of-states near the Fermi energy. This study evidences the important role of band effects in the electron-lattice interaction in solids, in particular in superconductors.

cond-mat.supr-con↗

arXiv2013

Identification of coherent lattice modulations coupled to charge and orbital order in a manganite

We apply grazing-incidence femtosecond x-ray diffraction to investigate the details of the atomic motion connected with a displacively excited coherent optical phonon. We concentrate on the low frequency phonon associated with the charge and orbital order in the mixed valence manganite La0.25Pr0.375Ca0.375MnO3 for T < 210 K. We measure the response of three superlattice reflections that feature different sensitivities to the motion of the unit cell constituents. The results support the assignment to a translational mode of the Mn4+ atoms together with the oxygen atoms connecting adjacent Mn4+ sites.

cond-mat.str-el↗

arXiv2013

Imaging the antiferromagnetic to ferromagnetic first order phase transition of FeRh

The antiferromagnetic (AFM) to ferromagnetic (FM) first order phase transition of an epitaxial FeRh thin-film has been studied with x-ray magnetic circular dichroism using photoemission electron microscopy. The FM phase is magnetized in-plane due to shape anisotropy, but the magnetocrystalline anisotropy is negligible and there is no preferred in-plane magnetization direction. When heating through the AFM to FM phase transition the nucleation of the FM phase occurs at many independent nucleation sites with random domain orientation. The domains subsequently align to form the final FM domain structure. We observe no pinning of the FM domain structure.

cond-mat.mtrl-sci↗

arXiv2012

Direct observation of non-fully-symmetric coherent optical phonons by femtosecond x-ray diffraction

We directly measure by femtosecond time-resolved x-ray diffraction the E$_g$ symmetry coherent phonon excited in bismuth by strong optical excitation. The magnitude of the E$_g$ mode observed is 0.2 pm peak-to-peak, compared against the 2.7 pm initial displacement of the fully-symmetric A$_{1g}$ mode. The much smaller motion of the E$_g$ mode is a consequence of the short lifetime of the electronic states that drive the atomic motion. The experimentally measured magnitude of the E$_g$ motion allows us to rule out a previously suggested scenario for explaining the dynamics in bismuth that relies on strong coupling between these modes.

cond-mat.mtrl-sci↗

arXiv2012

Coherent phonon dynamics at the martensitic phase transition of Ni_2MnGa

We use time-resolved optical reflectivity to study the laser stimulated dynamics in the magnetic shape memory alloy Ni_2MnGa. We observe two coherent optical phonons, at 1.2 THz in the martensite phase and at 0.7 THz in the pre-martensite phase, which we interpret as a zone-folded acoustic phonon and a heavily damped amplitudon respectively. In the martensite phase the martensitic phase transition can be induced by a fs laser pulse on a timescale of a few ps.

cond-mat.mtrl-sci↗

arXiv2012

Structural and magnetic dynamics of a laser induced phase transition in FeRh

We use time-resolved x-ray diffraction and magnetic optical Kerr effect to study the laser induced antiferromagnetic to ferromagnetic phase transition in FeRh. The structural response is given by the nucleation of independent ferromagnetic domains (τ_1 ~ 30ps). This is significantly faster than the magnetic response (τ_2 ~ 60ps) given by the subsequent domain realignment. X-ray diffraction shows that the two phases co-exist on short time-scales and that the phase transition is limited by the speed of sound. A nucleation model describing both the structural and magnetic dynamics is presented.

cond-mat.mtrl-sci↗