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

A dynamical stability limit for the charge density wave in K0.3MoO3

We study the response of the one-dimensional charge density wave in K0.3MoO3 to different types of excitation with femtosecond optical pulses. We compare the response to direct excitation of the lattice at mid-infrared frequencies with that to the injection of quasi-particles across the low-energy charge density wave gap and to charge transfer excitations in the near infrared. For all three cases, we observe a fluence threshold above which the amplitude-mode oscillation frequency is softened and the mode becomes increasingly damped. We show that all the data can be collapsed onto a universal curve in which the melting of the charge density wave occurs abruptly at a critical lattice excursion. These data highlight the existence of a universal stability limit for a charge density wave, reminiscent of the empirical Lindemann criterion for the stability of a crystal lattice

Non-equilibrium control of complex solids by nonlinear phononics

We review some recent advances in the use of optical fields at terahertz frequencies to drive the lattice of complex materials. We will focus on the control of low energy collective properties of solids, which emerge on average when a high frequency vibration is driven and a new crystal structure induced. We first discuss the fundamentals of these lattice rearrangements, based on how anharmonic mode coupling transforms an oscillatory motion into a quasi-static deformation of the crystal structure. We then discuss experiments, in which selectively changing a bond angle turns an insulator into a metal, accompanied by changes in charge, orbital and magnetic order. We then address the case of light induced non-equilibrium superconductivity, a mysterious phenomenon observed in some cuprates and molecular materials when certain lattice vibrations are driven. Finally, we show that the dynamics of electronic and magnetic phase transitions in complex-oxide heterostructures follow distinctly new physical pathways in case of the resonant excitation of a substrate vibrational mode

New insights into correlated materials in the time domain—combining far-infrared excitation with x-ray probes at cryogenic temperatures

Modern techniques for the investigation of correlated materials in the time domain combine selective excitation in the THz frequency range with selective probing of coupled structural, electronic and magnetic degrees of freedom using x-ray scattering techniques. Cryogenic sample temperatures are commonly required to prevent thermal occupation of the low energy modes and to access relevant material ground states. Here, we present a chamber optimized for high-field THz excitation and (resonant) x-ray diffraction at sample temperatures between 5 and 500 K. Directly connected to the beamline vacuum and featuring both a Beryllium window and an in-vacuum detector, the chamber covers the full (2–12.7) keV energy range of the femtosecond x-ray pulses available at the Bernina endstation of the SwissFEL free electron laser. Successful commissioning experiments made use of the energy tunability to selectively track the dynamics of the structural, magnetic and orbital order of Ca2RuO4 and Tb2Ti2O7 at the Ru (2.96 keV) and Tb (7.55 keV) L-edges, respectively. THz field amplitudes up to 1.12 MV cm−1 peak field were demonstrated and used to excite the samples at temperatures as low as 5 K.ISSN:0953-8984ISSN:1361-648

Strong modulation of carrier effective mass in WTe2 via coherent lattice manipulation

The layered transition-metal dichalcogenide WTe2 is characterized by distinctive transport and topological properties. These properties are largely determined by electronic states close to the Fermi level, specifically to electron and hole pockets in the Fermi sea. In principle, these states can be manipulated by changes to the crystal structure. The precise impact of particular structural changes on the electronic properties is a strong function of the specific nature of the atomic displacements. Here, we report on time-resolved X-ray diffraction and infrared reflectivity measurements of the coherent structural dynamics in WTe2 induced by femtosecond laser pulses excitation (central wavelength 800 nm), with emphasis on a quantitative description of both in-plane and out-of-plane vibrational modes. We estimate the magnitude of these motions, and calculate via density functional theory their effect on the electronic structure. Based on these results, we predict that phonons periodically modulate the effective mass of carriers in the electron and hole pockets up to 20%. This work opens up new opportunities for modulating the peculiar transport properties of WTe2 on short time scales.ISSN:2397-713

Optical second harmonic generation in LiB3O5 modulated by intense femtosecond X-ray pulses

ISSN:1094-408

A setup for hard x-ray time-resolved resonant inelastic x-ray scattering at SwissFEL

We present a new setup for resonant inelastic hard x-ray scattering at the Bernina beamline of SwissFEL with energy, momentum, and temporal resolution. The compact R = 0.5 m Johann-type spectrometer can be equipped with up to three crystal analyzers and allows efficient collection of RIXS spectra. Optical pumping for time-resolved studies can be realized with a broad span of optical wavelengths. We demonstrate the performance of the setup at an overall ∼180 meV resolution in a study of ground-state and photoexcited (at 400 nm) honeycomb 5d iridate α-Li2IrO3. Steady-state RIXS spectra at the iridium L3-edge (11.214 keV) have been collected and are in very good agreement with data collected at synchrotrons. The time-resolved RIXS transients exhibit changes in the energy loss region <2 eV, whose features mostly result from the hopping nature of 5d electrons in the honeycomb lattice. These changes are ascribed to modulations of the Ir-to-Ir inter-site transition scattering efficiency, which we associate to a transient screening of the on-site Coulomb interaction

Non-equilibrium dynamics of spin-lattice coupling

Quantifying the dynamics of normal modes and how they interact with other excitations is of central importance in condensed matter. Spin-lattice coupling is relevant to several sub-fields of condensed matter physics; examples include spintronics, high-Tc superconductivity, and topological materials. However, experimental approaches that can directly measure it are rare and incomplete. Here we use time-resolved X-ray diffraction to directly access the ultrafast motion of atoms and spins following the coherent excitation of an electromagnon in a multiferroic hexaferrite. One striking outcome is the different phase shifts relative to the driving field of the two different components. This phase shift provides insight into the excitation process of such a coupled mode. This direct observation of combined lattice and magnetization dynamics paves the way to access the mode-selective spin-lattice coupling strength, which remains a missing fundamental parameter for ultrafast control of magnetism and is relevant to a wide variety of materials.ISSN:2041-172

Anomalous temperature dependence of the experimental x-ray structure factor of supercooled water

The structural changes of water upon deep supercooling were studied through wide-angle x-ray scattering at SwissFEL. The experimental setup had a momentum transfer range of 4.5 angstrom(-1), which covered the principal doublet of the x-ray structure factor of water. The oxygen-oxygen structure factor was obtained for temperatures down to 228.5 +/- 0.6 K. Similar to previous studies, the second diffraction peak increased strongly in amplitude as the structural change accelerated toward a local tetrahedral structure upon deep supercooling. We also observed an anomalous trend for the second peak position of the oxygen-oxygen structure factor (q(2)). We found that q(2) exhibits an unprecedented positive partial derivative with respect to temperature for temperatures below 236 K. Based on Fourier inversion of our experimental data combined with reference data, we propose that the anomalous q(2) shift originates from that a repeat spacing in the tetrahedral network, associated with all peaks in the oxygen-oxygen pair-correlation function, gives rise to a less dense local ordering that resembles that of low-density amorphous ice. The findings are consistent with that liquid water consists of a pentamer-based hydrogen-bonded network with low density upon deep supercooling. (C) 2021 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).11Ysciescopu

Enhancement and maximum in the isobaric specific-heat capacity measurements of deeply supercooled water using ultrafast calorimetry

Knowledge of the temperature dependence of the isobaric specific heat (Cp) upon deep supercooling can give insights regarding the anomalous properties of water. If a maximum in Cp exists at a specific temperature, as in the isothermal compressibility, it would further validate the liquid-liquid critical point model that can explain the anomalous increase in thermodynamic response functions. The challenge is that the relevant temperature range falls in the region where ice crystallization becomes rapid, which has previously excluded experiments. Here, we have utilized a methodology of ultrafast calorimetry by determining the temperature jump from femtosecond X-ray pulses after heating with an infrared laser pulse and with a sufficiently long time delay between the pulses to allow measurements at constant pressure. Evaporative cooling of ∼15-μm diameter droplets in vacuum enabled us to reach a temperature down to ∼228 K with a small fraction of the droplets remaining unfrozen. We observed a sharp increase in Cp, from 88 J/mol/K at 244 K to about 218 J/mol/K at 229 K where a maximum is seen. The Cp maximum is at a similar temperature as the maxima of the isothermal compressibility and correlation length. From the Cp measurement, we estimated the excess entropy and self-diffusion coefficient of water and these properties decrease rapidly below 235 K.QC 20220317</p