arXiv subjects

Christopher Arrell

Publications and source records attributed to Christopher Arrell.

10 recordsLinked to original sources

arXiv2026

High-Power Polarization-Controlled Attosecond-Scale Soft X-ray Pulses

We demonstrate a versatile platform for high-power attosecond soft X-ray pulse generation with polarization and photon energy control at the SwissFEL free-electron laser. An isolated high-current spike embedded within a long electron-beam pedestal emits soft X-ray pulses with single-spike spectra and multi-electronvolt bandwidths in the tunable magnetic fields of Apple-X undulators. Demonstrated pulse parameters include a photon energy range of 450--1070 eV, circular as well as linear polarization, and pulse energies from tens to above hundred microjoules. By tuning the longitudinal slice-dependent transverse electron beam orbit we can rapidly switch between attosecond and few femtosecond pulse length. By exploiting magnetic chicanes in the undulator line we can produce two-colour pulse pairs with tunable delay or increase the pulse energy beyond 200~\textmu J through multi-stage amplification schemes. High-resolution longitudinal phase-space measurements and start-to-end simulations in addition to spectral measurements provide consistent evidence for attosecond-scale pulse durations. This unique combination of high pulse energy and polarization control of attosecond-scale soft X-ray pulses enables the element-specific investigations of spin and chiral dynamics on the natural time scale of electron motion.

physics.acc-ph↗

arXiv2026

Emergent Antiphase Stacking in a Transient Charge Density Wave

Photoexcitation can induce novel states in materials that are inaccessible in equilibrium, a recent example being the light-induced charge density wave (CDW) observed in $\text{LaTe}_3$. Here, we investigate this transient CDW using infrared-pump x-ray-probe scattering at a free-electron laser, with high momentum and time resolution. We find that the transient CDW Bragg peak is broad in reciprocal space, indicating a highly disordered state. The ordering wavevector of the transient state is different from the equilibrium orders that develop in this class of materials - the transient peak appears near (2/7, 0, 0) reciprocal lattice units, whereas the equilibrium $a$ order and $c$ order occur at $\approx (5/7, 0, 0)$ and $(0, 0, 2/7)$, respectively. The transient CDW is therefore distinct from the equilibrium $a$ order, differing in the relative phase of the CDW displacement between the two equivalent nearly-square Te-Te nets in the conventional unit cell. Our work highlights how photoexcitation can access states with no equilibrium analog, and how x-ray scattering can provide microscopic insight into such elusive phases.

cond-mat.str-el↗

arXiv2026

Ultrafast Decoherence of Charge Density Waves in K$_{0.3}$MoO$_{3}$

Recent works have suggested that transient suppression of a charge density wave (CDW) by an ultra-short excitation can lead to an inversion of the CDW phase. We experimentally investigate the dynamics of the CDW in K$_{0.3}$MoO$_{3}$ by time resolved x-ray diffraction after excitation with optical pulses. Our results indicate a transient inversion of the CDW phase close to the surface that evolves into a highly disordered state in less than one picosecond. Numerical simulations solving the Ginzburg-Landau equation including disorder from strong pinning defects reproduce our main observations. Our findings highlight the critical role of disorder in schemes for coherent control in condensed matter systems.

cond-mat.str-el↗

arXiv2023

Dynamical Scaling Reveals Topological Defects and Anomalous Evolution of a Photoinduced Phase Transition

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic lengthscales. Our results provide direct evidence that ultrafast excitation of LaTe$_3$ leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

cond-mat.mtrl-sci↗

arXiv2021

Hard X-ray Transient Grating Spectroscopy on Bismuth Germanate

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods.

physics.optics↗

arXiv2020

Ultrafast electron localization in a correlated metal

Ultrafast electron delocalization induced by a fs laser pulse is a well-known process and is the initial step for important applications such as fragmentation of molecules or laser ablation in solids. It is well understood that an intense fs laser pulse can remove several electrons from an atom within its pulse duration. [1] However, the speed of electron localization out of an electron gas, the capture of an electron by ion, is unknown. Here, we demonstrate that electronic localization out of the conduction band can occur within only a few hundred femtoseconds. This ultrafast electron localization into 4f states has been directly quantified by transient x-ray absorption spectroscopy following photo-excitation of a Eu based correlated metal with a fs laser pulse. Our x-ray experiments show that the driving force for this process is either an ultrafast reduction of the energy of the 4f states, a change of their bandwidth or an increase of the hybridization between the 4f and the 3d states. The observed ultrafast electron localization process raises further basic questions for our understanding of electron correlations and their coupling to the lattice.

cond-mat.str-el↗

arXiv2016

A Versatile Setup for Ultrafast Broadband Optical Spectroscopy of Coherent Collective Modes in Strongly Correlated Quantum Systems

A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide range of temperatures. By combining a temporal resolution of 45 fs and a broad detection range between 1.75 and 2.85 eV, this apparatus can provide insightful information on the interplay between coherent collective modes and high-energy electronic excitations, which is one of the distinctive characteristics of strongly interacting and correlated quantum systems. The use of a single-shot readout CMOS array detector at frame rates up to 10 kHz allows to resolve coherent oscillations with amplitudes below 10$^{-4}$ in $\Delta$R/R. We demonstrate the operation of this setup on the prototypical charge-transfer insulator La$_2$CuO$_4$, revealing the presence of coherent optical phonons with frequencies as high as 13 THz.

physics.ins-det↗

arXiv2015

Clocking the Onset of Bilayer Coherence in a High-$\mathrm{T_C}$ Cuprate

In cuprates, a precursor state of superconductivity is speculated to exist above the critical temperature $\mathrm{T_C}$. Here we show via a combination of far-infrared ellipsometry and ultrafast broadband optical spectroscopy that signatures of such a state can be obtained via three independent observables in an underdoped sample of NdBa$_2$Cu$_3$O$_{6+\delta}$. The pseudogap correlations were disentangled from the response of laser-broken pairs by clocking their characteristic time-scales. The onset of a superconducting precursor state was found at a temperature $\mathrm{T_{ONS}}$ $>$ $\mathrm{T_C}$, consistent with the temperature scale identified via static optical spectroscopy. Furthermore, the temperature evolution of the coherent vibration of the Ba ion, strongly renormalized by the onset of superconductivity, revealed a pronounced anomaly at the same temperature $\mathrm{T_{ONS}}$. The microscopic nature of such a precursor state is discussed in terms of pre-formed pairs and enhanced bilayer coherence.

cond-mat.supr-con↗

arXiv2015

Coherent generation of symmetry-forbidden phonons by light-induced electron-phonon interactions in magnetite

Symmetry breaking across phase transitions often causes changes in selection rules and emergence of optical modes which can be detected via spectroscopic techniques or generated coherently in pump-probe experiments. In second-order or weakly first-order transitions, fluctuations of the order parameter are present above the ordering temperature, giving rise to intriguing precursor phenomena, such as critical opalescence. Here, we demonstrate that in magnetite (Fe$_3$O$_4$) light excitation couples to the critical fluctuations of the charge order and coherently generates structural modes of the ordered phase above the critical temperature of the Verwey transition. Our findings are obtained by detecting coherent oscillations of the optical constants through ultrafast broadband spectroscopy and analyzing their dependence on temperature. To unveil the coupling between the structural modes and the electronic excitations, at the origin of the Verwey transition, we combine our results from pump-probe experiments with spontaneous Raman scattering data and theoretical calculations of both the phonon dispersion curves and the optical constants. Our methodology represents an effective tool to study the real-time dynamics of critical fluctuations across phase transitions.

cond-mat.mtrl-sci↗

arXiv2015

Probing the electron-phonon interaction in correlated systems with coherent lattice fluctuation spectroscopy

Tailoring the properties of correlated oxides is accomplished by chemical doping, pressure, temperature or magnetic field. Photoexcitation is a valid alternative to reach out-of-equilibrium states otherwise inaccessible. Here, we quantitatively estimate the coupling between a lattice distortion and the charge-transfer excitation in (La$_2$CuO$_{4+\delta}$). We photoinduce a coherent La ion vibration and monitor the response of the optical constants in a broad energy range, providing quantitative information on the electron-phonon matrix element that can be compared to theoretical models. We propose the same methodology to probe electron-electron interactions in other materials.

cond-mat.supr-con↗