arXiv subjects

Giacomo Coslovich

Publications and source records attributed to Giacomo Coslovich.

At least 19 recordsLinked to original sources

arXiv2026

The chemRIXS Instrument for the LCLS-II X-Ray Free Electron Laser

The chemRIXS instrument at the Linac Coherent Light Source offers new opportunities for studying solution-phase systems with time-resolved soft X-ray spectroscopy through the recently commissioned high-repetition-rate LCLS-II X-ray free electron laser. The orders-of-magnitude X-ray flux improvement provided by the superconducting accelerator, combined with corresponding advances in the optical laser system and the liquid jet recirculation system, enables studies on dilute systems with high signal-to-noise compared to what was possible with the LCLS-I copper accelerator. These capabilities open up time-resolved X-ray absorption spectroscopy and resonant inelastic X-ray scattering to entirely new classes of samples, as well as enabling the development of new soft X-ray spectroscopies on liquid samples. An overview of the beamline components and the first LCLS-II commissioning results are presented.

physics.ins-det↗

arXiv2025

Tracking Electron, Proton, and Solvent Motion in Proton-Coupled Electron Transfer with Ultrafast X-rays

Proton-coupled electron transfer (PCET) is foundational to catalysis, bioenergetics, and energy conversion, yet capturing and disentangling the coupled motions of electrons, protons, and solvent has remained a major experimental challenge. We combine femtosecond optical spectroscopy, site-specific ultrafast soft X-ray absorption spectroscopy, and time-resolved X-ray scattering with advanced calculations to disentangle the elementary steps of PCET in solution. Using a ruthenium polypyridyl model complex, we directly resolve photoinduced electron redistribution, ligand-site protonation within 100 ps, and the accompanying solvent reorganization. This unified multi-modal approach provides an orbital-level, atomistic picture of PCET, showing how electronic, nuclear, and solvation degrees of freedom can be separated experimentally. Our results establish a general X-ray framework for understanding and ultimately controlling PCET in catalysis, artificial photosynthesis, and biological energy flow.

physics.chem-ph↗

arXiv2024

Picosecond expansion in LaAlO3 resonantly driven by infrared-active phonons

We investigate the ultrafast structural dynamics of LaAlO3 thin films driven by short mid-infrared laser pulses at 20 THz. Time-resolved X-ray diffraction reveals an immediate lattice expansion and an acoustic breathing mode of the film. First-principles theory and a spring-mass model identify the direct coupling between coherently driven infrared-active phonons and strain as the underlying mechanism. Time-resolved optical birefringence measurements confirm that the amplitude of this acoustic mode scales linearly with the pump fluence, which agrees with the theory. Furthermore, time-resolved X-ray diffuse scattering indicates that THz excitation enhances crystallinity by inducing a non-thermal increase in structural symmetry originating from preexisting defects. These findings highlight the potential of a multimodal approach-combining time-resolved X-ray and optical measurements and first-principles theory-to elucidate and control structural dynamics in nanoscale materials.

cond-mat.mtrl-sci↗

arXiv2023

Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La$_{1.65}$Eu$_{0.2}$Sr$_{0.15}$CuO$_4$

Understanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump-probe time-resolved resonant x-ray scattering on the (0 0 1) Bragg peak at the Cu $L_3$ and O $K$ resonances, we investigate non-equilibrium dynamics of $Q_a = Q_b = 0$ nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La$_{1.65}$Eu$_{0.2}$Sr$_{0.15}$CuO$_4$. The orbital selectivity of the resonant x-ray scattering cross-section allows nematicity dynamics associated with the planar O 2$p$ and Cu 3$d$ states to be distinguished from the response of anisotropic lattice distortions. A direct time-domain comparison of CDW translational-symmetry breaking and nematic rotational-symmetry breaking reveals that these broken symmetries remain closely linked in the photoexcited state, consistent with the stability of CDW topological defects in the investigated pump fluence regime.

cond-mat.str-el↗

arXiv2022

Ultrafast perturbation of magnetic domains by optical pumping in a ferromagnetic multilayer

Ultrafast optical pumping of spatially nonuniform magnetic textures is known to induce far-from-equilibrium spin transport effects. Here, we use ultrafast x-ray diffraction with unprecedented dynamic range to study the laser-induced dynamics of labyrinth domain networks in ferromagnetic CoFe/Ni multilayers. We detected azimuthally isotropic, odd order, magnetic diffraction rings up to 5th order. The amplitudes of all three diffraction rings quench to different degrees within 1.6 ps. In addition, all three of the detected diffraction rings both broaden by 15% and radially contract by 6% during the quench process. We are able to rigorously quantify a 31% ultrafast broadening of the domain walls via Fourier analysis of the order-dependent quenching of the three detected diffraction rings. The broadening of the diffraction rings is interpreted as a reduction in the domain coherence length, but the shift in the ring radius, while unambiguous in its occurrence, remains unexplained. In particular, we demonstrate that a radial shift explained by domain wall broadening can be ruled out. With the unprecedented dynamic range of our data, our results provide convincing evidence that labyrinth domain structures are spatially perturbed at ultrafast speeds under far-from-equilibrium conditions, albeit the mechanism inducing the perturbations remains yet to be clarified.

cond-mat.mes-hall↗

arXiv2021

State-resolved ultrafast charge and spin dynamics in [Co/Pd] multilayers

We use transient absorption spectroscopy with circularly polarized x-rays to detect laser-excited hole states below the Fermi level and compare their dynamics with that of unoccupied states above the Fermi level in ferromagnetic [Co/Pd] multilayers. While below the Fermi level an instantaneous and significantly stronger demagnetization is observed, above the Fermi level the demagnetization is delayed by 35+/-10 fs. This provides a direct visualization of how ultrafast demagnetization proceeds via initial spin-flip scattering of laser-excited holes to the subsequent formation of spin waves.

cond-mat.mtrl-sci↗

arXiv2020

Transient Resonant Auger-Meitner Spectra of Photoexcited Thymine

We present the first investigation of excited state dynamics by resonant Auger-Meitner spectroscopy (also known as resonant Auger spectroscopy) using the nucleobase thymine as an example. Thymine is photoexcited in the UV and probed with X-ray photon energies at and below the oxygen K-edge. After initial photoexcitation to a ππ* excited state, thymine is known to undergo internal conversion to an nπ* excited state with a strong resonance at the oxygen K-edge, red-shifted from the ground state π* resonances of thymine (see our previous study Wolf et al., Nat. Commun., 2017, 8, 29). We resolve and compare the Auger-Meitner electron spectra associated both with the excited state and ground state resonances, and distinguish participator and spectator decay contributions. Furthermore, we observe simultaneously with the decay of the nπ* state signatures the appearance of additional resonant Auger-Meitner contributions at photon energies between the nπ* state and the ground state resonances. We assign these contributions to population transfer from the nπ* state to a ππ* triplet state via intersystem crossing on the picosecond timescale based on simulations of the X-ray absorption spectra in the vibrationally hot triplet state. Moreover, we identify signatures from the initially excited ππ* singlet state which we have not observed in our previous study.

physics.chem-ph↗

arXiv2019

Evidence for photoinduced sliding of the charge-order condensate in La$_{1.875}$Ba$_{0.125}$CuO$_4$

We use femtosecond resonant soft x-ray scattering to measure the ultrafast optical melting of charge-order correlations in La$_{1.875}$Ba$_{0.125}$CuO$_4$. By analyzing both the energy-resolved and energy-integrated order parameter dynamics, we find evidence of a short-lived nonequilibrium state, whose features are compatible with a sliding charge density wave coherently set in motion by the pump. This transient state exhibits shifts in both the quasielastic line energy and its wave vector, as expected from a classical Doppler effect. The wave vector change is indeed found to directly follow the pump propagation direction. These results demonstrate the existence of sliding charge order behavior in an unconventional charge density wave system and underscore the power of ultrafast optical excitation as a tool to coherently manipulate electronic condensates.

cond-mat.str-el↗

arXiv2019

Orbital dynamics during an ultrafast insulator to metal transition

Phase transitions driven by ultrashort laser pulses have attracted interest both for understanding the fundamental physics of phase transitions and for potential new data storage or device applications. In many cases these transitions involve transient states that are different from those seen in equilibrium. To understand the microscopic properties of these states, it is useful to develop elementally selective probing techniques that operate in the time domain. Here we show fs-time-resolved measurements of V Ledge Resonant Inelastic X-Ray Scattering (RIXS) from the insulating phase of the Mott- Hubbard material V2O3 after ultrafast laser excitation. The probed orbital excitations within the d-shell of the V ion show a sub-ps time response, which evolve at later times to a state that appears electronically indistinguishable from the high-temperature metallic state. Our results demonstrate the potential for RIXS spectroscopy to study the ultrafast orbital dynamics in strongly correlated materials.

cond-mat.str-el↗

arXiv2019

Tunable Isolated Attosecond X-ray Pulses with Gigawatt Peak Power from a Free-Electron Laser

The quantum mechanical motion of electrons in molecules and solids occurs on the sub-femtosecond timescale. Consequently, the study of ultrafast electronic phenomena requires the generation of laser pulses shorter than 1 fs and of sufficient intensity to interact with their target with high probability. Probing these dynamics with atomic-site specificity requires the extension of sub-femtosecond pulses to the soft X-ray spectral region. Here we report the generation of isolated GW-scale soft X-ray attosecond pulses with an X-ray free-electron laser. Our source has a pulse energy that is six orders of magnitude larger than any other source of isolated attosecond pulses in the soft X-ray spectral region, with a peak power in the tens of gigawatts. This unique combination of high intensity, high photon energy and short pulse duration enables the investigation of electron dynamics with X-ray non-linear spectroscopy and single-particle imaging.

physics.optics↗

arXiv2018

Ultrafast time-resolved x-ray scattering reveals diffusive charge order dynamics in La$_{2-x}$Ba$_x$CuO$_4$

Charge order is universal among high-T$_c$ cuprates but its relevance to superconductivity is not established. It is widely believed that, while static order competes with superconductivity, dynamic order may be favorable and even contribute to Cooper pairing. We use time-resolved resonant soft x-ray scattering to study the collective dynamics of the charge order in the prototypical cuprate, La$_{2-x}$Ba$_x$CuO$_4$. We find that, at energy scales $0.4$ meV $ \lesssim ω\lesssim 2$ meV, the excitations are overdamped and propagate via Brownian-like diffusion. At energy scales below 0.4 meV the charge order exhibits dynamic critical scaling, displaying universal behavior arising from propagation of topological defects. Our study implies that charge order is dynamic, so may participate tangibly in superconductivity.

cond-mat.str-el↗

arXiv2017

Ultrafast Dynamics of Vibrational Symmetry Breaking in a Charge-ordered Nickelate

The ability to probe symmetry breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-THz response of the model stripe compound La$_{1.75}$Sr$_{0.25}$NiO$_{4}$, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen - as witnessed by time-delayed suppression of zone-folded Ni-O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. The hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry breaking dynamics in solids.

cond-mat.str-el↗

arXiv2015

Femtosecond X-ray magnetic circular dichroism absorption spectroscopy at an X-ray free electron laser

X-ray magnetic circular dichroism spectroscopy using an X-ray free electron laser is demonstrated with spectra over the Fe L$_{3,2}$-edges. This new ultrafast time-resolved capability is then applied to a fluence-dependent study of all-optical magnetic switching dynamics of Fe and Gd magnetic sublattices in a GdFeCo thin film above its magnetization compensation temperature. At the magnetic switching fuence, we corroborate the existence of a transient ferromagnetic-like state. The timescales of the dynamics, however, are longer than previously observed below the magnetization compensation temperature. Above and below the switching fluence range, we observe secondary demagnetization with about 5 ps timescales. This indicates that the spin thermalization takes longer than 5 ps.

cond-mat.mtrl-sci↗

arXiv2014

Photo-enhanced antinodal conductivity in the pseudogap state of high Tc cuprates

A major challenge in understanding the cuprate superconductors is to clarify the nature of the fundamental electronic correlations that lead to the pseudogap phenomenon. Here we use ultrashort light pulses to prepare a non-thermal distribution of excitations and capture novel properties that are hidden at equilibrium. Using a broadband (0.5-2 eV) probe we are able to track the dynamics of the dielectric function, unveiling an anomalous decrease of the scattering rate of the charge carriers in a pseudogap-like region of the temperature ($T$) and hole-doping ($p$) phase diagram. In this region, delimited by a well-defined $T^*_{neq}(p)$ line, the photo-excitation process triggers the evolution of antinodal excitations from gapped (localized) to delocalized quasi-particles characterized by a longer lifetime. The novel concept of photo-enhanced antinodal conductivity is naturally explained within the single-band Hubbard model, in which the short-range Coulomb repulsion leads to a k-space differentiation between "nodal" quasiparticles and antinodal excitations.

cond-mat.str-el↗

arXiv2013

In search for the pairing glue in cuprates by non-equilibrium optical spectroscopy

In strongly correlated materials the electronic and optical properties are significantly affected by the coupling of fermionic quasiparticles to different degrees of freedom, such as lattice vibrations and bosonic excitations of electronic origin. Broadband ultrafast spectroscopy is emerging as the premier technique to unravel the subtle interplay between quasiparticles and electronic or phononic collective excitations, by their different characteristic timescales and spectral responses. By investigating the femtosecond dynamics of the optical properties of Y-Bi2212 crystals over the 0.5-2 eV energy range, we disentangle the electronic and phononic contributions to the generalized electron-boson Eliashberg function, showing that the spectral distribution of the electronic excitations, such as spin fluctuations and current loops, and the strength of their interaction with quasiparticles can account for the high critical temperature of the superconducting phase transition. Finally, we discuss how the use of this technique can be extended to the underdoped region of the phase diagram of cuprates, in which a pseudogap in the quasiparticle density of states opens. The microscopic modeling of the interaction of ultrashort light pulses with unconventional superconductors will be one of the key challenges of the next-years materials science, eventually leading to the full understanding of the role of the electronic correlations in controlling the dynamics on the femtosecond timescale.

cond-mat.supr-con↗

arXiv2012

Disentangling the electronic and phononic glue in a high-Tc superconductor

Unveiling the nature of the bosonic excitations that mediate the formation of Cooper pairs is a key issue for understanding unconventional superconductivity. A fundamen- tal step toward this goal would be to identify the relative weight of the electronic and phononic contributions to the overall frequency (Ω) dependent bosonic function, Π(Ω). We perform optical spectroscopy on Bi2212 crystals with simultaneous time- and frequency-resolution; this technique allows us to disentangle the electronic and phononic contributions by their different temporal evolution. The strength of the interaction (λ~1.1) with the electronic excitations and their spectral distribution fully account for the high critical temperature of the superconducting phase transition.

cond-mat.supr-con↗

arXiv2011

Revealing the high-energy electronic excitations underlying the onset of high-temperature superconductivity in cuprates

In strongly-correlated systems the electronic properties at the Fermi energy (EF) are intertwined with those at high energy scales. One of the pivotal challenges in the field of high-temperature superconductivity (HTSC) is to understand whether and how the high energy scale physics associated with Mott-like excitations (|E-E$_{F}$|>1 eV) is involved in the condensate formation. Here we show the interplay between the many-body high-energy CuO2 excitations at 1.5 and 2 eV and the onset of HTSC. This is revealed by a novel optical pump supercontinuum-probe technique, which provides access to the dynamics of the dielectric function in Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+δ}$ over an extended energy range, after the photoinduced suppression of the superconducting pairing. These results unveil an unconventional mechanism at the base of HTSC both below and above the optimal hole concentration required to attain the maximum critical temperature (T$_c$).

cond-mat.str-el↗

arXiv2009

Ultrafast insulator-to-metal phase transition as a switch to measure the spectrogram of a supercontinuum light pulse

In this letter we demonstrate the possibility to determine the temporal and spectral structure (spectrogram) of a complex light pulse exploiting the ultrafast switching character of a non-thermal photo-induced phase transition. As a proof, we use a VO2 multi-film, undergoing an ultrafast insulator-to-metal phase transition when excited by femtosecond near-infrared laser pulses. The abrupt variation of the multi-film optical properties, over a broad infrared/visible frequency range, is exploited to determine, in-situ and in a simple way, the spectrogram of a supercontinuum pulse produced by a photonic crystal fiber. The determination of the structure of the pulse is mandatory to develop new pump-probe experiments with frequency resolution over a broad spectral range (700-1100 nm).

physics.optics↗