arXiv subjects

Michael W. Zuerch

Publications and source records attributed to Michael W. Zuerch.

8 recordsLinked to original sources

arXiv2026

A table-top few-femtosecond broadband extreme-ultraviolet absorption spectrometer with cryogenic cooling

We present a table-top cryogenic ultrafast broadband XUV absorption spectroscopy (c-UBXAS) beamline designed for temperature-dependent and time-resolved investigations of quantum materials. The instrument combines a broadband high-harmonic generation source spanning 22-73 eV with automated image registration and cryogenic sample control down to 20 K, enabling element-specific measurements under both equilibrium and nonequilibrium conditions. The beamline provides sub-50-meV energy resolution and a sub-10-fs instrument response function, while maintaining long-term stability suitable for extended, ultrasensitive measurements. Benchmark experiments on NiI$_2$, a van der Waals multiferroic, reveal temperature-dependent spectral evolution across its magnetic phase transitions, demonstrating the ability to identify element-specific contributions to the ground state and its transient response in the femtosecond regime. This instrument introduces the opportunity to unravel the very first response of a solid-state material during light-matter interaction, paving the way for understanding the complex phase space of nonequilibrium dynamics and emergent states in strongly correlated systems where the few-femtosecond electronic response has eluded most other types of time-resolved techniques.

physics.ins-det↗

arXiv2025

Isostructural electronic transition in MoS$_2$ probed by solid-state high harmonic generation spectroscopy

Studying materials under extreme pressure in diamond anvil cells (DACs) is key to discovering new states of matter, yet no method currently allows the direct measurement of the electronic structure in this environment. Solid-state high harmonic generation (sHHG) offers a new all-optical window into the electronic structure of materials. We demonstrate sHHG spectroscopy inside a DAC by probing $2H$-MoS$_2$, up to 30 GPa, revealing a pressure-induced crossover of the lowest direct bandgap from the $\textbf{K}$-point to the $Γ$-point. This transition manifests as a sharp minimum in harmonic intensity and a 30° rotation of the sHHG polarization anisotropy, despite the absence of a structural phase change. First-principles simulations attribute these features to interference between competing excitation pathways at distinct points in the Brillouin zone. Our results establish sHHG as a sensitive probe of electronic transitions at high pressure, enabling access to quantum phenomena that evade detection by conventional techniques.

cond-mat.mtrl-sci↗

arXiv2025

The dynamical role of optical phonons and sub-lattice screening in a solid-state ion conductor

Solid-state electrolytes (SSEs) require ionic conductivities that are competitive with liquid electrolytes to realize applications in all-solid state batteries. Although numerous materials have been discovered, the underlying mechanisms enabling superionic conduction remain elusive. In particular, the role of ultrafast lattice dynamics in mediating ion migration, which involves couplings between ions, phonons, and electrons, is rarely explored experimentally at their corresponding timescales. To investigate the contributions of coupled lattice dynamics on ion migration, we modulate the charge density occupations within the crystal, and then measure the time-resolved change in impedance on picosecond timescales for a candidate SSE, Li0.5La0.5TiO3. Upon perturbation, we observe enhanced ion migration at ultrafast timescales that are shorter than laser-induced heating. The respective transients match the timescales of optical and acoustic phonon vibrations, suggesting their involvement in ion migration. We further computationally evaluate the effect of a charge transfer from the O 2p to Ti 3d band on the electronic and physical structure of LLTO. We hypothesize that the charge transfer excitation distorts the TiO6 polyhedra by altering the local charge density occupancy of the hopping site at the migration pathway saddle point, thereby causing a reduction in the migration barrier for the Li+ hop, shown using computation. We rule out the contribution of photogenerated electrons and laser heating. Overall, our investigation introduces a new spectroscopic tool to probe fundamental ion hopping mechanisms transiently at ultrafast timescales, which has previously only been achieved in a time-averaged manner or solely via computational methods. Our proposed technique expands our capability to answer dynamical questions previously limited by incumbent spectroscopic strategies.

cond-mat.mtrl-sci↗

arXiv2024

Core-level signature of long-range density-wave order and short-range excitonic correlations probed by attosecond broadband spectroscopy

Advances in attosecond core-level spectroscopies have successfully unlocked the fastest dynamics involving high-energy electrons. Yet, these techniques are not conventionally regarded as an appropriate probe for low-energy quasiparticle interactions that govern the ground state of quantum materials, nor for studying long-range order because of their limited sensitivity to local charge environments. Here, by employing a unique cryogenic attosecond beamline, we identified clear core-level signatures of long-range charge-density-wave (CDW) formation in a quasi-2D excitonic insulator candidate, even though equilibrium photoemission and absorption measurements of the same core levels showed no spectroscopic singularity at the phase transition. Leveraging the high time resolution and intrinsic sensitivity to short-range charge excitations in attosecond core-level absorption, we observed compelling time-domain evidence for excitonic correlations in the normal-state of the material, whose presence has been subjected to a long-standing debate in equilibrium experiments because of interfering phonon fluctuations in a similar part of the phase space. Our findings support the scenario that short-range excitonic fluctuations prelude long-range order formation in the ground state, providing important insights in the mechanism of exciton condensation in a quasi-low-dimensional system. These results further demonstrate the importance of a simultaneous access to long- and short-range order with underlying dynamical processes spanning a multitude of time- and energy-scales, making attosecond spectroscopy an indispensable tool for both understanding the equilibrium phase diagram and for discovering novel, nonequilibrium states in strongly correlated materials.

cond-mat.str-el↗

arXiv2024

Hidden correlations in stochastic photoinduced dynamics of a solid-state electrolyte

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and offering a microscopic view of complex dynamics at the molecular level. The photo response following a laser pulse is, in general, non-identical between multiple exposures due to spatiotemporal fluctuations in a material or the stochastic nature of dynamical pathways. However, most ultrafast experiments using a stroboscopic pump-probe scheme struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing seemingly random deviations from the averaged shot-to-shot response. Leveraging the stability and high photon-flux of time-resolved X-ray micro-diffraction at a synchrotron, we developed a method to quantitatively characterize the shot-to-shot variation of the photoinduced dynamics in a solid-state electrolyte. By analyzing temporal evolutions of the lattice parameter of a single grain in a powder ensemble, we found that the sample responses after different shots contain random fluctuations that are, however, not independent. Instead, there is a correlation between the nonequilibrium lattice trajectories following adjacent laser shots with a characteristic "correlation length" of approximately 1,500 shots, which represents an energy barrier of 0.38~eV for switching the photoinduced pathway, a value interestingly commensurate with the activation energy of lithium ion diffusion. Not only does our nonequilibrium noise correlation spectroscopy provide a new strategy for studying fluctuations that are central to phase transitions in both condensed matter and molecular systems, it also paves the way for discovering hidden correlations and novel metastable states buried in oft-presumed random, uncorrelated fluctuating dynamics.

cond-mat.mtrl-sci↗

arXiv2023

Coherent Phonons in Antimony: an Undergraduate Physical Chemistry Solid-State Ultrafast Laser Spectroscopy Experiment

Ultrafast laser pump-probe spectroscopy is an important and growing field of physical chemistry that allows the measurement of chemical dynamics on their natural timescales, but undergraduate laboratory courses lack examples of such spectroscopy and the interpretation of the dynamics that occur. Here we develop and implement an ultrafast pump probe spectroscopy experiment for the undergraduate physical chemistry laboratory course at the University of California Berkeley. The goal of the experiment is to expose students to concepts in solid-state chemistry and ultrafast spectroscopy via classic coherent phonon dynamics principles developed by researchers over multiple decades. The experiment utilizes a modern high-repetition-rate 800 nm femtosecond Ti:Sapphire laser, split pulses with a variable time delay, and sensitive detection of transient reflectivity signals using the lock-in technique. The experiment involves minimal intervention from students and is therefore easy and safe to implement in the laboratory. Students first perform an intensity autocorrelation measurement on the femtosecond laser pulses to obtain their temporal duration. Then, students measure the pump-probe reflectivity of a single-crystal antimony sample to determine the period of coherent phonon oscillations initiated by an ultrafast pulse excitation, which is analyzed by fitting to a sine wave. Students who completed the experiment in-person obtained good experimental results, and students who took the course remotely due to the COVID-19 pandemic were provided with the data they would have obtained during the experiment to analyze. Evaluation of student written and oral reports reveals that the learning goals were met, and that students gained an appreciation for the field of ultrafast laser-induced chemistry.

physics.ed-ph↗

arXiv2022

Ultrafast formation of topological defects in a 2D charge density wave

Topological defects play a key role in nonequilibrium phase transitions, ranging from birth of the early universe to quantum critical behavior of ultracold atoms. In solids, transient defects are known to generate a variety of hidden orders not accessible in equilibrium, but how defects are formed at the nanometer lengthscale and femtosecond timescale remains unknown. Here, we employ an intense laser pulse to create topological defects in a 2D charge density wave, and track their morphology and dynamics with ultrafast electron diffraction. Leveraging its high temporal resolution and sensitivity in detecting weak diffuse signals, we discover a dual-stage growth of 1D domain walls within 1 ps, a process not dictated by the order parameter amplitude but instead mediated by a nonthermal population of longitudinal optical phonons. Our work provides a framework for ultrafast engineering of topological defects based on selective excitation of collective modes, opening new avenues for dynamical control of nonequilibrium phases in correlated materials.

cond-mat.mtrl-sci↗

arXiv2022

Light-induced dimension crossover in 1T-TiSe$_2$ dictated by excitonic correlations

In low-dimensional systems with strong electronic correlations, the application of an ultrashort laser pulse often yields novel phases that are otherwise inaccessible. The central challenge in understanding such phenomena is to determine how dimensionality and many-body correlations together govern the pathway of a non-adiabatic transition. To this end, we examine a layered compound, 1T-TiSe$_2$, whose three-dimensional charge-density-wave (3D CDW) state also features exciton condensation due to strong electron-hole interactions. We find that photoexcitation suppresses the equilibrium 3D CDW while creating a nonequilibrium 2D CDW. Remarkably, the dimension reduction does not occur unless bound electron-hole pairs are broken. This relation suggests that excitonic correlations maintain the out-of-plane CDW coherence, settling a long-standing debate over their role in the CDW transition. Our findings demonstrate how optical manipulation of electronic interaction enables one to control the dimensionality of a broken-symmetry order, paving the way for realizing other emergent states in strongly correlated systems.

cond-mat.str-el↗