arXiv subjects

Samuel W. Teitelbaum

Publications and source records attributed to Samuel W. Teitelbaum.

18 recordsLinked to original sources

arXiv2026

Origins of suppressed self-diffusion of nanoscale constituents of a complex liquid

Understanding and ultimately controlling the transformations and properties of nanoscale systems, from proteins to synthetic nanomaterial assemblies, is limited by the inability to uncover their dynamics on their characteristic length and time scales. Here, we nevertheless demonstrate this ability using MHz X-ray photon correlation spectroscopy (XPCS) -- directly elucidating the characteristic microsecond-dynamics of density fluctuations of semiconductor nanocrystals (NCs), not only in a colloidal dispersion but also in a liquid phase consisting of densely packed, yet mobile, NCs with no long-range order. We find the wavevector-dependent fluctuation rates in the liquid phase are suppressed relative to those in the colloidal phase and relative to observations of densely packed repulsive particles. We show that the suppressed rates are due to a substantial decrease in the self-diffusion of NCs, which we attribute to explicit attractive interactions. Using coarse-grained simulations, we find that the extracted shape and strength of the interparticle potential explains the stability of the liquid phase, in contrast to the gelation observed via XPCS in many other charged colloidal systems. This work opens the door to elucidating fast, condensed phase dynamics in complex fluids and other nanoscale soft matter, such as densely packed proteins and non-equilibrium self-assembly processes, in addition to designing microscopic strategies to avert gelation.

cond-mat.soft↗

arXiv2026

diffpy.morph: Python tools for model independent comparisons between sets of 1D functions

diffpy$.$morph addresses a need to gain scientific insights from 1D scientific spectra in model independent ways. A powerful approach for this is to take differences between pairs of spectra and look for meaningful changes that might indicate underlying chemical, structural, or other modifications. The challenge is that the difference curve may contain uninteresting differences such as experimental inconsistencies and benign physical changes such as the effects of thermal expansion. diffpy$.$morph allows researchers to apply simple transformations, or "morphs", to one of the datasets to remove the unwanted differences revealing, when they are present, non-trivial differences. diffpy$.$morph is an open-source Python package available on the Python Package Index and conda-forge. Here, we describe its functionality and apply it to solve a range of experimental challenges on diffraction and PDF data from x-rays and neutrons, though we note that it may be applied to any 1D function in principle.

physics.comp-ph↗

arXiv2025

Dimensionality reduction of optically generated vortex strings in a charge density wave

In phase transitions, mesoscale structures such as topological defects, vortex strings, and domain walls control the path towards equilibrium, and thus the functional properties of many active devices. In photoinduced phase transitions driven by femtosecond laser excitation, the temporal (pulse duration) and spatial (penetration depth) structure of the optical excitation present opportunities for control and creating structures with unique topologies. By performing time-resolved optical pump, x-ray probe experiments on the CDW system Pd-intercalated ErTe$_{3}$, we gain access to the nanoscale dynamics of the mesoscale topological features (vortex strings) produced after a quench, which have a different apparent dimensionality than the topological defects predicted from the bulk system. We show that these vortex strings persist for much longer than the electronic recovery time. The critical exponent obtained from power-law scaling of the intensity as a function of wavevector shows a reduction in the effective dimensionality of the topological defects in the system, corroborated by time-dependent Ginzburg-Landau simulations. Our results demonstrate a novel pathway to use light to control the dimensionality and orientation of topological defects in quantum materials, which could be used to stabilize competing quantum states.

cond-mat.mes-hall↗

arXiv2025

Enhancing nanoscale charged colloid crystallization near a metastable liquid binodal

Bottom-up assembly of nanocrystals (NCs) into ordered arrays, or superlattices (SLs), is a promising route to design materials with new functionalities, but the degree of control over assembly into functional structures remains challenging. Using electrostatics, rather than density, to tune the interactions between semiconductor NCs, we watch self-assembly proceeding through a metastable liquid phase. We systematically investigate the phase behavior as a function of quench conditions in situ and in real time using small angle X-ray scattering (SAXS). Through quantitative fitting to colloid, liquid, and SL models, we extract the time evolution of each phase and the system phase diagram, which we find to be consistent with short-range attractive interactions. Using the phase diagram's predictive power, we establish control of the self-assembly rate over three orders of magnitude, and identify one- and two-step self-assembly regimes, with only the latter implicating the metastable liquid as an intermediate. Importantly, the presence of the metastable liquid increases SL formation rates relative to the equivalent one-step pathway, and SL order counterintuitively increases with the rate, revealing a highly desirable and generalizable kinetic strategy to promote and enhance ordered assembly.

cond-mat.soft↗

arXiv2025

Characterization of Spatiotemporal Overlap of Femtosecond Lasers and Electron Beam With Ce:YAG Screens

Interactions between short laser pulses and electron bunches determine a wide range of accelerator applications. Finding spatiotemporal overlap between few-micron-sized optical and electron beams is critical, yet there are few routine diagnostics for this purpose. We present a method for achieving spatiotemporal overlap between a picosecond laser pulse and a relativistic sub-ps electron bunch. The method uses the transient change in optical transmission of a Ce:YAG screen upon irradiation with a short electron bunch to co-time the electron and laser beams. We demonstrate and quantify the performance of this method using an inverse Compton source comprised of a 30 MeV electron beam from an X-band linac focused to a 10 $μ$m spot, overlapped with a joule-class picosecond Yb:YAG laser system. This method is applicable to electron beams with few-microjoule bunch energies, and uses standard scintillator screens common in electron accelerators.

physics.acc-ph↗

arXiv2024

In situ coherent X-ray scattering reveals polycrystalline structure and discrete annealing events in strongly-coupled nanocrystal superlattices

Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though the mechanism of annealing remains to be elucidated. Here, we use a combination of Bragg coherent diffractive imaging and X-ray photon correlation spectroscopy to create real-space maps of supercrystalline order along with a real-time view of the strain fluctuations in aging strongly coupled nanocrystal superlattices while they remain suspended and immobilized in solution. By combining the results, we deduce that the self-assembled superstructures are polycrystalline, initially comprising multiple nucleation sites, and that shear avalanches at grain boundaries continue to increase crystallinity long after growth has substantially slowed. This multimodal approach should be generalizable to characterize a breadth of materials in situ in their native chemical environments, thus extending the reach of high-resolution coherent X-ray characterization to the benefit of a much wider range of physical systems.

cond-mat.mtrl-sci↗

arXiv2024

In situ X-ray scattering reveals coarsening rates of superlattices self-assembled from electrostatically stabilized metal nanocrystals depend non-monotonically on driving force

Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with new functionalities. Mechanistic studies are still needed to uncover the design principles for SL self-assembly, but such studies have been difficult to perform due to the fast time- and short length scales of NC systems. To address this challenge, we developed an apparatus to directly measure the evolving phases \textit{in situ} and in real time of an electrostatically stabilized Au NC solution before, during, and after it is quenched to form SLs using small angle X-ray scattering (SAXS). By developing a quantitative model, we fit the time-dependent scattering patterns to obtain the phase diagram of the system and the kinetics of the colloidal and SL phases as a function of varying quench conditions. The extracted phase diagram is consistent with particles whose interactions are short in range relative to their diameter. We find the degree of SL order is primarily determined by fast (sub-second) initial nucleation and growth kinetics, while coarsening at later times depends non-monotonically on the driving force for self-assembly. We validate these results by direct comparison with simulations and use them to suggest dynamic design principles to optimize crystallinity within a finite time window. The combination of this measurement methodology, quantitative analysis, and simulation should be generalizable to elucidate and better control the microscopic self-assembly pathways of a wide range of bottom-up assembled systems and architectures.

cond-mat.soft↗

arXiv2024

Hard X-ray Generation and Detection of Nanometer-Scale Localized Coherent Acoustic Wave Packets in SrTiO$_3$ and KTaO$_3$

We demonstrate that the absorption of femtosecond x-ray pulses can excite quasi-spherical high-wavevector coherent acoustic phonon wavepackets using an all x-ray pump and probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with strain pulses induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the strain wavepacket and the energy absorption efficiency, which are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO$_3$ and KTaO$_3$ single crystals, even though there are no nanoscale structures or light-intensity patterns that would ordinarily be required to generate acoustic waves of wavelengths much shorter than the penetration depth. Whereas in GaAs and GaP we do not observe a signal above background. The results provide crucial information on x-ray matter interactions, which sheds light on the mechanism of x-ray energy deposition, and the study of high wavevector acoustic phonons and thermal transport at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2023

Ultrafast measurements of mode-specific deformation potentials of Bi$_2$Te$_3$ and Bi$_2$Se$_3$

Quantifying electron-phonon interactions for the surface states of topological materials can provide key insights into surface-state transport, topological superconductivity, and potentially how to manipulate the surface state using a structural degree of freedom. We perform time-resolved x-ray diffraction (XRD) and angle-resolved photoemission (ARPES) measurements on Bi$_2$Te$_3$ and Bi$_2$Se$_3$, following the excitation of coherent A$_{1g}$ optical phonons. We extract and compare the deformation potentials coupling the surface electronic states to local A$_{1g}$-like displacements in these two materials using the experimentally determined atomic displacements from XRD and electron band shifts from ARPES.We find the coupling in Bi$_2$Te$_3$ and Bi$_2$Se$_3$ to be similar and in general in agreement with expectations from density functional theory. We establish a methodology that quantifies the mode-specific electron-phonon coupling experimentally, allowing detailed comparison to theory. Our results shed light on fundamental processes in topological insulators involving electron-phonon coupling.

cond-mat.mtrl-sci↗

arXiv2022

Ultrafast x-ray scattering reveals composite amplitude collective mode in the Weyl charge density wave material (TaSe$_4$)$_2$I

We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe$_4$)$_2$I following photoexcitation with femtosecond infrared laser pulses. From the time-dependent diffraction signal at the CDW sidebands we identify an amplitude mode derived primarily from the transverse acoustic component of the CDW static distortion. The dynamics of this acoustic amplitude mode are described well by a model of a displacive excitation, which we interpret as mediated through a coupling to the optical phonon component associated with the tetramerization of the Ta chains.

cond-mat.mtrl-sci↗

arXiv2022

Influence of local symmetry on lattice dynamics coupled to topological surface states

We investigate coupled electron-lattice dynamics in the topological insulator Bi2Te3 with time-resolved photoemission and time-resolved x-ray diffraction. It is well established that coherent phonons can be launched by optical excitation, but selection rules generally restrict these modes to zone-center wavevectors and Raman-active branches. We find that the topological surface state couples to additional modes, including a continuum of surface-projected bulk modes from both Raman- and infrared-branches, with possible contributions from surface-localized modes when they exist. Our calculations show that this surface vibrational spectrum occurs naturally as a consequence of the translational and inversion symmetries broken at the surface, without requiring the splitting-off of surface-localized phonon modes. The generality of this result suggests that coherent phonon spectra are useful by providing unique fingerprints for identifying surface states in more controversial materials. These effects may also expand the phase space for tailoring surface state wavefunctions via ultrafast optical excitation.

cond-mat.mtrl-sci↗

arXiv2022

The Persistence of Memory in Ionic Conduction Probed by Nonlinear Optics

Predicting practical rates of ion transport from atomistic descriptors enables the rational design of materials, devices, and processes, which is especially critical to developing low-carbon energy technologies such as rechargeable batteries. The correlated mechanisms of ionic conduction, variation of conductivity with timescale and confinement, and ambiguity in the vibrational origin of translation, the attempt frequency, call for a direct atomic probe of the most fundamental steps of ionic diffusion: ion hops. However, such hops are rare-event large-amplitude translations, and are challenging to excite and detect. Here we use single-cycle terahertz pumps to impulsively trigger ionic hopping in battery solid electrolytes. This is visualized by an induced transient birefringence enabling direct probing of anisotropy in ionic hopping on the picosecond timescale. The relaxation of the transient signal measures the decay of orientational memory, and the production of entropy in diffusion. We extend experimental results using in silico transient birefringence to identify attempt frequencies for ion hopping. Using nonlinear optical methods, we probe ion transport at its fastest limit, distinguish correlated conduction mechanisms from a true random walk at the atomic scale, and demonstrate the connection between activated transport and the thermodynamics of information.

cond-mat.mtrl-sci↗

arXiv2020

Nonlinear resonant X-ray Raman scattering

We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines cease dispersing, turning into orescence lines with energies much greater than obtainable by single electron transitions, and additional Raman lines appear. We attribute these processes to electron-correlation mediated multielectron transitions involving double-core hole excitation and various two-electron de-excitation processes to a final state involving one or more L and M core-holes.

physics.atom-ph↗

arXiv2019

Measurements of Nonequilibrium Interatomic Forces in Photoexcited Bismuth

We determine experimentally the excited-state interatomic forces in photoexcited bismuth. The forces are obtained by a constrained least-squares fit of the excited-state dispersion obtained by femtosecond time-resolved x-ray diffuse scattering to a fifteen-nearest neighbor Born-von Karman model. We find that the observed softening of the zone-center $A_{1g}$ optical mode and transverse acoustic modes with photoexcitation are primarily due to a weakening of three nearest neighbor forces along the bonding direction. This provides a more complete picture of what drives the partial reversal of the Peierls distortion previously observed in photoexcited bismuth.

cond-mat.mtrl-sci↗

arXiv2019

Dynamics of a Persistent Insulator-to-Metal Transition in Strained Manganite Films

Transition metal oxides possess complex free energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained $\mathrm{La_{0.67}Ca_{0.33}MnO_3}$, optical excitation with a sub-100 fs pulse above $2\ \mathrm{mJ/cm^2}$ leads to a persistent metallic phase below 100 K. Using single-shot optical and terahertz spectroscopy, we show that this phase transition is a multi-step process. We conclude that the phase transition is driven by partial charge order melting, followed by growth of the persistent metallic phase on longer timescales. A time-dependent Ginzburg-Landau model can describe the fast dynamics of the reflectivity, followed by longer timescale in-growth of the metallic phase.

cond-mat.str-el↗

arXiv2017

Real-time observation of a coherent lattice transformation into a high-symmetry phase

Excursions far from their equilibrium structures can bring crystalline solids through collective transformations including transitions into new phases that may be transient or long-lived. Direct spectroscopic observation of far-from-equilibrium rearrangements provides fundamental mechanistic insight into chemical and structural transformations, and a potential route to practical applications, including ultrafast optical control over material structure and properties. However, in many cases photoinduced transitions are irreversible or only slowly reversible, or the light fluence required exceeds material damage thresholds. This precludes conventional ultrafast spectroscopy in which optical excitation and probe pulses irradiate the sample many times, each measurement providing information about the sample response at just one probe delay time following excitation, with each measurement at a high repetition rate and with the sample fully recovering its initial state in between measurements. Using a single-shot, real-time measurement method, we were able to observe the photoinduced phase transition from the semimetallic, low-symmetry phase of crystalline bismuth into a high-symmetry phase whose existence at high electronic excitation densities was predicted based on earlier measurements at moderate excitation densities below the damage threshold. Our observations indicate that coherent lattice vibrational motion launched upon photoexcitation with an incident fluence above 10 mJ/cm2 in bulk bismuth brings the lattice structure directly into the high-symmetry configuration for tens of picoseconds, after which carrier relaxation and diffusion restore the equilibrium lattice configuration.

cond-mat.mtrl-sci↗

arXiv2017

Direct Measurement of Anharmonic Decay Channels of a Coherent Phonon

We observe anharmonic decay of the photoexcited coherent A1g phonon in bismuth to points in the Brillouin zone where conservation of momentum and energy are satisfied for three-phonon scattering. The decay of a coherent phonon can be understood as a parametric resonance process whereby the atomic displacement periodically modulates the frequency of a broad continuum of modes. This results in energy transfer through resonant squeezing of the target modes. Using ultrafast diffuse x-ray scattering, we observe build up of coherent oscillations in the target modes driven by this parametric resonance over a wide range of the Brillouin zone. We compare the extracted anharmonic coupling constant to first principles calculations for a representative decay channel.

cond-mat.mtrl-sci↗

arXiv2015

Cooperative photoinduced metastable phase control in strained manganite films

A major challenge in condensed matter physics is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic-lattice coupling that, in turn, stabilize the metallic phase. These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.

cond-mat.str-el↗