arXiv subjects

Kasra Amini

Publications and source records attributed to Kasra Amini.

At least 19 recordsLinked to original sources

arXiv2026

Frequency-resolved ultrafast electron diffraction: visualizing vibrational dynamics in frequency- and real-space

Ultrafast electron diffraction (UED) provides direct information on changes in molecular structure following photoexcitation, but identifying the individual vibrational motions contributing to these dynamics remains challenging. Here, we introduce frequency-resolved UED, where Fourier transformation of the time-dependent difference pair distribution function ($\Delta$PDF) gives a two-dimensional frequency-distance representation of the structural dynamics. We apply this approach to allene and 1,2-butadiene following photoexcitation to the $S_1(\pi\pi^*)$ state at 200 nm, using electron scattering signals simulated from previously-published ab initio multiple spawning trajectories (S. P. Neville et al., J. Chem. Phys., 2016, 144, 014305). We identify C=C stretching and CCC bending motions and the internuclear distances over which they contribute, and separate overlapping CH$_2$ vibrational motions. By changing the pump-probe delay range used for the Fourier transform, we identify when specific frequency components contribute during the excited-state dynamics. Methyl substitution reduces the C=C stretching and CCC bending frequencies and introduces an additional frequency component in 1,2-butadiene during the first 90 fs. We further show the importance of sub-20-fs, and ultimately few-femtosecond, temporal resolution for retrieving these frequency components. Frequency-resolved UED therefore provides the vibrational frequencies, internuclear distances, and reaction times associated with photoinduced structural dynamics.

physics.chem-ph↗

arXiv2026

Sub-Yield Dynamics in Yield-Stress Materials

The mechanical response of yield-stress materials below the yield point remains a subject of debate. Two of the most widely used constitutive models for these materials offer fundamentally conflicting views: one permits plastic flow at all stress levels, the other assumes entirely recoverable viscoelasticity below yield. Using parallel superposition rheometry, we test the sub-yield behaviour of a microgel and an emulsion. When residual slip effects are properly accounted for, both fluids exhibit bounded, periodic strain responses, offering compelling evidence that they do not flow in the studied regime. Our results indicate that the sub-yield regime is underpinned by nonlinear viscoelasticity and underscore the need for improved constitutive relations that capture such effects without treating yielding as a precursor for nonlinearity.

physics.flu-dyn↗

arXiv2026

Photo-induced non-thermal lattice disorder in aluminium thin-film

We investigate the ultrafast dynamics of photo-induced non-thermal lattice disorder in a polycrystalline aluminium thin film to elucidate transient short- and long-range lattice distortions, their thermalization and electron-phonon coupling timescales. Using a high-repetition-rate 95-keV ultrafast electron diffraction setup (UED), we measured the transient dynamics for the differential scattering signal in a momentum transfer, $q$, range longer than in conventional keV UED setups. Analysis of ten Bragg and six diffuse scattering revealed a prompt increase in the mean-square displacement (MSD), indicating rapid energy transfer from the excited electronic system to the lattice. The subsequent relaxation dynamics of the elastic scattering intensities exhibit a pronounced dependence on diffraction order. Lower-order reflections relax more rapidly, whereas higher-order reflections show significantly slower relaxation or near-plateau behaviour, indicating that lattice equilibration proceeds on multiple $q$-dependent timescales. Exponential fits to the MSD dynamics reveal oscillatory residuals, indicative of coherent non-thermal lattice motion. Power spectral density analysis of these residuals uncovers coherent lattice oscillations with a fundamental frequency of $ω_0 = 0.192$ THz, corresponding to the acoustic breathing (A$_{1g}$) mode of aluminium. Higher frequency components are also observed, consistent with coherent phonon oscillations originating from a single zero-wavevector mode populated by multiple coherent phonons. While individual phonon branches are not directly resolved, the observed dependence on the lattice plane of the relaxation behaviour and oscillatory signatures are consistent with a mode-selective lattice response and non-thermal energy redistribution as described by non-thermal lattice models.

cond-mat.mtrl-sci↗

arXiv2026

High-repetition-rate terahertz and ultraviolet radiation for high-throughput ultrafast electron diffraction

Scaling femtosecond terahertz (THz) and ultraviolet (UV) sources to high repetition rates is essential for high-throughput ultrafast spectroscopy and imaging applications. Yet, their efficient generation at high average power remains limited by thermal effects, phase-matching constraints, and material damage. Here, we demonstrate broadband THz and UV generation driven by a common Yb:KGW laser operating from at 40 - 600 kHz. THz radiation is produced by optical rectification in stoichiometric MgO:LiNbO$_3$ using a line-focus geometry, yielding single-cycle pulses of 55 - 92 nJ energy with peak electric fields of 37 - 90 kV/cm. Electro-optic sampling and beam-quality measurements reveal tunable control between central frequency, bandwidth and field amplitude by translating the generation region transversely within the crystal. Using shorter pump pulses preserves THz conversion efficiency, while longer pulses at 100 kHz reduce THz output by up to a factor of four due to cumulative thermal effects. Femtosecond 257.5 nm UV pulses are generated by cascaded fourth-harmonic generation in $β$-barium borate with conversion efficiencies exceeding 10% at 40 kHz and stable operation up to 600 kHz. These results demonstrate a compact, thermally robust platform for high-average-power nonlinear conversion and are directly relevant to next-generation high-repetition-rate ultrafast electron diffraction and spectroscopy systems.

physics.optics↗

arXiv2025

Local slip length and surfactant effects on liquid-infused surfaces

Robust surfaces capable of reducing flow drag, controlling heat and mass transfer, and resisting fouling in fluid flows are important for various applications. In this context, textured surfaces impregnated with a liquid lubricant show promise due to their ability to sustain a liquid-liquid layer that induces slippage. However, theoretical and numerical studies suggest that the slippage can be compromised by surfactants in the overlying fluid, which contaminate the liquid-liquid interface and generate Marangoni stresses. In this study, we use Doppler-optical coherence tomography, an interferometric imaging technique, combined with numerical simulations to investigate how surfactants influence the slip length of lubricant-infused surfaces with longitudinal grooves in a laminar flow. We introduce surfactants by adding tracer particles (milk) to the working fluid (water). Local measurements of slip length at the liquid-liquid interface are significantly smaller than theoretical predictions for clean interfaces (Schönecker & Hardt 2013). In contrast, measurements are in good agreement with numerical simulations of fully immobilized interfaces, indicating that milk particles adsorbed at the interface are responsible for the reduction in slippage. This work provides the first experimental evidence that liquid-liquid interfaces within textured surfaces can become immobilized in the presence of surfactants and flow.

physics.flu-dyn↗

arXiv2025

Optical Coherence Tomography in Soft Matter

Optical Coherence Tomography (OCT) has become an indispensable tool for investigating mesoscopic features in soft matter and fluid mechanics. Its ability to provide high-resolution, non-invasive measurements in both spatial and temporal domains bridges critical gaps in experimental instrumentation, enabling the study of complex, confined, and dynamic systems. This review serves as both an introduction to OCT and a practical guide for researchers seeking to adopt this technology. A set of tutorials, complemented by Python scripts, are provided for both intensity- and Doppler-based techniques. The versatility of OCT is illustrated through case studies, including time-resolved velocimetry, particle-based velocity measurements, slip velocity characterization, detection of shear-induced structures, and analysis of fluid-fluid and fluid-structure interactions. Drawing on our experiences, we also present a set of practical guidelines for avoiding common pitfalls.

physics.flu-dyn↗

arXiv2024

High repetition rate ultrafast electron diffraction with direct electron detection

Ultrafast electron diffraction (UED) instruments typically operate at kHz or lower repetition rates and rely on indirect detection of electrons. However, these experiments encounter limitations because they are required to use electron beams containing a relatively large number of electrons (>>100 electrons/pulse), leading to severe space-charge effects. Consequently, electron pulses with long durations and large transverse diameters are used to interrogate the sample. Here, we introduce a novel UED instrument operating at a high repetition rate and employing direct electron detection. We operate significantly below the severe space-charge regime by using electron beams containing 1 to 140 electrons per pulse at 30-kHz. We demonstrate the ability to detect time-resolved signals from thin film solid samples with a difference contrast signal, $ΔI/I_0$, and an instrument response function as low as $10^{-5}$ and 184-fs (FWHM), respectively, without temporal compression. Overall, our findings underscore the importance of increasing the repetition rate of UED experiments and adopting a direct electron detection scheme, which will be particularly impactful for gas-phase UED. Our newly developed scheme enables more efficient and sensitive investigations of ultrafast dynamics in photoexcited samples using ultrashort electron beams.

physics.chem-ph↗

arXiv2023

Experimental Investigation on Particle-Laden Flows of Viscoelastic Fluids in Micro-Channels Using Optical Coherence Tomography

Considering the nonlinear response of non-Newtonian fluids to the local shear exerted on the bulks of fluid, the initially quasi-uniform distribution of the particles might be subject to alteration as well, due to the unbalanced force distribution on the particles. The current research investigates such particle migrations for flows of Viscoelastic Fluids (VEFs) in a straight micro-channel with a 1 by 3.25 mm rectangular cross-section. Polyacrylamide polymer in concentrations of 210 and 250 ppm have been used, where the heavy, linear, long-chain structure of the polymer introduces elasticity to the fluid. The flow measurements are performed using the state-of-the-art Optical Coherence Tomography (OCT) in 2D acquisition and doppler modes (D-OCT) to simultaneously resolve tomographic velocity field, and the transition of particles through the monitored cross-sections. Through the implementation of the experimental method in the current manuscript, the capability and convenience of using OCT for the problem at hand are demonstrated, as the abovementioned obtained data were to be equivalently captured by simultaneous use of Particle Image Velocimetry (PIV), for the ambient medium velocity field, and Lagrangian Particle Tracking (LPT) schemes, for identification and tracking the position of the particles. The velocity field is obtained with the spatial resolution of 2.58um in the depth direction, and through sub-pixel image processing, highly accurate positioning of the particles is realized. The experimental results are then used for statistical calculations, such as the Probability Distribution Function (PDF) of the cross-sectional map of the space frequented by the particles to explain the underlying physics.

physics.flu-dyn↗

arXiv2021

A tutorial review: probing molecular structure and dynamics with CEI and LIED

Knowledge of the molecular structure is key to understanding the function of participating molecules in photo-induced chemical reactions. Visualizing the nuclear dynamics of a photochemical reaction requires an ultrafast measurement technique that can identify the location of atoms in molecules with atomic Ångstrom spatial resolution evolving on the nuclear (i.e. hundreds of femtosecond) timescale. Coulomb explosion imaging (CEI) and laser-induced electron diffraction (LIED) offer the required sub-Ångstrom spatial and tens of femtosecond temporal resolution to track in real-time changes in the molecular structure. In this tutorial review, details of the tools, analysis procedures, exemplary previous results and future perspectives of both CEI and LIED techniques are described.

physics.chem-ph↗

arXiv2021

Machine learning for laser-induced electron diffraction imaging of molecular structures

Ultrafast diffraction imaging is a powerful tool to retrieve the geometric structure of gas-phase molecules with combined picometre spatial and attosecond temporal resolution. However, structural retrieval becomes progressively difficult with increasing structural complexity, given that a global extremum must be found in a multi-dimensional solution space. Worse, pre-calculating many thousands of molecular configurations for all orientations becomes simply intractable. As a remedy, here, we propose a machine learning algorithm with a convolutional neural network which can be trained with a limited set of molecular configurations. We demonstrate structural retrieval of a complex and large molecule, Fenchone (C$_{10}$H$_{16}$O), from laser-induced electron diffraction (LIED) data without fitting algorithms or ab initio calculations. Retrieval of such a large molecular structure is not possible with other variants of LIED or ultrafast electron diffraction. Combining electron diffraction with machine learning presents new opportunities to image complex and larger molecules in static and time-resolved studies.

physics.chem-ph↗

arXiv2021

Quantum interference and imaging using intense laser fields

The interference of matter waves is one of the intriguing features of quantum mechanics that has impressed researchers and laymen since it was first suggested almost a century ago. Nowadays, attosecond science tools allow us to utilize it in order to extract valuable information from electron wavepackets. Intense laser fields are routinely employed to create electron wave packets and control their motion with sub-femtosecond and sub-nanometer precision. In this perspective article, we discuss some of the peculiarities of intense light-matter interaction. We review some of the most important techniques used in attosecond imaging, namely photoelectron holography and laser-induced electron diffraction. We attempt to ask and answer a few questions that do not get asked very often. For example, if we are interested in position space information, why are measurements carried out in momentum space? How to accurately retrieve photoelecron spactra from the numerical solution of the time-dependent Schrödinger equation? And, what causes the different coherence properties of high-harmonic generation and above-threshold ionization?

physics.chem-ph↗

arXiv2021

Generating high density molecular jets of complex neutral organic molecules using micro-sized Tesla valves

We report the design and implementation of multiple Tesla type micro valves in the target delivery system of a reaction microscope (ReMi) to study gas phase structural dynamics of complex polyatomic molecules, when no delivery system currently exists that can deliver dense enough molecular jets of neutral complex molecules without ionizing or exciting the target. We show, the Tesla valves provide an efficient unidirectional flow of the cis-stilbene molecules into the ReMi. We demonstrate using a bubbler with Tesla valves an order-of-magnitude increase in the detected stilbene molecular ion signal following the strong-field tunnel ionization (SFTI), compared to conventional bubbler without any Tesla valves. Our results for the first time, opens the door for studying large, complex neutral molecules in the gas-phase with low vapour pressures in future ultrafast studies.

physics.atom-ph↗

arXiv2020

Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia

Visualizing molecular transformations in real-time requires a structural retrieval method with Ångström spatial and femtosecond temporal atomic resolution. Imaging of hydrogen-containing molecules additionally requires an imaging method that is sensitive to the atomic positions of hydrogen nuclei, with most methods possessing relatively low sensitivity to hydrogen scattering. Laser-induced electron diffraction (LIED) is a table top technique that can image ultrafast structural changes of gas-phase polyatomic molecules with sub-Ångström and femtosecond spatiotemporal resolution together with relatively high sensitivity to hydrogen scattering. Here, we image the umbrella motion of an isolated ammonia molecule (NH$_3$) following its strong field ionization. Upon ionization of a neutral ammonia molecule, the ammonia cation (NH$_3^+$) undergoes an ultrafast geometrical transformation from a pyramidal ($Φ_{HNH} = 107 ^\circ$) to planar ($Φ_{HNH}=120^\circ$) structure in approximately 8 femtoseconds. Using LIED, we retrieve a near-planar ($Φ_{HNH}=117 \pm 5^\circ$) field-dressed NH$_3^+$ molecular structure $7.8-9.8$ femtoseconds after ionization. Our measured field-dressed NH$_3^+$ structure is in excellent agreement with our calculated equilibrium field dressed structure using quantum chemical ab initio calculations.

physics.chem-ph↗

arXiv2020

Symphony on Strong Field Approximation

This paper has been prepared by the Symphony collaboration (University of Warsaw, Uniwersytet Jagielloński, DESY/CNR and ICFO) on the occasion of the 25th anniversary of the "simple man's models" which underlie most of the phenomena that occur when intense ultrashort laser pulses interact with matter. The phenomena in question include High-Harmonic Generation, Above-Threshold Ionization, and Non-Sequential Multielectron Ionization. "Simple man's models" provide, both an intuitive basis for understanding the numerical solutions of the time-dependent Schrödinger equation, and the motivation for the powerful analytic approximations generally known as the Strong Field Approximation (SFA). In this paper we first review the SFA in the form developed by us in the last 25 years. In this approach SFA is a method to solve the TDSE using a systematic perturbation theory in a part of the Hamiltonian describing continuum-continuum transitions in the presence of the laser field. In this review we focus on recent applications of SFA to HHG, ATI and NSMI from multi-electron atoms and from multi-atom. The main novel part of the presented theory concerns generalizations of SFA to: (i) time-dependent treatment of two-electron atoms, allowing for studies of an interplay between Electron Impact Ionization (EII) and Resonant Excitation with Subsequent Ionization (RESI); (ii) time-dependent treatment in the single active electron (SAE) approximation of "large" molecules and targets which are themselves undergoing dynamics during the HHG or ATI process. In particular, we formulate the general expressions for the case of arbitrary molecules, combining input from quantum chemistry and quantum dynamics. We formulate also theory of time-dependent separable molecular potentials to model analytically the dynamics of realistic electronic wave packets for molecules in strong laser fields.

quant-ph↗

arXiv2020

Ultrafast electron diffraction imaging of gas-phase molecules

Knowledge of molecular structure is paramount in understanding, and ultimately influencing, chemical reactivity. For nearly a century, diffractive imaging has been used to identify the structures of many biologically-relevant gas-phase molecules with atomic (i.e. Angstrom, A; 1 A = 10$^{-10}$ m) spatial resolution. Unravelling the mechanisms of chemical reactions requires the capability to record multiple well-resolved snapshots of the molecular structure as it is evolving on the nuclear (i.e. femtosecond, fs; 1 fs = 10$^{-15}$ s) timescale. We present the latest, state-of-the-art ultrafast electron diffraction methods used to retrieve the molecular structure of gas-phase molecules with Angstrom and femtosecond spatio-temporal resolution. We first provide a historical and theoretical background to elastic electron scattering in its application to structural retrieval, followed by details of field-free and field-dressed ultrafast electron diffraction techniques. We discuss the application of these ultrafast methods to time-resolving chemical reactions in real-time, before providing a future outlook of the field and the challenges that exist today and in the future.

physics.chem-ph↗

arXiv2019

Imaging an isolated water molecule using a single electron wave packet

Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of ${\rm H_2O^+}$ with picometre and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched ${\rm H_2O^+}$ field-dressed structure that is most likely in the ground electronic state. We subsequently study the nuclear response of an isolated water molecule to an external laser field at four different field strengths. We show that upon increasing the laser field strength from 2.5 to 3.8 V/Å, the O-H bond is further stretched and the molecule slightly bends. The observed ultrafast structural changes lead to an increase in the dipole moment of water and, in turn, a stronger dipole interaction between the nuclear framework of the molecule and the intense laser field. Our results provide important insights into the coupling of the nuclear framework to a laser field as the molecular geometry of ${\rm H_2O^+}$ is altered in the presence of an external field.

physics.chem-ph↗

arXiv2019

Imaging the Renner-Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS$_2$) in the B$^1$B$_2$ excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS$_2$ molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the B$^1$B$_2$ excited state in neutral CS$_2$, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS$_2$, which is known to appear as a two-center scatterer.

physics.chem-ph↗

arXiv2019

Gas-phase structural isomer identification by Coulomb explosion of aligned molecules

The gas-phase structures of four difluoroiodobenzene and two dihydroxybromobenzene isomers were identified by correlating the emission angles of atomic fragment ions created following femtosecond laser-induced Coulomb explosion. The structural determinations were facilitated by confining the most polarizable axis of each molecule to the detection plane prior to the Coulomb explosion event using one-dimensional laser-induced adiabatic alignment. For a molecular target consisting of two difluoroiodobenzene isomers, each constituent structure could additionally be singled out and distinguished.

physics.chem-ph↗