arXiv subjects

I. Madan

Publications and source records attributed to I. Madan.

12 recordsLinked to original sources

arXiv2023

Generation and control of localized terahertz fields in photoemitted electron plasmas

Dense micron-sized electron plasmas, such as those generated upon irradiation of nanostructured metallic surfaces by intense femtosecond laser pulses, constitute a rich playground to study light-matter interactions, many-body phenomena, and out-of-equilibrium charge dynamics. Besides their fundamental interest, laser-induced plasmas hold potential for the generation of localized terahertz radiation pulses. However, the underlying mechanisms ruling the formation and evolution of these plasmas is not yet well understood. Here, we develop a comprehensive microscopic theory to predictably describe the spatiotemporal dynamics of laser-pulse-induced plasmas. Through detailed analysis of electron emission, metal screening, and plasma cloud interactions, we investigate the spatial, temporal, and spectral characteristics of the so-generated terahertz fields, which can be extensively controlled through the metal morphology and the illumination conditions. We further describe the interaction with femtosecond electron beams to explain recent ultrafast electron microscopy experiments, whereby the position and temporal dependence of the observed electron acceleration permits assessing the associated terahertz field. Besides its potential application to the design of low-frequency light sources, our work contributes with fundamental insight on the generation and dynamics of micron-scale electron plasmas and their interaction with ultrafast electron pulses.

cond-mat.mes-hall↗

arXiv2022

Ultrafast generation of hidden phases via energy-tuned electronic photoexcitation in magnetite

Metal-insulator transitions (MIT) occurring in non-adiabatic conditions can evolve through high-energy intermediate states that are difficult to observe and control via static methods. By monitoring the out-of-equilibrium structural dynamics of a magnetite (Fe3O4) crystal via ultrafast electron diffraction, we show that MITs can evolve through different pathways by properly selecting the electronic excitation with light. Near-infrared (800 nm) photons inducing d-d electronic transitions is found to favor the destruction of the long-range zigzag network of the trimerons and to generate a phase separation between cubic-metallic and monoclinic-insulating regions. Instead, visible light (400 nm) further promotes the long-range order of the trimerons by stabilizing the charge density wave fluctuations through the excitation of the oxygen 2p to iron 3d charge transfer and, thus, fosters a reinforcement of the monoclinic insulating phase. Our experiments demonstrate that tailored light pulses can drive strongly correlated materials into different hidden phases, influencing the lifetime and emergent properties of the intermediate states.

cond-mat.str-el↗

arXiv2022

Resonant Inelastic X-ray Scattering Study of Electron-Exciton Coupling in High-Tc Cuprates

Explaining the mechanism of superconductivity in the high-$T_c$ cuprates requires an understanding of what causes electrons to form Cooper pairs. Pairing can be mediated by phonons, the screened Coulomb force, spin or charge fluctuations, excitons, or by a combination of these. An excitonic pairing mechanism has been postulated, but experimental evidence for coupling between conduction electrons and excitons in the cuprates is sporadic. Here we use resonant inelastic x-ray scattering (RIXS) to monitor the temperature dependence of the $\underline{d}d$ exciton spectrum of Bi$_2$Sr$_2$CaCu$_2$O$_{8-x}$ (Bi-2212) crystals with different charge carrier concentrations. We observe a significant change of the $\underline{d}d$ exciton spectra when the materials pass from the normal state into the superconductor state. Our observations show that the $\underline{d}d$ excitons start to shift up (down) in the overdoped (underdoped) sample when the material enters the superconducting phase. We attribute the superconductivity-induced effect and its sign-reversal from underdoped to overdoped to the exchange coupling of the site of the $\underline{d}d$ exciton to the surrounding copper spins.

cond-mat.supr-con↗

arXiv2022

Ultrafast Transverse Modulation of Free Electrons by Interaction with Shaped Optical Fields

Spatio-temporal shaping of electron beams is a bold frontier in electron microscopy, enabling new routes toward spatial-resolution enhancement, selective probing, low-dose imaging and faster data acquisition. Over the last decade, shaping methods evolved from passive phase plates to low-speed electrostatic and magnetostatic displays. Recently, higher shaping speed and flexibility have become feasible by the advent of ultrafast electron microscopy, embodying a swift change of paradigm that relies on using light to control free electrons. Here, we experimentally demonstrate that arbitrary transverse modulation of electron beams is possible without the need for designing and fabricating complicated electron-optics elements or material nanostructures, but rather resorting to shaping light beams reflected from a planar thin film. We demonstrate arbitrary transverse modulation of electron wavepackets via inelastic interaction with a shaped ultrafast light field controlled by an external spatial light modulator (SLM). We illustrate this method by generating Hermite-Gaussian (HG) electron beams with HG10 and HG01 symmetry and discuss their possible use in enhancing the imaging contrast of microscopic features. Relative to current schemes, our approach adopting an external SLM dramatically widens the range of patterns that can be imprinted on the electron wave function and makes electron shaping a much easier task to perform.

physics.optics↗

arXiv2018

Ultrafast Generation and Control of an Electron Vortex Beam via Chiral Plasmonic Near Fields

Vortex-carrying matter waves, such as chiral electron beams, are of significant interest in both applied and fundamental science. Continuous wave electron vortex beams are commonly prepared via passive phase masks imprinting a transverse phase modulation on the electron's wave function. Here, we show that femtosecond chiral plasmonic near fields enable the generation and dynamic control on the ultrafast timescale of an electron vortex beam. The vortex structure of the resulting electron wavepacket is probed in both real and reciprocal space using ultrafast transmission electron microscopy. This method offers a high degree of scalability to small length scales and a highly efficient manipulation of the electron vorticity with attosecond precision. Besides the direct implications in the investigation of nanoscale ultrafast processes in which chirality plays a major role, we further discuss the perspectives of using this technique to shape the wave function of charged composite particles, such as protons, and how it can be used to probe their internal structure.

quant-ph↗

arXiv2018

Laser-Induced Skyrmion Writing and Erasing in an Ultrafast Cryo-Lorentz Transmission Electron Microscopy

We demonstrate that light-induced heat pulses of different duration and energy can write skyrmions in a broad range of temperatures and magnetic field in FeGe. Using a combination of camera-rate and pump-probe cryo-Lorentz Transmission Electron Microscopy, we directly resolve the spatio-temporal evolution of the magnetization ensuing optical excitation. The skyrmion lattice was found to maintain its structural properties during the laser-induced demagnetization, and its recovery to the initial state happened in the sub-μs to μs range, depending on the cooling rate of the system.

cond-mat.str-el↗

arXiv2018

Ultrafast holography enabled by quantum interference of ultrashort electrons

Holography relies on the interference between a known reference and a signal of interest to reconstruct both the amplitude and phase of that signal. Commonly performed with photons and electrons, it finds numerous applications in imaging, cryptography and arts. With electrons, the extension of holography to the ultrafast time domain remains a challenge, although it would yield the highest possible combined spatio-temporal resolution. Here, we show that holograms of local electromagnetic fields can be obtained with combined attosecond/nanometer resolution in an ultrafast transmission electron microscope (UEM). Unlike conventional holography, where the signal and the reference are spatially separated and then recombined to interfere, in our method we use electromagnetic fields to split an electron wave function in a quantum coherent superposition of different energy states. In the image plane, spatial modulation of the electron-energy distribution reflects the phase relation between reference and signal fields, which we map via energy-filtered UEM. Beyond imaging applications, this approach allows implementing optically-controlled and spatially-resolved quantum measurements in parallel, providing an efficient and versatile tool for the exploration of electron quantum optics.

cond-mat.mes-hall↗

arXiv2017

From attosecond to zeptosecond coherent control of free-electron wave functions using semi-infinite light fields

Light-electron interaction in empty space is the seminal ingredient for free-electron lasers and also for controlling electron beams to dynamically investigate materials and molecules. Pushing the coherent control of free electrons by light to unexplored timescales, below the attosecond, would enable unprecedented applications in light-assisted electron quantum circuits and diagnostics at extremely small timescales, such as those governing intramolecular electronic motion and nuclear phenomena. We experimentally demonstrate attosecond coherent manipulation of the electron wave function in a transmission electron microscope, and show that it can be pushed down to the zeptosecond regime with existing technology. We make a relativistic pulsed electron beam interact in free space with an appropriately synthesized semi-infinite light field generated by two femtosecond laser pulses reflected at the surface of a mirror and delayed by fractions of the optical cycle. The amplitude and phase of the resulting coherent oscillations of the electron states in energymomentum space are mapped via momentum-resolved ultrafast electron energy-loss spectroscopy. The experimental results are in full agreement with our theoretical framework for light-electron interaction, which predicts access to the zeptosecond timescale by combining semi-infinite X-ray fields with free electrons.

physics.optics↗

arXiv2017

meV resolution in laser-assisted energy-filtered transmission electron microscopy

The electronic, optical, and magnetic properties of quantum solids are determined by their low-energy (< 100 meV) many-body excitations. Dynamical characterization and manipulation of such excitations relies on tools that combine nm-spatial, fs-temporal, and meV-spectral resolution. Currently, phonons and collective plasmon resonances can be imaged in nanostructures with sub-nm and 10s meV space/energy resolution using state-of-the-art energy-filtered transmission electron microscopy (TEM), but only under static conditions, while fs-resolved measurements are common but lack spatial or energy resolution. Here, we demonstrate a new method of spectrally resolved photon-induced near-field electron microscopy (SRPINEM) that allows us to obtain nm-fs-resolved maps of nanoparticle plasmons with an energy resolution determined by the laser linewidth (20 meV in this work), and not limited by electron beam and spectrometer energy spreading. This technique can be extended to any optically-accessible low-energy mode, thus pushing TEM to a previously inaccessible spectral domain with an unprecedented combination of space, energy and temporal resolution.

cond-mat.mes-hall↗

arXiv2017

Dynamics of the superconducting order parameter through ultrafast normal-to-superconducting phase transition in Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ from multi-pulse polarization-resolved transient optical reflectivity

A systematic temperature dependent study of the femtosecond optical superconducting (SC) state destruction and recovery in Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ cuprate superconductor by means of the all-optical polarization-sensitive multi-pulse spectroscopy is presented. At low temperatures and a partial SC state suppression an anisotropic SC-gap recovery-timescale is suggested by the data. The SC state destruction and recovery dynamics are compared to the recent TR-ARPES-inferred SC-gap dynamics and a qualitative agreement is found. Using a phenomenological response function the experimental data are also compared to time dependent Ginzburg-Landau model simulations.

cond-mat.supr-con↗

arXiv2016

Real time measurement of the emergence of superconducting order in a high temperature superconductor

Systems which rapidly evolve through symmetry-breaking transitions on timescales comparable to the fluctuation timescale of the single-particle excitations may behave very differently than under controlled near-ergodic conditions. A real-time investigation with high temporal resolution may reveal new insights into the ordering through the transition that are not available in static experiments. We present an investigation of the system trajectory through a normal-to-superconductor transition in a prototype high-temperature superconducting cuprate in which such a situation occurs. Using a multiple pulse femtosecond spectroscopy technique we measure the system trajectory and time-evolution of the single-particle excitations through the transition in La$_{1.9}$Sr$_{0.1}$CuO$_{4}$ and compare the data to a simulation based on time-dependent Ginzburg-Landau theory, using laser excitation fluence as an adjustable parameter controlling the quench conditions in both experiment and theory. The comparison reveals the presence of significant superconducting fluctuations which precede the transition on short timescales. By including superconducting fluctuations as a seed for the growth of superconducting order we can obtain a satisfactory agreement of the theory with the experiment. Remarkably, the pseudogap excitations apparently play no role in this process.

cond-mat.supr-con↗

arXiv2013

Dynamics of broken symmetry nodal and anti-nodal excitations in Bi_{2} Sr_{2} CaCu_{2} O_{8+δ} probed by polarized femtosecond spectroscopy

The dynamics of excitations with different symmetry is investigated in the superconducting (SC) and normal state of the high-temperature superconductor Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ (Bi2212) using optical pump-probe (Pp) experiments with different light polarizations at different doping levels. The observation of distinct selection rules for SC excitations, present in A$_{\rm 1g}$ and B$_{\rm 1g}$ symmetries, and for the PG excitations, present in A$_{\rm 1g}$ and B$_{\rm 2g}$ symmetries, by the probe and absence of any dependence on the pump beam polarization leads to the unequivocal conclusion of the existence of a spontaneous spatial symmetry breaking in the pseudogap (PG) state.

cond-mat.supr-con↗