arXiv subjects

Ivan Madan

Publications and source records attributed to Ivan Madan.

12 recordsLinked to original sources

arXiv2024

Ultrafast momentum-resolved visualization of the interplay between phonon-mediated scattering and plasmons in graphite

Scattering between individual charges and collective modes in materials governs fundamental phenomena such as electrical resistance, energy dissipation, switching between different phases, and ordering. The study of such scattering requires a simultaneous access to the ultrafast momentum-resolved dynamics of single-particle and collective excitations, which remains as an experimental challenge. Here, we demonstrate time- and momentum-resolved electron energy-loss spectroscopy, and apply it to graphite showing that large ($\Delta q\simeq$1.2~{\AA}$^{-1}$) photoexcited electron-hole (e-h) pockets in the band structure induce a renormalization of the collective in-plane and bulk plasmons that can be described quantitatively by invoking intra- and inter-valley scattering processes mediated by $E_{2g}$ and $A_{1}'$ phonon modes, which we directly observe by ultrafast electron diffraction and identify via ab initio calculations. Conversely, the photoexcitation of smaller e-h pockets ($\Delta q\simeq$0.7~{\AA}$^{-1}$) close to the K point of graphite results in the renormalization of in-plane plasmons, which can only be partially explained by phonon-mediated scattering and thermal expansion. Our results show the importance of combining momentum- and time-resolved information to elucidate microscopic details associated with electronic scattering processes.

cond-mat.mes-hall↗

arXiv2024

Revisiting the excitation of the low-lying $^{181\text{m}}$Ta isomer in optical laser-generated plasma

The excitation of the $^{181\text{m}}$Ta isomer in the laser-plasma scenario was claimed to have been observed more than two decades ago. However, the reported experimental findings - and the respective high excitation rate - were later questioned as they could not be reproduced theoretically. The controversy has remained open ever since. In this work, we reinvestigate both theoretically and experimentally the $^{181\text{m}}$Ta nuclear excitation in an optical laser-generated plasma. Experimentally we have found no evidence for such an excitation process as consistently predicted by previous and our theoretical models.

nucl-ex↗

arXiv2022

Observation of a new light-induced skyrmion phase in the Mott insulator Cu2OSeO3

We report the discovery of a novel skyrmion phase in the multiferroic insulator Cu2OSeO3 for magnetic fields below the equilibrium skyrmion pocket. This phase can be accessed by exciting the sample out of equilibrium with near-infrared (NIR) femtosecond laser pulses but can not be reached by any conventional field cooling protocol. From the strong wavelength dependence of the photocreation process and via spin dynamics simulations, we identify the magnetoelastic effect as the most likely photocreation mechanism. This effect results in a transient modification of the magnetic interaction extending the equilibrium skyrmion pocket to lower magnetic fields. Once created, the skyrmions rearrange and remain stable over a long time, reaching minutes. The presented results are relevant for designing high-efficiency non-volatile data storage based on magnetic skyrmions.

cond-mat.str-el↗

arXiv2022

Imaging the ultrafast coherent control of a skyrmion crystal

Exotic magnetic textures emerging from the subtle interplay between thermodynamic and topological fluctuation have attracted intense interest due to their potential applications in spintronic devices. Recent advances in electron microscopy have enabled the imaging of random photo-generated individual skyrmions. However, their deterministic and dynamical manipulation is hampered by the chaotic nature of such fluctuations and the intrinsically irreversible switching between different minima in the magnetic energy landscape. Here, we demonstrate a method to coherently control the rotation of a skyrmion crystal by discrete amounts at speeds which are much faster than previously observed. By employing circularly polarized femtosecond laser pulses with an energy below the bandgap of the Mott insulator Cu2OSeO3, we excite a collective magnon mode via the inverse Faraday effect. This triggers coherent magnetic oscillations that directly control the rotation of a skyrmion crystal imaged by cryo-Lorentz Transmission Electron Microscopy. The manipulation of topological order via ultrafast laser pulses shown here can be used to engineer fast spin-based logical devices.

cond-mat.str-el↗

arXiv2022

Nuclear Excitation by Electron Capture in Excited Ions

A nuclear excitation following the capture of an electron in an empty orbital has been recently observed for the first time. So far, the evaluation of the cross section of the process has been carried out widely using the assumption that the ion is in its electronic ground state prior to the capture. We show that by lifting this restriction new capture channels emerge resulting in a boost of more than three orders of magnitude to the electron capture resonance strength.

nucl-th↗

arXiv2022

Charge dynamics electron microscopy: nanoscale imaging of femtosecond plasma dynamics

Understanding and actively controlling the spatio-temporal dynamics of non-equilibrium electron clouds is fundamental for the design of light and electron sources, novel high-power electronic devices, and plasma-based applications. However, electron clouds evolve in a complex collective fashion on nanometer and femtosecond scales, producing electromagnetic screening that renders them inaccessible to existing optical probes. Here, we solve the long-standing challenge of characterizing the evolution of electron clouds generated upon irradiation of metallic structures using an ultrafast transmission electron microscope to record the charged plasma dynamics. Our approach to charge dynamics electron microscopy (CDEM) is based on the simultaneous detection of electron-beam acceleration and broadening with nanometer/femtosecond resolution. By combining experimental results with comprehensive microscopic theory, we provide deep understanding of this highly out-of-equilibrium regime, including previously inaccessible intricate microscopic mechanisms of electron emission, screening by the metal, and collective cloud dynamics. Beyond the present specific demonstration, the here introduced CDEM technique grants us access to a wide range of non-equilibrium electrodynamic phenomena involving the ultrafast evolution of bound and free charges on the nanoscale.

physics.app-ph↗

arXiv2022

Ultrafast Electron Microscopy of Nanoscale Charge Dynamics in Semiconductors

The ultrafast dynamics of charge carriers in solids plays a pivotal role in emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, the investigation and direct visualization of such non-equilibrium transport phenomena remains as a long-standing challenge, owing to the nanometer-femtosecond spatio-temporal scales at which the charge carriers evolve. Here, we propose and demonstrate a novel interaction mechanism enabling nanoscale imaging of the femtosecond dynamics of charge carriers in solids. This imaging modality, which we name charge dynamics electron microscopy (CDEM), exploits the strong interaction between terahertz (THz) electromagnetic near fields produced by the moving charges and synchronized free-electron pulses in an ultrafast scanning transmission electron microscope. The measured free-electron energy at different spatio-temporal coordinates allows us to directly retrieve the THz near-field amplitude and phase, from which we reconstruct movies of the generated charges by comparison with microscopic theory. The introduced CDEM technique thus allows us to investigate previously inaccessible spatio-temporal regimes of charge dynamics in solids, for example revealing new insight into the photo-Dember effect, showing oscillations of photo-generated electron-hole distributions inside a semiconductor. Our work lays the foundation for exploring a wide range of previously inaccessible charge-transport phenomena in condensed matter using ultrafast electron microscopy.

cond-mat.mes-hall↗

arXiv2022

Nuclear Excitation by Muon Capture

Efficient excitation of nuclei via exchange of a real or virtual photon has a fundamental importance for nuclear science and technology development. Here, we present a new mechanism of nuclear excitation based on the capture of a free muon into the atomic orbits (NE$μ$C). The cross section of such a new process is evaluated using the Feshbach projection operator formalism and compared to other known excitation phenomena, i.e. photo-excitation and nuclear excitation by electron capture (NEEC), showing up to ten orders of magnitude increase in cross section. NE$μ$C is particularly interesting for MeV excitations that become accessible thanks to the stronger binding of muons to the nucleus. The binding energies of muonic atoms have been calculated introducing a state of the art modification to the Flexible Atomic Code (FAC). An analysis of an experimental scenarios in the context of modern muon production facilities shows that the effect can be detectable for selected isotopes. The total probability of NE$μ$C is predicted to be $ P \approx 10^{-6}$ per incident muon in a beam-based scenario. Given the high transition energy provided by muons, NE$μ$C can have important consequences for isomer feeding and particle-induced fission.

nucl-th↗

arXiv2020

Nanoscale-femtosecond dielectric response of Mott insulators captured by two-colour near-field ultrafast electron microscopy

Characterizing and controlling the out-of-equilibrium state of nanostructured Mott insulators hold great promises for emerging quantum technologies while providing an exciting playground for investigating fundamental physics of strongly-correlated systems. Here, we use two-colour near-field ultrafast electron microscopy to photo-induce the insulator-to-metal transition in a single VO2 nanowire and probe the ensuing electronic dynamics with combined nanometer-femtosecond resolution. We take advantage of a femtosecond temporal gating of the electron pulse mediated by an infrared laser pulse, and exploit the sensitivity of inelastic electron-light scattering to changes in the material dielectric function. By spatially mapping the near-field dynamics of an individual nanowire of VO2, we observe that ultrafast photo-doping drives the system into a metallic state on a time scale of about 150 fs without yet perturbing the crystalline lattice. Due to the high versatility and sensitivity of the electron probe, our method would allow capturing the electronic dynamics of a wide range of nanoscale materials with ultimate spatio-temporal resolution.

physics.app-ph↗

arXiv2019

Stacking transition in rhombohedral graphite

Few layer graphene (FLG) has been recently intensively investigated for its variable electronic properties defined by a local atomic arrangement. While the most natural layers arrangement in FLG is ABA (Bernal) stacking, a metastable ABC (rhombohedral) stacking characterized by a relatively high energy barrier can also occur. When both stacking occur in the same FLG device this results in in-plane heterostructure with a domain wall (DW). We show that ABC stacking in FLG can be controllably and locally turned into ABA stacking by two following approaches. In the first approach, Joule heating was introduced and the transition was characterized by 2D-peak Raman spectra at a submicron spatial resolution. The observed transition was initiated at a small region and then the DW controllably shifted until the entire device became ABA stacked. In the second approach, the transition was achieved by illuminating the ABC region with a train of laser pulses of 790 nm wavelength, while the transition was visualized by transmission electron microscopy in both diffraction and dark field modes. Also, with this approach, a DW was visualized in the dark-field imaging mode, at a nanoscale spatial resolution.

cond-mat.mes-hall↗

arXiv2014

Ultrafast carrier localisation in the pseudogap state of cuprate superconductors from coherent quench experiments

A pseudogap (PG) was introduced by Mott to describe a state of matter which has a minimum in the density of states at the Fermi level, deep enough for states to become localized. It can arise either from Coulomb repulsion between electrons, or due to an incipient charge or spin order, or a combination of the two. These states are rapidly fluctuating in time with random phase, so they are hard to observe experimentally. Here we present the first coherent quench measurements of the dynamical transition to the pseudogap state in the prototype high temperature superconductor Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$, revealing a marked absence of incipient collective ordering beyond a few coherence lengths on short timescales at any level of doping. Instead we find evidence for sub-picosecond carrier localization favouring a picture of pairing resulting from the competing Coulomb interaction and strain, enhanced by a Fermi surface instability.

cond-mat.str-el↗

arXiv2014

Separating pairing from quantum phase coherence dynamics above the superconducting transition by femtosecond spectroscopy

In classical superconductors an energy gap and phase coherence appear simultaneously with pairing at the transition to the superconducting state. In high-temperature superconductors, the possibility that pairing and phase coherence are distinct and independent processes has led to intense experimental search of their separate manifestations, but so far without success. Using femtosecond spectroscopy methods we now show that it is possible to clearly separate fluctuation dynamics of the superconducting pairing amplitude from the phase relaxation above the critical transition temperature. Empirically establishing a close correspondence between the superfluid density measured by THz spectroscopy and superconducting optical pump-probe response over a wide region of temperature, we find that in differently doped Bi_{2}Sr_{2}CaCu_{2}O_{8+δ} crystals the pairing gap amplitude monotonically extends well beyond T_{c}, while the phase coherence shows a pronounced power-law divergence as T\rightarrow T_{c}, thus showing for the first time that phase coherence and gap formation are distinct processes which occur on different timescales.

cond-mat.supr-con↗