arXiv subjects

J. Biegert

Publications and source records attributed to J. Biegert.

At least 19 recordsLinked to original sources

arXiv2023

Enhanced optical conductivity and many-body effects in strongly-driven photo-excited semi-metallic graphite

The excitation of quasi-particles near the extrema of the electronic band structure is a gateway to electronic phase transitions in condensed matter. In a many-body system, quasi-particle dynamics are strongly influenced by the electronic single-particle structure and have been extensively studied in the weak optical excitation regime. Yet, under strong optical excitation, where light fields coherently drive carriers, the dynamics of many-body interactions that can lead to new quantum phases remain largely unresolved. Here, we induce such a highly non-equilibrium many-body state through strong optical excitation of charge carriers near the van Hove singularity in graphite. We investigate the system's evolution into a strongly-driven photo-excited state with attosecond soft X-ray core-level spectroscopy. Surprisingly, we find an enhancement of the optical conductivity of nearly ten times the quantum conductivity and pinpoint it to carrier excitations in flat bands. This interaction regime is robust against carrier-carrier interaction with coherent optical phonons acting as an attractive force reminiscent of superconductivity. The strongly-driven non-equilibrium state is markedly different from the single-particle structure and macroscopic conductivity and is a consequence of the non-adiabatic many-body state.

cond-mat.mtrl-sci↗

arXiv2022

Pulse length effects in long wavelength driven non-sequential double ionization

We present a joint experimental and theoretical study of non-sequential double ionization (NSDI) in argon driven by a 3100-nm laser source. The correlated photoelectron momentum distribution (PMD) shows a strong dependence on the pulse duration, and the evolution of the PMD can be explained by an envelope-induced intensity effect. Determined by the time difference between tunneling and rescattering, the laser vector potential at the ionization time of the bound electron will be influenced by the pulse duration, leading to different drift momenta. Such a mechanism is extracted through a classical trajectory Monte Carlo-based model and it can be further confirmed by quantum mechanical simulations. This work sheds light on the importance of the pulse duration in NSDI and improves our understanding of the strong field tunnel-recollision dynamics under mid-IR laser fields.

physics.atom-ph↗

arXiv2022

Laser-induced electron diffraction in the over-the-barrier ionization (OBI) regime

Large polyatomic molecules typically exhibit low ionization potentials, Ip, leading to over-the-barrier ionization (OBI) already at relatively low intensities (~1013 W/cm2). We revisit laser-induced electron diffraction (LIED) in the over-the-barrier ionization (OBI) regime and answer the question of whether imaging of molecular structure is still possible with LIED. We employ a hydrogen-like model system mimicking a molecule with low Ip using a classical trajectory-based model (CT) that incorporates the Coulomb potential; we also use the numerical solution to the time-dependent Schrodinger equation (TDSE). Specifically, we adopt the Fourier transform variant of LIED (FT-LIED) to show that even a significant contribution of short trajectories in the OBI regime does not preclude structure retrieval from strong-field diffractive patterns. This theoretical investigation shows that LIED can be well described by the classical recollision model even when ionization occurs within the OBI regime. This study paves the way towards strong-field imaging of chemical transformations of large polyatomic molecules in real-time based on strong-field electron recollision.

physics.atom-ph↗

arXiv2022

Non-Adiabatic Electronic and Vibrational Ring-Opening Dynamics resolved with Attosecond Core-Level Spectroscopy

Non-adiabatic dynamics and conical intersections play a central role in the chemistry of most polyatomic molecules, ranging from isomerization to heterocyclic ring opening and avoided photo-damage of DNA. Studying the underpinning correlated dynamics of electronic and nuclear wave packets is a major challenge in real-time and, many times involves optically dark transient states. We show that attosecond core-level spectroscopy reveals the pathway dynamics of neutral furan across its conical intersections and dark states. Our method measures electronic-nuclear correlations to detect the dephasing of electronic coherence due to nuclear motion and identifies the ring-opened isomer as the dominant product. These results demonstrate the efficacy of attosecond core level spectroscopy as a potent method to investigate the real-time dynamics of photochemical reaction pathways in complex molecular systems.

physics.chem-ph↗

arXiv2022

Attosecond Physics and Quantum Information Science

In this article, we will discuss a possibility of a symbiosis for attophysics (AP) and quantum information (QI) and quantum technologies (QT). We will argue that within few years AP will reach Technology Readiness Level (RTL) 4-5 in QT, and will thus become a legitimate platform for QI and QT.

quant-ph↗

arXiv2021

Probing the energy conversion pathways between light, carriers and lattice in real time with attosecond core-level spectroscopy

Detection of the energy conversion pathways, between photons, charge carriers, and the lattice is of fundamental importance to understand fundamental physics and to advance materials and devices. Yet, such insight remains incomplete due to experimental challenges in disentangling the various signatures on overlapping time scales. Here, we show that attosecond core-level X-ray spectroscopy can identify these interactions with attosecond precision and across a picosecond range. We demonstrate this methodology on graphite since its investigation is complicated by a variety of mechanisms occurring across a wide range of temporal scales. Our methodology reveals, through the simultaneous real-time detection of electrons and holes, the different dephasing mechanisms for each carrier type dependent on excitation with few-cycle-duration light fields. These results demonstrate the general ability of our methodology to detect and distinguish the various dynamic contributions to the flow of energy inside materials on their native time scales.

cond-mat.mtrl-sci↗

arXiv2021

Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.

physics.atom-ph↗

arXiv2021

Few-cycle mid-infrared pulses from BaGa2GeSe6

BGGSe is a newly developed nonlinear material that is attractive for ultrabroad frequency mixing and ultrashort pulse generation due to its comparably low dispersion and high damage threshold.In a first experiment, we show that a long crystal length of 2.6 mm yields a pulse energy of 21 pJ at 100 MHz with a spectral bandwidth covering 5.8 to 8.5 microns. The electric field of the carrier-envelope-phase stable pulse is directly measured with electro-optical sampling and reveals a pulse duration of 91 fs, which corresponds to sub-four optical cycles, thus confirming some of the prospects of the material for ultrashort pulse generation and mid-infrared spectroscopy.

physics.optics↗

arXiv2017

Above-threshold ionization (ATI) in multicenter molecules: the role of the initial state

A possible route to extract electronic and nuclear dynamics from molecular targets with attosecond temporal and nanometer spatial resolution is to employ recolliding electrons as `probes'. The recollision process in molecules is, however, very challenging to treat using {\it ab initio} approaches. Even for the simplest diatomic systems, such as H$_2$, today's computational capabilities are not enough to give a complete description of the electron and nuclear dynamics initiated by a strong laser field. As a consequence, approximate qualitative descriptions are called to play an important role. In this contribution we extend the work presented in N. Su\'arez {\it et al.}, Phys.~Rev. A {\bf 95}, 033415 (2017), to three-center molecular targets. Additionally, we incorporate a more accurate description of the molecular ground state, employing information extracted from quantum chemistry software packages. This step forward allows us to include, in a detailed way, both the molecular symmetries and nodes present in the high-occupied molecular orbital. We are able to, on the one hand, keep our formulation as analytical as in the case of diatomics, and, on the other hand, to still give a complete description of the underlying physics behind the above-threshold ionization process. The application of our approach to complex multicenter - with more than 3 centers, targets appears to be straightforward.

physics.atom-ph↗

arXiv2016

Above-Threshold Ionization and Laser-Induced Electron Diffraction in Diatomic Molecules

Strong field photoemission and electron recollision provide a viable route to extract electronic and nuclear dynamics from molecular targets with attosecond temporal resolution. However, since an {\em ab-initio} treatment of even the simplest diatomic systems is beyond today's capabilities approximate qualitative descriptions are warranted. In this paper, we develop such a theoretical approach to model the photoelectrons resulting from intense laser-molecule interaction. We present a general theory for symmetric diatomic molecules in the single active electron approximation that, amongst other capabilities, allows adjusting both the internuclear separation and molecular potential in a direct and simple way. More importantly we derive an analytic approximate solution of the time dependent Schr\"odinger equation (TDSE), based on a generalized strong field approximation (SFA) version. Using that approach we obtain expressions for electrons emitted transition amplitudes from two different molecular centres, and accelerated then in the strong laser field. One innovative aspect of our theory is the fact that the dipole matrix elements are free from non-physical gauge and coordinate system dependent terms -- this is achieved by adapting the coordinate system, in which SFA is performed, to the centre from which the corresponding part of the time dependent wave function originates. Our analytic results agree very well with the numerical solution of the full three-dimensional TDSE for the H$_2^+$ molecule. Moreover, the theoretical model was applied to describe laser-induced electron diffraction (LIED) measurements of O$_2^+$ molecules, obtained at ICFO, and reproduces the main features of the experiment very well. Our approach can be extended in a natural way to more complex molecules and multi-electron systems.

physics.atom-ph↗

arXiv2016

Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets

The ability to directly follow and time resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as {\pi}g) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval of the structure of randomly oriented O2 and C2H2 molecules, with {\pi}g and {\pi}u symmetries, respectively, and where their ionisation probabilities do not maximise along their molecular axes. While this removes a serious bottleneck for laser induced diffraction imaging, we find unexpectedly strong back scattering contributions from low-Z atoms.

physics.atom-ph↗

arXiv2016

0.5 keV soft X-ray attosecond continua

Attosecond light pulses in the extreme ultraviolet have drawn a great deal of attention due to their ability to interrogate electronic dynamics in real time. Nevertheless, to follow charge dynamics and excitations in materials, element selectivity is a prerequisite, which demands such pulses in the soft X-ray region, above 200 eV, to simultaneously cover several fundamental absorption edges of the constituents of the materials. Here, we experimentally demonstrate the exploitation of a transient phase matching regime to generate carrier envelope controlled soft X-ray supercontinua with pulse energies up to 2.9 +/- 0.1 pJ and a flux of (7.3 +/- 0.1)x10^7 photons/s across the entire water window and attosecond pulses with 13 as transform limit. Our results herald attosecond science at the fundamental absorption edges of matter by bridging the gap between ultrafast temporal resolution and element specific probing.

physics.atom-ph↗

arXiv2013

Enabling high-precision 3D strong-field measurements - Ionization with low-frequency fields in the tunneling regime

Ionization of an atom or molecule presents surprising richness beyond our current understanding: strong-field ionization with low-frequency fields recently revealed unexpected kinetic energy structures (1, 2). A solid grasp on electron dynamics is however pre-requisite for attosecond-resolution recollision imaging (3), orbital tomography (4), for coherent sources of keV light (5), or to produce zeptosecond-duration x-rays (6). We present a methodology that enables scrutinizing strong-field dynamics at an unprecedented level. Our method provides high-precision measurements only 1 meV above the threshold despite 5 orders higher ponderomotive energies. Such feat was realized with a specifically developed ultrafast mid-IR light source in combination with a reaction microscope. We observe electron dynamics in the tunneling regime (γ = 0.3) and show first 3D momentum distributions demonstrating surprising new observations of near-zero momentum electrons and low momentum structures, below the eV, despite quiver energies of 95 eV.

physics.atom-ph↗

arXiv2012

Above threshold ionization by few-cycle spatially inhomogeneous fields

We present theoretical studies of above threshold ionization (ATI) produced by spatially inhomogeneous fields. This kind of field appears as a result of the illumination of plasmonic nanostructures and metal nanoparticles with a short laser pulse. We use the time-dependent Schr\"odinger equation (TDSE) in reduced dimensions to understand and characterize the ATI features in these fields. It is demonstrated that the inhomogeneity of the laser electric field plays an important role in the ATI process and it produces appreciable modifications to the energy-resolved photoelectron spectra. In fact, our numerical simulations reveal that high energy electrons can be generated. Specifically, using a linear approximation for the spatial dependence of the enhanced plasmonic field and with a near infrared laser with intensities in the mid- 10^{14} W/cm^{2} range, we show it is possible to drive electrons with energies in the near-keV regime. Furthermore, we study how the carrier envelope phase influences the emission of ATI photoelectrons for few-cycle pulses. Our quantum mechanical calculations are supported by their classical counterparts.

physics.optics↗

arXiv2012

Tailoring high-order harmonic generation with nonhomogeneous fields and electron confinement

We study high-order harmonic generation (HHG) resulting from the illumination of plasmonic nanostructures with a short laser pulse. We show that both the inhomogeneities of the local electric field and the confinement of the electron motion play an important role in the HHG process and lead to a significant increase of the harmonic cutoff. In order to understand and characterize this feature, we combine the numerical solution of the time dependent Schroedinger equation (TDSE) with the electric fields obtained from 3D finite element simulations. We employ time-frequency analysis to extract more detailed information from the TDSE results and to explain the extended harmonic spectra. Our findings have the potential to boost up the utilization of HHG as coherent extreme ultraviolet (XUV) sources.

physics.atom-ph↗

arXiv2012

High-order harmonic generation from inhomogeneous fields

We present theoretical studies of high-order harmonic generation (HHG) produced by non-homogeneous fields as resulting from the illumination of plasmonic nanostructures with a short laser pulse. We show that both the inhomogeneity of the local fields and the confinement of the electron movement play an important role in the HHG process and lead to the generation of even harmonics and a significantly increased cutoff, more pronounced for the longer wavelengths cases studied. In order to understand and characterize the new HHG features we employ two different approaches: the numerical solution of the time dependent Schrödinger equation (TDSE) and the semiclassical approach known as Strong Field Approximation (SFA). Both approaches predict comparable results and show the new features, but using the semiclassical arguments behind the SFA and time-frequency analysis tools, we are able to fully understand the reasons of the cutoff extension.

physics.atom-ph↗

arXiv2011

Multi-octave supercontinuum from mid-IR filamentation in bulk

In supercontinuum generation, various propa- gation effects combine to produce a dramatic spec- tral broadening of intense ultrashort optical pulses with far reaching possibilities. Different applications place highly divergent and challenging demands on source characteristics such as spectral coverage from the ultraviolet (UV) across the visible (VIS) to the near-infrared (NIR), and into the mid-infrared (MIR). Shot-to-shot repeatability, high spectral energy density, an absence of complicated or non-deterministic pulse splitting are also essential for many applications. Here we present an "all in one" solution with the first supercontinuum in bulk covering the broad- est bandwidth from just above UV far into the MIR. The spectrum spans more than three octaves, carries high spectral energy density (3pJ up to 10 nJ per nanometer), has high shot-to-shot reproducibility, and is carrier-to-envelope phase (CEP) stable. Our method, based on filamentation of a femtosecond MIR pulse in the anoma- lous dispersion regime, allows for a new class of simple and compact supercontinuum sources.

physics.optics↗

arXiv2011

Coherent Control of Vibrational State Population in a Nonpolar Molecule

A coherent control scheme for the population distribution in the vibrational states of nonpolar molecules is proposed. Our theoretical analysis and results of numerical simulations for the interaction of the hydrogen molecular ion in its electronic ground state with an infrared laser pulse reveal a selective two-photon transition between the vibrational states via a coupling with the first excited dissociative state. We demonstrate that for a given temporal intensity profile the population transfer between vibrational states, or a superposition of vibrational states, can be made complete for a single chirped pulse or a train of chirped pulses, which accounts for the accumulated phase difference due to the AC Stark effect. Effects of a spatial intensity (or, focal) averaging are discussed.

quant-ph↗