arXiv subjects

Jens Biegert

Publications and source records attributed to Jens Biegert.

At least 37 records · Page 2Linked to original sources

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

Table-top high-energy 7 um OPCPA and 260 mJ Ho:YLF pump laser

We present the state of the art of a compact high-energy mid-infrared laser system for TW-level 8-cycle pulses at 7 um. This system consists of an Er:Tm:Ho:fiber MOPA which serves as the seeder for a ZGP-based OPCPA chain in addition to a Ho:YLF amplifier which is Tm:fiber pumped. Featuring all-optical synchronization, the system delivers 260-mJ pump energy at 2052 nm, 16-ps duration at 100 Hz with a stability of 0.8 % rms over 20 min. We show that chirp inversion in the OPCPA chain leads to excellent energy extraction and aids in compression of the 7-um pulses to 8 optical cycles (188 fs) in bulk BaF2 with 93.5 % efficiency. Using 21.7 mJ of the available pump energy, we generate 0.75-mJ-energy pulses at 7 um due to increased efficiency with a chirp-inversion scheme. The pulse quality of the system's output is shown by generating high harmonics in ZnSe which span up to harmonic order 13 with excellent contrast. The combination of the passive carrier-envelope phase stable mid-infrared seed pulses and the high-energy 2052 nm picosecond pulses makes this compact system a key enabling tool for the next generation of studies on extreme photonics, strong field physics and table-top coherent X-ray science.

physics.optics↗

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

All semiconductor enhanced high-harmonic generation from a single nano-structure

The enhancement and control of non-linear phenomena at a nanometer scale has a wide range of applications in science and in industry. Among these phenomena, high-harmonic generation in solids is a recent focus of research to realize next generation petahertz optoelectronic devices or compact all solid state EUV sources. Here, we report on the realization of the first nanoscale high harmonic source. The strong field regime is reached by confining the electric field from a few nanojoules femtosecond laser in a single 3D semiconductor waveguide. We reveal a strong competition between enhancement of coherent harmonics and incoherent fluorescence favored by excitonic processes. However, far from the band edge, clear enhancement of the harmonic emission is reported with a robust sustainability offering a compact nanosource for applications. We illustrate the potential of our harmonic nano-device by performing a coherent diffractive imaging experiment. Ultra-compact UV/X-ray nanoprobes are foreseen to have other potential applications such as petahertz electronics, nano-tomography or nano-medicine.

physics.optics↗

arXiv2018

Infrared electric-field sampled frequency comb spectroscopy

Molecular spectroscopy in the mid-infrared portion of the electromagnetic spectrum (3--25 um) has been a cornerstone interdisciplinary analytical technique widely adapted across the biological, chemical, and physical sciences. Applications range from understanding mesoscale trends in climate science via atmospheric monitoring to microscopic investigations of cellular biological systems via protein characterization. Here, we present a compact and comprehensive approach to infrared spectroscopy incorporating the development of broadband laser frequency combs across 3--27 um, encompassing the entire mid-infrared, and direct electric-field measurement of the corresponding near single-cycle infrared pulses of light. Utilizing this unified apparatus for high-resolution and accurate frequency comb spectroscopy, we present the infrared spectra of important atmospheric compounds such as ammonia and carbon dioxide in the molecular fingerprint region. To further highlight the ability to study complex biological systems, we present a broadband spectrum of a monoclonal antibody reference material consisting of more than 20,000 atoms. The absorption signature resolves the amide I and II vibrations, providing a means to study secondary structures of proteins. The approach described here, operating at the boundary of ultrafast physics and precision spectroscopy, provides a table-top solution and a widely adaptable technique impacting both applied and fundamental scientific studies.

physics.ins-det↗

arXiv2018

Attosecond dispersive soft X-ray absorption fine structure spectroscopy in graphite

Phase transitions of solids and structural transformations of molecules are canonical examples of important photo-induced processes, whose underlying mechanisms largely elude our comprehension due to our inability to correlate electronic excitation with atomic position in real time. Here, we present a decisive step towards such new methodology based on water-window-covering (284 eV to 543 eV) attosecond soft X-ray pulses that can simultaneously access electronic and lattice parameters via dispersive X-ray absorption fine-structure (XAFS) spectroscopy. We validate attoXAFS with an identification of the σ* and π* orbital contributions to the density of states in graphite simultaneously with its lattice's four characteristic bonding distances. This work demonstrates the concept of attoXAFS as a powerful real-time investigative tool which is equally applicable to gas-, liquid- and condensed phase.

cond-mat.mtrl-sci↗

arXiv2017

Attosecond Streaking in the Water Window: A New Regime of Attosecond Pulse Characterization

We report on the first streaking measurement of water-window attosecond pulses generated via high harmonic generation, driven by sub-2-cycle, CEP-stable, 1850 nm laser pulses. Both the central photon energy and the energy bandwidth far exceed what has been demonstrated thus far, warranting the investigation of the attosecond streaking technique for the soft X-ray regime and the limits of the FROGCRAB retrieval algorithm under such conditions. We also discuss the problem of attochirp compensation and issues regarding much lower photo-ionization cross sections compared with the XUV in addition to the fact that several shells of target gases are accessed simultaneously. Based on our investigation, we caution that the vastly different conditions in the soft X-ray regime warrant a diligent examination of the fidelity of the measurement and the retrieval procedure.

physics.atom-ph↗

arXiv2017

Amplification of high harmonics in 3D semiconductor waveguides

Nanoscale amplification of non-linear processes in solid-state devices opens novel applications in nano-electronics, nano-medicine or high energy conversion for example. Coupling few nano-joules laser energy at a nanometer scale for strong field physics is demonstrated. We report enhancement of high harmonic generation in nano-structured semiconductors using nanoscale amplification of a mid-infrared laser in the sample rather than using large laser amplifier systems. Field amplification is achieved through light confinement in nano-structured semiconductor 3D waveguides. The high harmonic nano-converter consists of an array of zinc-oxide nanocones. They exhibit a large amplification volume, 6 orders of magnitude larger than previously reported and avoid melting observed in metallic plasmonic structures. The amplification of high harmonics is observed by coupling only 5-10 nano-joules of a 3.2 μm high repetition-rate OPCPA laser at the entrance of each nanocone. Harmonic amplification (factor 30) depends on the laser energy input, wavelength and nanocone geometry.

physics.optics↗

arXiv2017

Soliton-effect self-compressed single-cycle 9.6-W mid-IR pulses from a 21-W OPCPA at 3.25 μm and 160 kHz

We report a 21-W mid-IR OPCPA that generates 131-μJ and 97 fs (sub-9-cycle) pulses at 160 kHz repetition rate and at a centre wavelength of 3.25 μm. Pulse-to-pulse stability of the CEP-stable output is excellent with 0.33% rms over 288 million pulses (30 min) and compression close to a single optical cycle was achieved through soliton self- compression inside a gas-filled mid-IR anti-resonant-guiding photonic crystal fibre. Without any additional compression device, stable generation of 14.5 fs (1.35-optical-cycle) pulses was achieved at an average power of 9.6 W. The resulting peak power of 3.9 GW in combination with the near-single-cycle duration and intrinsic CEP stability, make our OPCPA a key-enabling technology for the next generation of extreme photonics, strong-field attosecond research and coherent X-ray science.

physics.optics↗

arXiv2017

Petahertz optical response in graphene

The temporal dynamics of charge carriers determines the speed with which electronics can be realized in condensed matter, and their direct manipulation with optical fields promises electronic processing at unprecedented petahertz frequencies, consisting in a million-fold increase from state of the art technology. Graphene is of particular interest for the implementation of petahertz optoelectronics due to its unique transport properties, such as high carrier mobility with near-ballistic transport and exceptionally strong coupling to optical fields. The back action of carriers in response to an optical field is therefore of key importance towards applications. Here we investigate the instantaneous response of graphene to petahertz optical fields and elucidate the role of hot carriers on a sub-100 fs timescale. Measurements of the nonlinear response and its dependence on interaction time and field polarization allow us to identify the back action of hot carriers over timescales that are commensurate with the optical field. An intuitive picture is given for the carrier trajectories in response to the optical-field polarization state. We note that the peculiar interplay between optical fields and charge carriers in graphene may also apply to surface states in topological insulators with similar Dirac cone dispersion relations.

cond-mat.mes-hall↗

arXiv2017

High-order harmonic generation in atomic and molecular systems

High-order harmonic generation (HHG) results from strong-field laser matter interaction and it is one of the main processes that are used to extract electron structural and dynamical information about the atomic or molecular targets with sub-femtosecond temporal resolution. Moreover, it is the workhorse for the generation of attosecond pulses. Here we develop an analytical description of HHG, which extends the well established theoretical strong-field approximation (SFA). Our approach involves two innovative aspects: i) First, using a model non-local, but separable potential, we calculate the bound-free dipole and the rescattering transition matrix elements analytically for both atomic and molecular multicenter systems. In comparison with the standard approaches to the HHG process, these analytic derivations of the different matrix elements allows us to study directly how the HHG spectra depend on the atomic target and laser pulse features. We can turn on and of contributions having distinct physical origins or corresponding to different physical mechanisms. Our SFA results are compared, when possible, with the direct numerical integration of the time-dependent Schrödinger equation (TDSE) in reduced and full dimensionality. Excellent agreement is found for single and multielectronic atomic systems, modeled under the single active electron approximation, and for simple diatomic molecular systems. Our model captures also the interference features, ubiquitously present in every strong-field phenomenon involving a multicenter target.

physics.atom-ph↗

arXiv2016

Transition from non-sequential to sequential double ionisation in many-electron systems

Obtaining a detailed understanding of strong-field double ionisation of many-electron systems (heavy atoms and molecules) remains a challenging task. By comparing experimental and theoretical results in the mid-IR regime, we have unambiguously identified the transition from non-sequential (e,2e) to sequential double ionisation in Xe and shown that it occurs at an intensity below $10^{14}$ Wcm$^{-2}$. In addition, our data demonstrate that ionisation from the Xe 5s orbital is decisive at low intensities. Moreover, using the acetylene molecule, we propose how sequential double ionisation in the mid-IR can be used to study molecular dynamics and fragmentation on unprecedented few-femtosecond timescales.

physics.atom-ph↗

arXiv2015

Above-threshold ionization and photoelectron spectra in atomic systems driven by strong laser fields

Above-threshold ionization (ATI) results from strong field laser-matter interaction and it is one of the fundamental processes that may be used to extract electron structural and dynamical information about the atomic or molecular target. Moreover, it can also be used to characterize the laser field itself. Here, we develop an analytical description of ATI, which extends the theoretical Strong Field Approximation (SFA), for both the direct and re-scattering transition amplitudes in atoms. From a non-local, but separable potential, the bound-free dipole and the re-scattering transition matrix elements are analytically computed. In comparison with the standard approaches to the ATI process, our analytical derivation of the re-scattering matrix elements allows us to study directly how the re-scattering process depends on the atomic target and laser pulse features -we can turn on and off contributions having different physical origins or corresponding to different physical mechanisms. We compare SFA results with the full numerical solutions of the time-dependent Schroedinger equation (TDSE) within the few-cycle pulse regime. Good agreement between our SFA and TDSE model is found for the ATI spectrum. Our model captures also the strong dependence of the photoelectron spectra on the carrier envelope phase of the laser field.

physics.atom-ph↗

arXiv2015

Strong-field physics with mid-IR fields

Strong-field physics is currently experiencing a shift towards the use of mid-IR driving wavelengths. This is because they permit conducting experiments unambiguously in the quasi-static regime and enable exploiting the effects related to ponderomotive scaling of electron recollisions. Initial measurements taken in the mid-IR immediately led to a deeper understanding of photo-ionization and allowed a discrimination amongst different theoretical models. Ponderomotive scaling of rescattering has enabled new avenues towards time resolved probing of molecular structure. Essential for this paradigm shift was the convergence of two experimental tools: 1) intense mid-IR sources that can create high energy photons and electrons while operating within the quasi-static regime, and 2) detection systems that can detect the generated high energy particles and image the entire momentum space of the interaction in full coincidence. Here we present a unique combination of these two essential ingredients, namely a 160kHz mid-IR source and a reaction microscope detection system, to present an experimental methodology that provides an unprecedented three-dimensional view of strong-field interactions. The system is capable of generating and detecting electron energies that span a six order of magnitude dynamic range. We demonstrate the versatility of the system by investigating electron recollisions, the core process that drives strong-field phenomena, at both low (meV) and high (hundreds of eV) energies. The low energy region is used to investigate recently discovered low-energy structures, while the high energy electrons are used to probe atomic structure via laser-induced electron diffraction. Moreover we present, for the first time, the correlated momentum distribution of electrons from non-sequential double-ionization driven by mid-IR pulses.

physics.atom-ph↗

arXiv2015

Imaging an aligned polyatomic molecule with laser-induced electron diffraction

Laser-induced electron diffraction is an evolving tabletop method, which aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolution. Here, we provide the general foundation for the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based upon the combination of a 160 kHz mid-IR few-cycle laser source with full three-dimensional electron-ion coincidence detection. Our technique provides an accessible and robust route towards imaging ultrafast processes in complex gas phase molecules with atto- to femto-second temporal resolution.

physics.atom-ph↗

arXiv2014

Spatio-temporal isolation of attosecond soft X-ray pulses in the water window

We demonstrate experimentally the isolation of single attosecond pulses at the carbon K- shell edge in the soft-X-ray water window. Attosecond pulses at photon energies that cover the principal absorption edges of the building blocks of materials are a prerequisite for time resolved probing of the triggering events leading to electronic dynamics such as exciton formation and annihilation. Herewith, we demonstrate successful isolation of individual attosecond pulses at the carbon K edge (284 eV) with a pulse duration below 400 as and with a bandwidth supporting a 30 as pulse duration. Our approach is based on spatio-temporal isolation of ponderomotively shifted harmonics and validates a straightforward and scalable approach for robust and reproducible attosecond pulse isolation.

physics.optics↗

arXiv2014

Formation of very low energy states crossing the ionization threshold of argon atoms in strong mid-infrared fields

Atomic ionization by intense mid-infrared (mid-IR) pulses produces low electron energy features that the strong-field approximation, which is expected to be valid in the tunneling ionization regime characterized by small Keldysh parameters ($γ\ll 1$), cannot describe. These features include the low-energy structure (LES), the very-low-energy structure (VLES), and the more recently found zero-energy structure (ZES). They result from the interplay between the laser electric field and the atomic Coulomb field which controls the low-energy spectrum also for small $γ$. In the present joint experimental and theoretical study we investigate the vectorial momentum spectrum at very low energies. Using a reaction microscope optimized for the detection of very low energy electrons, we have performed a thorough study of the three-dimensional momentum spectrum well below 1 eV. Our measurements are complemented by quantum and classical simulations, which allow for an interpretation of the LES, VLES and of the newly identified ZES in terms of two-dimensional Coulomb focusing and recapture into Rydberg states, respectively.

physics.atom-ph↗