arXiv subjects

Christoph Lemell

Publications and source records attributed to Christoph Lemell.

At least 19 recordsLinked to original sources

arXiv2021

Influence of coherent vibronic excitation on the high harmonics generation of diatomic molecules

The generation of high harmonics (HHG) in atomic systems by the highly non-linear response to an intense laser field is a prominent pathway to the synthesis of ever shorter laser pulses at increasingly higher photon energies. Extensions of this process to molecules add to the complexity but also offers novel opportunities as multi-center effects and the coupling to nuclear degrees of freedom can influence HHG. In this work we theoretically explore the impact of coherent vibronic excitations of diatomic molecules on the HHG spectrum within the framework of time-dependent density functional theory. We observe the appearance of novel interference structures in the HHG spectra controlled by resonances between the driving field and the vibronic wavepacket.

physics.atom-ph↗

arXiv2020

60 years of attosecond physics at ICPEAC: from collisions to ultrashort pulses

The field of attosecond physics has seen an almost explosive growth since the early 2000's and represents by now an increasing fraction of contributions to the bi-annual series of International Conferences of Photonic, Electronic, and Atomic Collisions (ICPEAC). The latter is anything but a coincidence as many of the underlying concepts of electronic and photonic dynamics are closely intertwined with atomic-scale collision processes. We illustrate this fruitful connection and its implications with the help of a few prototypical examples of current topical interest.

quant-ph↗

arXiv2019

Energy of the $^{229}$Th nuclear clock transition

The first nuclear excited state of $^{229}$Th offers the unique opportunity for laser-based optical control of a nucleus. Its exceptional properties allow for the development of a nuclear optical clock which offers a complementary technology and is expected to outperform current electronic-shell based atomic clocks. The development of a nuclear clock was so far impeded by an imprecise knowledge of the energy of the $^{229}$Th nuclear excited state. In this letter we report a direct excitation energy measurement of this elusive state and constrain this to 8.28$\pm$0.17 eV. The energy is determined by spectroscopy of the internal conversion electrons emitted in-flight during the decay of the excited nucleus in neutral $^{229}$Th atoms. The nuclear excitation energy is measured via the valence electronic shell, thereby merging the fields of nuclear- and atomic physics to advance precision metrology. The transition energy between ground and excited state corresponds to a wavelength of 149.7$\pm$3.1 nm. These findings set the starting point for high-resolution nuclear laser spectroscopy and thus the development of a nuclear optical clock of unprecedented accuracy. A nuclear clock is expected to have a large variety of applications, ranging from relativistic geodesy over dark matter research to the observation of potential temporal variation of fundamental constants.

nucl-ex↗

arXiv2017

Ab-initio multi-scale simulation of high-harmonic generation in solids

High-harmonic generation by a highly non-linear interaction of infrared laser fields with matter allows for the generation of attosecond pulses in the XUV spectral regime. This process, well established for atoms, has been recently extended to the condensed phase. Remarkably well pronounced harmonics up to order ~30 have been observed for dielectrics. We present the first ab-initio multi-scale simulation of solid-state high-harmonic generation. We find that mesoscopic effects of the extended system, in particular the realistic sampling of the entire Brillouin zone, the pulse propagation in the dense medium, and the inhomogeneous illumination of the crystal have a strong effect on the formation of clean harmonic spectra. Our results provide a novel explanation for the formation of clean harmonics and have implications for a wide range of non-linear optical processes in dense media.

physics.optics↗

arXiv2017

High Visibility in Two-Color Above-Threshold Photoemission from Tungsten Nanotips in a Coherent Control Scheme

In this article we present coherent control of above-threshold photoemission from a tungsten nanotip achieving nearly perfect modulation. Depending on the pulse delay between fundamental (1560 nm) and second harmonic (780 nm) pulses of a femtosecond fiber laser at the nanotip, electron emission is significantly enhanced or depressed during temporal overlap. Electron emission is studied as a function of pulse delay, optical near-field intensities, DC bias field, and final photoelectron energy. Under optimized conditions modulation amplitudes of the electron emission of 97.5% are achieved. Experimental observations are discussed in the framework of quantum- pathway interference supported by local density of states (LDOS) simulations.

physics.optics↗

arXiv2017

Localizing High-Lying Rydberg Wave Packets with Two-Color Laser Fields

We demonstrate control over the localization of high-lying Rydberg wave packets in argon atoms with phase-locked orthogonally polarized two-color (OTC) laser fields. With a reaction microscope, we measured ionization signals of high-lying Rydberg states induced by a weak dc field and black-body radiation as a function of the relative phase between the two-color fields. We find that the dc-field ionization yields of high-lying Rydberg argon atoms oscillate with the relative two-color phase with a period of $2π$ while the photoionization signal by black-body radiation shows a period of $π$. These observations are a clear signature of the asymmetric localization of electrons recaptured into high-lying Rydberg states after conclusion of the laser pulse and are supported by a semiclassical simulation of argon-OTC laser interaction. Our findings thus open an effective pathway to control the localization of high-lying Rydberg wave packets.

physics.atom-ph↗

arXiv2016

Two-color coherent control of femtosecond above-threshold photoemission from a tungsten nanotip

We demonstrate coherent control of multiphoton and above-threshold photoemission from a single solid-state nanoemitter driven by a fundamental and a weak second harmonic laser pulse. Depending on the relative phase of the two pulses, electron emission is modulated with a contrast of the oscillating current signal of up to 94%. Electron spectra reveal that all observed photon orders are affected simultaneously and similarly. We confirm that photoemission takes place within 10 fs. Accompanying simulations indicate that the current modulation with its large contrast results from two interfering quantum pathways leading to electron emission.

physics.optics↗

arXiv2016

Coincidence spectroscopy of high-lying Rydberg states produced in strong laser fields

We report on the measurement of electron emission after the interaction of strong laser pulses with atoms and molecules. These electrons originate from high-lying Rydberg states with quantum numbers up to $n \lesssim 120$ formed by frustrated field ionization. Simulations show that both tunneling ionization by a weak dc field and photoionization by the black-body radiation contribute to delayed electron emission on the nano- to microsecond scale. We measured ionization rates from these Rydberg states by coincidence spectroscopy. Further, the dependence of the Rydberg-state production on the ellipticity of the driving laser field proves that such high-lying Rydberg states are populated through electron recapture. The present experiment provides detailed quantitative information on Rydberg production by frustrated field ionization.

physics.atom-ph↗

arXiv2015

Observation of molecular dipole excitations by attosecond self-streaking

We propose a protocol to probe the ultrafast evolution and dephasing of coherent electronic excitation in molecules in the time domain by the intrinsic streaking field generated by the molecule itself. Coherent electronic motion in the endohedral fullerene \Necsixty~is initiated by a moderately intense femtosecond UV-VIS pulse leading to coherent oscillations of the molecular dipole moment that persist after the end of the laser pulse. The resulting time-dependent molecular near-field is probed through the momentum modulation of photoemission from the central neon atom by a time-delayed attosecond XUV pulse. Our ab-initio time-dependent density functional theory and classical trajectory simulations predict that this self-streaking signal accurately traces the molecular dipole oscillations in real time. We discuss the underlying processes and give an analytical model that captures the essence of our ab-initio simulations.

physics.optics↗

arXiv2015

Controlling ultrafast currents by the non-linear photogalvanic effect

We theoretically investigate the effect of broken inversion symmetry on the generation and control of ultrafast currents in a transparent dielectric (SiO2) by strong femto-second optical laser pulses. Ab-initio simulations based on time-dependent density functional theory predict ultrafast DC currents that can be viewed as a non-linear photogalvanic effect. Most surprisingly, the direction of the current undergoes a sudden reversal above a critical threshold value of laser intensity I_c ~ 3.8*10^13 W/cm2. We trace this switching to the transition from non-linear polarization currents to the tunneling excitation regime. We demonstrate control of the ultrafast currents by the time delay between two laser pulses. We find the ultrafast current control by the non-linear photogalvanic effect to be remarkably robust and insensitive to laser-pulse shape and carrier-envelope phase.

physics.optics↗

arXiv2015

Large optical field enhancement for nanotips with large opening angles

We theoretically investigate the dependence of the enhancement of optical near-fields at nanometric tips on the shape, size, and material of the tip. We confirm a strong dependence of the field enhancement factor on the radius of curvature. In addition, we find a surprisingly strong increase of field enhancement with increasing opening angle of the nanotips. For gold and tungsten nanotips in the experimentally relevant parameter range (radius of curvature $\geq 5\,$nm at $800\,$nm laser wavelength), we obtain field enhancement factors of up to ${\sim}35$ for Au and ${\sim}12$ for W for large opening angles. We confirm this strong dependence on the opening angle for many other materials featuring a wide variety in their dielectric response. For dielectrics, the opening angle dependence is traced back to the electrostatic force of the induced surface charge at the tip shank. For metals, the plasmonic response strongly increases the field enhancement and shifts the maximum field enhancement to smaller opening angles.

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↗

arXiv2014

Ab Initio Simulation of Electrical Currents Induced by Ultrafast Laser Excitation of Dielectric Materials

We theoretically investigate the generation of ultrafast currents in insulators induced by strong few-cycle laser pulses. Ab initio simulations based on time-dependent density functional theory give insight into the atomic-scale properties of the induced current signifying a femtosecond-scale insulator-metal transition. We observe the transition from nonlinear polarization currents during the laser pulse at low intensities to tunnelinglike excitation into the conduction band at higher laser intensities. At high intensities, the current persists after the conclusion of the laser pulse considered to be the precursor of the dielectric breakdown on the femtosecond scale. We show that the transferred charge sensitively depends on the orientation of the polarization axis relative to the crystal axis suggesting that the induced charge separation reflects the anisotropic electronic structure. We find good agreement with very recent experimental data on the intensity and carrierenvelope phase dependence [A. Schiffrin et al., Nature (London) 493, 70 (2013)].

cond-mat.mtrl-sci↗

arXiv2013

Electron rescattering at metal nanotips induced by ultrashort laser pulses

We theoretically investigate the interaction of moderate intensity near-infrared few cycle laser pulses with nano-scale metal tips. Local field enhancement in a nanometric region around the tip apex triggers coherent electron emission on the nanometer length and femtosecond time scale. The quantum dynamics at the surface are simulated with time-dependent density functional theory (TDDFT) and interpreted based on the simple man's model. We investigate the dependence of the emitted electron spectra on the laser wavelength.

cond-mat.mes-hall↗

arXiv2012

Electron rescattering at metal nanotips induced by ultrashort laser pulses

We report on the first investigation of plateau and cut-off structures in photoelectron spectra from nano-scale metal tips interacting with few-cycle near-infrared laser pulses. These hallmarks of electron rescattering, well-known from atom-laser interaction in the strong-field regime, appear at remarkably low laser intensities with nominal Keldysh parameters of the order of $\gtrsim 10$. Quantum and quasi-classical simulations reveal that a large field enhancement near the tip and the increased backscattering probability at a solid-state target play a key role. Plateau electrons are by an order of magnitude more abundant than in comparable atomic spectra, reflecting the high density of target atoms at the surface. The position of the cut-off serves as an in-situ probe for the locally enhanced electric field at the tip apex.

physics.optics↗

arXiv2011

Probing scattering phase shifts by attosecond streaking

Attosecond streaking is one of the most fundamental processes in attosecond science allowing for a mapping of temporal (i.e. phase) information on the energy domain. We show that on the single-particle level attosecond streaking time shifts contain spectral phase information associated with the Eisenbud-Wigner-Smith (EWS) time delay, provided the influence of the streaking infrared field is properly accounted for. While the streaking phase shifts for short-ranged potentials agree with the associated EWS delays, Coulomb potentials require special care. We show that the interaction between the outgoing electron and the combined Coulomb and IR laser fields lead to a streaking phase shift that can be described classically.

physics.atom-ph↗

arXiv2011

Low-energy peak structure in strong-field ionization by mid-infrared laser-pulses: two-dimensional focusing by the atomic potential

We analyze the formation of the low-energy structure (LES) in above-threshold ionization spectra first observed by Quan et al.\ \cite{quan09} and Blaga et al.\ \cite{blaga09} using both quasi-classical and quantum approaches. We show this structure to be largely classical in origin resulting from a two-dimensional focusing in the energy-angular momentum plane of the strong-field dynamics in the presence of the atomic potential. The peak at low energy is strongly correlated with high angular momenta of the photoelectrons. Quantum simulations confirm this scenario. Resulting parameter dependences agree with experimental findings \cite{quan09,blaga09} and, in part, with other simulations \cite{liu10,yan10,kast11}.

physics.atom-ph↗

arXiv2011

Time-resolved photoemission by attosecond streaking: extraction of time information

Attosecond streaking of atomic photoemission holds the promise to provide unprecedented information on the release time of the photoelectron. We show that attosecond streaking phase shifts indeed contain timing (or spectral phase) information associated with the Eisenbud-Wigner-Smith time delay matrix of quantum scattering. However, this is only accessible if the influence of the streaking infrared (IR) field on the emission process is properly accounted for. The IR probe field can strongly modify the observed streaking phase shift. We show that the part of the phase shift ("time shift") due to the interaction between the outgoing electron and the combined Coulomb and IR laser fields can be described classically. By contrast, the strong initial-state dependence of the streaking phase shift is only revealed through the solution of the time-dependent Schrödinger equation in its full dimensionality. We find a time delay between the hydrogenic 2s and 2p initial states in He+ exceeding 20as for a wide range of IR intensities and XUV energies.

physics.atom-ph↗