arXiv subjects

Joachim Burgdörfer

Publications and source records attributed to Joachim Burgdörfer.

At least 37 records · Page 2Linked to original sources

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

Long-time expansion of a Bose-Einstein condensate: Can Anderson localization be observed?

We numerically explore the long-time expansion of a one-dimensional Bose-Einstein condensate in a disorder potential employing the Gross-Pitaevskii equation. The goal is to search for unique signatures of Anderson localization in the presence of particle-particle interactions. Using typical experimental parameters we show that the time scale for which the non-equilibrium dynamics of the interacting system begins to diverge from the non-interacting system exceeds the observation times up to now accessible in the experiment. We find evidence that the long-time evolution of the wavepacket is characterized by (sub)diffusive spreading and a growing effective localization length suggesting that interactions destroy Anderson localization.

cond-mat.quant-gas↗

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

Accurate high-harmonic spectra from time-dependent two-particle reduced density matrix theory

The accurate description of the non-linear response of many-electron systems to strong-laser fields remains a major challenge. Methods that bypass the unfavorable exponential scaling with particle number are required to address larger systems. In this paper we present a fully three-dimensional implementation of the time-dependent two-particle reduced density matrix (TD-2RDM) method for many-electron atoms. We benchmark this approach by a comparison with multi-configurational time-dependent Hartree-Fock (MCTDHF) results for the harmonic spectra of beryllium and neon. We show that the TD-2RDM is very well-suited to describe the non-linear atomic response and to reveal the influence of electron-correlation effects.

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

Electrostatically confined monolayer graphene quantum dots with orbital and valley splittings

The electrostatic confinement of massless charge carriers is hampered by Klein tunneling. Circumventing this problem in graphene mainly relies on carving out nanostructures or applying electric displacement fields to open a band gap in bilayer graphene. So far, these approaches suffer from edge disorder or insufficiently controlled localization of electrons. Here we realize an alternative strategy in monolayer graphene, by combining a homogeneous magnetic field and electrostatic confinement. Using the tip of a scanning tunneling microscope, we induce a confining potential in the Landau gaps of bulk graphene without the need for physical edges. Gating the localized states towards the Fermi energy leads to regular charging sequences with more than 40 Coulomb peaks exhibiting typical addition energies of 7-20 meV. Orbital splittings of 4-10 meV and a valley splitting of about 3 meV for the first orbital state can be deduced. These experimental observations are quantitatively reproduced by tight binding calculations, which include the interactions of the graphene with the aligned hexagonal boron nitride substrate. The demonstrated confinement approach appears suitable to create quantum dots with well-defined wave function properties beyond the reach of traditional techniques.

cond-mat.mes-hall↗

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

Anomalous Fano Profiles in External Fields

We show that external control of Fano resonances in general leads to complex Fano $q$-parameters. Fano line shapes of photo-electron and transient absorption spectra in presence of an infrared control field are investigated. Computed transient absorption spectra are compatible with a recent experiment [C. Ott {\it et al.}, Science 340, 716 (2013)] but suggest a modification of the interpretation proposed there. Control mechanisms for photo-electron spectra are exposed: control pulses applied {\em during} excitation modify the line shapes by momentum boosts of the continuum electrons. Pulses arriving {\em after} excitation generate interference fringes due to infrared two-photon transitions.

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

Probing time-ordering in two-photon double ionization of helium on the attosecond time scale

We show that time ordering underlying time-dependent quantum dynamics is a physical observable accessible by attosecond streaking. We demonstrate the extraction of time ordering for the prototypical case of time-resolved two-photon double ionization (TPDI) of helium by an attosecond XUV pulse. The Eisenbud-Wigner-Smith time delay for the emission of a two-electron wavepacket and the time interval between subsequent emission events can be unambiguously determined by attosecond streaking. The delay between the two emission events sensitively depends on the energy, pulse duration, and angular distribution of the emitted electron pair. Our fully-dimensional ab-initio quantum mechanical simulations provide benchmark data for experimentally accessible observables.

physics.atom-ph↗

arXiv2014

Propagating two-particle reduced density matrices without wavefunctions

Describing time-dependent many-body systems where correlation effects play an important role remains a major theoretical challenge. In this paper we develop a time-dependent many-body theory that is based on the two-particle reduced density matrix (2-RDM). We develop a closed equation of motion for the 2-RDM employing a novel reconstruction functional for the three-particle reduced density matrix (3-RDM) that preserves norm, energy, and spin symmetries during time propagation. We show that approximately enforcing $N$-representability during time evolution is essential for achieving stable solutions. As a prototypical test case which features long-range Coulomb interactions we employ the one-dimensional model for lithium hydride (LiH) in strong infrared laser fields. We probe both one-particle observables such as the time-dependent dipole moment and two-particle observables such as the pair density and mean electron-electron interaction energy. Our results are in very good agreement with numerically exact solutions for the $N$-electron wavefunction obtained from the multiconfigurational time-dependent Hartree-Fock method.

physics.atom-ph↗

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↗

arXiv2014

Photovoltaic effect in an electrically tunable van der Waals heterojunction

Semiconductor heterostructures form the cornerstone of many electronic and optoelectronic devices and are traditionally fabricated using epitaxial growth techniques. More recently, heterostructures have also been obtained by vertical stacking of two-dimensional crystals, such as graphene and related two- dimensional materials. These layered designer materials are held together by van der Waals forces and contain atomically sharp interfaces. Here, we report on a type- II van der Waals heterojunction made of molybdenum disulfide and tungsten diselenide monolayers. The junction is electrically tunable and under appropriate gate bias, an atomically thin diode is realized. Upon optical illumination, charge transfer occurs across the planar interface and the device exhibits a photovoltaic effect. Advances in large-scale production of two-dimensional crystals could thus lead to a new photovoltaic solar technology.

cond-mat.mes-hall↗

arXiv2014

Characterizing wave functions in graphene nanodevices: electronic transport through ultrashort graphene constrictions on a boron nitride substrate

We present electronic transport measurements through short and narrow (30x30 nm) single layer graphene constrictions on a hexagonal boron nitride substrate. While the general observation of Coulomb-blockade is compatible with earlier work, the details are not: we show that the area on which charge is localized can be significantly larger than the area of the constriction, suggesting that the localized states responsible for Coulomb-blockade leak out into the graphene bulk. The high bulk mobility of graphene on hexagonal boron nitride, however, seems not consistent with the short bulk localization length required to see Coulomb-blockade. To explain these findings, charge must instead be primarily localized along the imperfect edges of the devices and extend along the edge outside of the constriction. In order to better understand the mechanisms, we compare the experimental findings with tight-binding simulations of such constrictions with disordered edges. Finally we discuss previous experiments in the light of these new findings.

cond-mat.mes-hall↗