arXiv subjects

Ulf Saalmann

Publications and source records attributed to Ulf Saalmann.

At least 19 recordsLinked to original sources

arXiv2026

Sensing coherent phonon dynamics in solids with delayed even harmonics

High harmonics have emerged as a powerful ultrafast probe of phonon dynamics and electron-phonon interactions in solids, with most studies focusing on odd harmonics. Here, in a pump-probe setup with variable delay, we theoretically investigate how even harmonics reveal coherent phonon dynamics. If pump and probe pulses overlap temporally, the spatial interference effect resulting from a non-coaxial pump-probe setup suppresses harmonic yields. At longer delays, odd-harmonic yields oscillate in phase at the optical phonon frequency, whereas even harmonics exhibit order-dependent phase-shifted oscillations. We identify a responsive range of even harmonic orders, in which the delay of yield oscillations is highly sensitive to subtle features of phonon dynamics and electron-electron interactions. Our findings highlight the potential of even harmonics to elucidate microscopic effects in systems with dynamically broken inversion symmetry.

physics.optics↗

arXiv2024

Zero-energy photoelectric effect

We predict a near-threshold ("zero energy") peak in multi-photon ionization for a dynamical regime where the photon frequency is large compared to the binding energy of the electron. The peak position does not depend on the laser frequency, but on the binding energy and the pulse duration. The effect originates from the fact that bound-continuum dipole transitions are stronger than continuum-continuum ones. To clearly observe this zero-energy photoelectric effect, the spectral width of the laser pulse should be comparable to the binding energy of the ionized orbital, and the second ionization potential should be larger than the photon energy. This suggests negative ions as ideal candidates for corresponding experiments.

physics.atom-ph↗

arXiv2024

Roadmap on Data-Centric Materials Science

Science is and always has been based on data, but the terms "data-centric" and the "4th paradigm of" materials research indicate a radical change in how information is retrieved, handled and research is performed. It signifies a transformative shift towards managing vast data collections, digital repositories, and innovative data analytics methods. The integration of Artificial Intelligence (AI) and its subset Machine Learning (ML), has become pivotal in addressing all these challenges. This Roadmap on Data-Centric Materials Science explores fundamental concepts and methodologies, illustrating diverse applications in electronic-structure theory, soft matter theory, microstructure research, and experimental techniques like photoemission, atom probe tomography, and electron microscopy. While the roadmap delves into specific areas within the broad interdisciplinary field of materials science, the provided examples elucidate key concepts applicable to a wider range of topics. The discussed instances offer insights into addressing the multifaceted challenges encountered in contemporary materials research.

cond-mat.mtrl-sci↗

arXiv2024

Strong-field quantum control in the extreme ultraviolet using pulse shaping

Tailored light-matter interactions in the strong coupling regime enable the manipulation and control of quantum systems with up to unit efficiency, with applications ranging from quantum information to photochemistry. While strong light-matter interactions are readily induced at the valence electron level using long-wavelength radiation, comparable phenomena have been only recently observed with short wavelengths, accessing highly-excited multi-electron and inner-shell electron states. However, the quantum control of strong-field processes at short wavelengths has not been possible, so far, due to the lack of pulse shaping technologies in the extreme ultraviolet (XUV) and X-ray domain. Here, exploiting pulse shaping of the seeded free-electron laser (FEL) FERMI, we demonstrate the strong-field quantum control of ultrafast Rabi dynamics in helium atoms with high fidelity. Our approach unravels a strong dressing of the ionization continuum, otherwise elusive to experimental observables. The latter is exploited to achieve control of the total ionization rate, with prospective applications in many XUV and soft X-ray experiments. Leveraging recent advances in intense few-femtosecond to attosecond XUV to soft X-ray light sources, our results open an avenue to the efficient manipulation and selective control of core electron processes and electron correlation phenomena in real time.

physics.atom-ph↗

arXiv2023

Time delays in anisotropic systems

Scattering properties and time delays for general (non-symmetric) potentials in terms of the respective S-matrices are discussed paradigmatically in one dimension and in comparison to symmetric potentials. Only for the latter the Wigner and Smith time delays coincide. Considering asymmetric potentials also reveals that only one version of S-matrices used in the literature (the one with reflection coefficients on the diagonal) generalizes to the asymmetric case. Finally, we give a criterion how to identify a potential with intrinsic symmetry which behaves like an asymmetric one if it is merely offset from the scattering center.

quant-ph↗

arXiv2023

Strong-field photoionization by circularly polarized light

We demonstrate that strong-field ionization of atoms driven by circularly polarized light becomes an adiabatic process when described in the frame rotating with the laser field. As a direct consequence, a conservation law emerges: in the rotating frame the energy of the tunneling electron is conserved for rotationally invariant potentials. This conservation law, arising from a classical picture, is retrieved through a proper classical-quantum correspondence when considering the full quantum system, beyond the Strong Field Approximation.

physics.atom-ph↗

arXiv2022

Symmetry-induced decoherence-free subspaces

Preservation of coherence is a fundamental yet subtle phenomenon in open systems. We uncover its relation to symmetries respected by the system Hamiltonian and its coupling to the environment. We discriminate between local and global classes of decoherence-free subspaces for many-body systems through the introduction of "ghost variables". The latter are orthogonal to the symmetry and the coupling to the environment does not depend on them. Constructing them is facilitated in classical phase space and can be transferred to quantum mechanics through the equivalent role that Poisson and Lie algebras play for symmetries in classical and quantum mechanics, respectively. Examples are given for an interacting spin system.

physics.atom-ph↗

arXiv2022

Enhanced high-order harmonics through periodicity breaks: from backscattering to impurity states

Backscattering of delocalized electrons has been recently established [Phys. Rev. A 105, L041101 (2022)] as a mechanism to enhance high-order harmonic generation (HHG) in periodic systems with broken translational symmetry. Here we study this effect for a variable spatial gap in an atomic chain. Propagating the many-electron dynamics numerically, we find enhanced HHG and identify its origin in two mechanisms, depending on the gap size, either backscattering or enhanced tunneling from an impurity state. Since the gapped atomic chain exhibits both impurities and vacancies in a unified setting, it provides insight how periodicity breaks influence HHG in different scenarios.

physics.atom-ph↗

arXiv2022

High harmonics from backscattering of delocalized electrons

It is shown that electron backscattering can enhance high-harmonic generation in periodic systems with broken translational symmetry. Paradigmatically, we derive for a finite chain of atoms the harmonic cutoff due to electrons backscattered from the edges of the chain and demonstrate a maximum in the harmonic yield if twice the quiver amplitude of the driven electrons equals the chain length. For an intuitive understanding of our quantum results we develop a refined semiclassical trajectory model with finite electron-hole separation after tunneling. We demonstrate that the same "tunnel exit" also holds for interband harmonics in conventional periodic solid-state systems.

physics.atom-ph↗

arXiv2021

Intense-pulse dynamics of massless Dirac electrons

We identify and describe how intense short light pulses couple to massless Dirac fermions in two-dimensional systems. The ensuing excitation dynamics exhibits unusual scaling with the wavelength of the light due the linear dispersion of the band structure and the fact that light coupling is efficient only close to the Dirac points. We exploit these features to achieve valley polarization of more than 70 % with simple pulse shapes. Quantitative results are given for pristine graphene.

cond-mat.mes-hall↗

arXiv2021

Non-adiabatic ionization with tailored laser pulses

Non-adiabatic photo-ionization is difficult to control as it relies on the derivatives of the envelope and not on phase-details of the short ionizing pulse. Here, we introduce a catalyzing state, whose presence render non-adiabatic ionization sensitive to phase-details of tailored pulses. Since a catalyzing state is in general easy to create, this opens a perspective for coherent control of ultra-fast ionization.

physics.atom-ph↗

arXiv2021

Semiclassical Lindblad master equation for spin dynamics

We derive the semi-classical Lindblad master equation in phase space for both canonical and non-canonical Poisson brackets using the Wigner-Moyal formalism and the Moyal star-product. The semi-classical limit for canonical dynamical variables, i.e., canonical Poisson brackets, is the Fokker-Planck equation, as derived before. We generalize this limit and show that it holds also for non-canonical Poisson brackets. Examples are gyro-Poisson brackets, which occur in spin ensembles, systems of recent interest in atomic physics and quantum optics. We show that the equations of motion for the collective spin variables are given by the Bloch equations of nuclear magnetization with relaxation. The Bloch and relaxation vectors are expressed in terms of the microscopic operators: The Hamiltonian and the Lindblad functions in the Wigner-Moyal formalism.

physics.atom-ph↗

arXiv2020

Perspectives for analyzing non-linear photo ionization spectra with deep neural networks trained with synthetic Hamilton matrices

We have constructed deep neural networks, which can map fluctuating photo-electron spectra obtained from noisy pulses to spectra from noise-free pulses. The network is trained on spectra from noisy pulses in combination with random Hamilton matrices, representing systems which could exist but do not necessarily exist. In [Giri et al., Phys. Rev. Lett. 124,113201 (2020)] we performed a purification of fluctuating spectra, that is mapping them to those from Fourier-limited Gaussian pulses. Here, we investigate the performance of such neural-network-based maps for predicting spectra of double pulses, pulses with a chirp and even partially-coherent pulses pulses from fluctuating spectra generated by noisy pulses. Secondly, we demonstrate that along with a purification of a fluctuating double-pulse spectrum, one can estimate the time-delay of the underlying double pulse, an attractive feature for single-shot spectra from SASE FELs. We demonstrate our approach with resonant two-photon ionization, a non-linear process, sensitive to details of the laser pulse.

physics.atom-ph↗

arXiv2020

Proper time delays measured by optical streaking

The generation of a streaking spectrogram is based on energy absorption from the streaking laser. Investigating this absorption we show rigorously under which condition the measured time shift is independent of properties of the streaking light. In this case it provides the Wigner-Smith time delay. The latter is infinite for systems with a long-range potential tail, such as Coulomb systems. Here, we suggest to determine the time delay relative to pure hydrogen for meaningful results. Finite delays obtained so far for Coulombic systems without the hydrogen reference are the consequence of a finite streaking frequency and depend on its value as well as on the electron's excess energy. Our analysis also suggests a time-delay measurement technique that avoids the record of a complete streaking scan.

physics.atom-ph↗

arXiv2020

Purifying electron spectra from noisy pulses with machine learning using synthetic Hamilton matrices

Photo-electron spectra obtained with intense pulses generated by free-electron lasers through self-amplified spontaneous emission are intrinsically noisy and vary from shot to shot. We extract the purified spectrum, corresponding to a Fourier-limited pulse, with the help of a deep neural network. It is trained on a huge number of spectra, which was made possible by an extremely efficient propagation of the Schrödinger equation with synthetic Hamilton matrices and random realizations of fluctuating pulses. We show that the trained network is sufficiently generic such that it can purify atomic or molecular spectra, dominated by resonant two- or three-photon ionization, non-linear processes which are particularly sensitive to pulse fluctuations. This is possible without training on those systems.

physics.atom-ph↗

arXiv2018

Adiabatic passage to the continuum

We demonstrate that by changing the direction of the chirp in VUV pulses one can switch between excitation and ionization with very high contrast, if the carrier frequency of the light is resonant with two bound states. This is a surprising consequence if rapid adiabatic passage is extended to include transitions to the continuum. The chirp phase locks the linear combination of two resonantly coupled bound states whose ionization amplitudes interfere constructively or destructively depending on the chirp direction under suitable conditions. We derive the phenomenon in a minimal model and verify the effect with calculations for helium as a realistic example.

physics.atom-ph↗

arXiv2018

Floquet approach for dynamics in short and intense laser pulses

We present a two-timescale Floquet method that allows one to apply the Kramers-Henneberger approach to short pulses and arbitrary laser frequencies. An efficient numerical procedure to propagate the Floquet Hamiltonian is provided that relies on the Toeplitz matrix formalism and Fast Fourier Transformations. It enables efficient time propagation with large Floquet expansions, while still taking advantage of the cycle-averaged Kramers-Henneberger basis. Three illustrative cases of ionization with different photon energies are analyzed, where the envelope of a short and intense pulse is crucial to the underlying dynamics.

physics.atom-ph↗

arXiv2018

Electron dynamics driven by light pulse derivatives

We demonstrate that ultrashort pulses carry the possibility for a new regime of light-matter interaction with nonadiabatic electron processes sensitive to the envelope-derivative of the light pulse. A standard single pulse with its two peaks in the derivative separated by the width of the pulse acts in this regime like a traditional double pulse. The two ensuing nonadiabatic ionization bursts have slightly different ionization amplitudes. This difference is due to redistribution of continuum electron energy during the bursts, negligible in standard photo-ionization. A time-dependent close- coupling approach based on cycle-averaged potentials in the Kramers-Henneberger reference frame permits a detailed understanding of light pulse derivative-driven electron dynamics.

physics.optics↗