arXiv subjects

Mette B. Gaarde

Publications and source records attributed to Mette B. Gaarde.

At least 19 recordsLinked to original sources

arXiv2026

Carrier-Resolved Attosecond Valley Polarimetry of Monolayer MoS$_2$

In recent years, all-optical writing and switching of valley polarization in two-dimensional semiconductors has been demonstrated on femtosecond timescales. Reading this polarization out on the same timescale, carrier by carrier, has so far remained out of reach. Employing semiconductor Bloch equation simulations of monolayer MoS$_2$, we show that attosecond transient absorption closes this gap by turning the Mo $4p$ semicore edge into a quantitative valley polarimeter. We find that pump-enabled core-to-valence absorption probes the holes while core-to-conduction bleaching probes the electrons, so that a single spectrum identifies each carrier by its photoabsorption energy. The hole channel, Pauli-blocked in equilibrium, emerges background-free. Its circular dichroism reverses sign with the pump helicity, and its normalized magnitude is proportional to the valley polarization. Finally, we show that scanning the probe delay clocks the few-femtosecond write in real time. Thus, attosecond core-level dichroism is a carrier-sensitive, quantitative probe of the creation and evolution of valley polarization.

cond-mat.mes-hall↗

arXiv2025

Redirection and Reshaping of Intense Extreme-Ultraviolet Radiation

The goal to control short-wavelength radiation for the investigation and manipulation of ultrafast dynamics in quantum systems coevolves with the growing availability of extreme-ultraviolet (XUV) and x-ray sources from high-harmonic generation and free-electron lasers. Here, we present an XUV spatio-spectral phase modulator based on an intense XUV laser beam propagating through an optically thick resonant target, introducing dispersion profile variations around the resonance both perpendicular to and along the laser propagation direction. The resulting dipole radiation gets spectrally reshaped and becomes more divergent as compared to the original beam in the far field. As an experimental demonstration, the intense-XUV-induced double-peak off-axis structure in the far-field spectrum obtained at the Free-Electron Laser in Hamburg (FLASH) shows indications of the underlying XUV-driven Rabi dynamics and resonant pulse propagation effects. The presented work highlights a ubiquitous phenomenon occurring when an intense laser beam passes through a resonant medium.

physics.atom-ph↗

arXiv2024

Quantitative comparison of TDDFT-calculated HHG yields in ring-shaped organic molecules

We compare the high-harmonic-generation (HHG) yield driven by a mid-infrared laser in three organic ring-shaped molecules, calculated using time-dependent density-functional theory (TDDFT). We average the yield over the relative orientation of the molecules and the linearly-polarized, 1825 nm driving laser pulse in order to compare to experimental spectra obtained by Alharbi et al., Phys. Rev. A 92, 041801 (2015). We find that the raw TDDFT-calculated HHG yield in cyclohexane (CHA) is strongly overestimated compared to those of benzene and cyclohexene, and that this can be attributed to unphysically large contributions from CHA orbitals lying well below the highest-occupied molecular orbital. We show that implementing a simple orbital-resolved scaling factor, which corrects the yield of the tunneling ionization contribution to the first step in the HHG process, leads to much better comparisons with experimental results. Our results are encouraging for the use of TDDFT in systematic computations of HHG in large molecules.

physics.atom-ph↗

arXiv2024

Strong-field ionization with few-cycle, mid-infrared laser pulses induces a localized ionization followed by long-lasting charge migration in halogenated organic molecules

We show that applying a few-femtosecond mid-infrared laser pulse parallel to the backbone of a halogenated, conjugated organic molecule induces localized ionization followed by long-lasting field-free charge migration (CM). Through time-dependent density-functional theory calculations, we find that this CM is robust with respect to the parameters of the applied laser pulse. We document the spatial and temporal origin of the localized hole, which is initiated via strong-field tunnel ionization in the halogen end of the molecule, and near the peak of the laser electric field. In bromobutadiyne we find a range of wavelengths around $1500~\text{nm}$ that consistently leads to the initiation of high-contrast CM. In addition, we show that the inclusion of Ehrenfest nuclear dynamics does not disrupt the creation of the localized hole, nor the subsequent CM motion, in bromobutadiyne or \emph{para}-bromoaniline.

physics.atom-ph↗

arXiv2023

Tracking Charge Migration with Frequency-Matched Strobo-Spectroscopy

We present frequency-matched strobo-spectroscopy (FMSS) of charge migration (CM) in bromobutadiyne, simulated with time-dependent density-functional theory. CM+FMSS is a pump-probe scheme that uses a frequency-matched HHG-driving laser as an independent probe step following the creation of a localized hole on the bromine atom that induces CM dynamics. We show that the delay-dependent harmonic yield tracks the phase of the CM dynamics through its sensitivity to the amount of electron density on the bromine end of the molecule. FMSS takes advantage of the intrinsic attosecond time resolution of the HHG process, in which different harmonics are emitted at different times and thus probe different locations of the electron hole. Finally, we show that the CM-induced modulation of the HHG signal is dominated by the recombination step of the HHG process, with negligible contribution from the ionization step.

physics.atom-ph↗

arXiv2023

Hamiltonian formulation and symplectic split-operator schemes for time-dependent density-functional-theory equations of electron dynamics in molecules

We revisit Kohn-Sham time-dependent density-functional theory (TDDFT) equations and show that they derive from a canonical Hamiltonian formalism. We use this geometric description of the TDDFT dynamics to define families of symplectic split-operator schemes that accurately and efficiently simulate the time propagation for certain classes of DFT functionals. We illustrate these with numerical simulations of the far-from-equilibrium electronic dynamics of a one-dimensional carbon chain. In these examples, we find that an optimized 4th order scheme provides a good compromise between the numerical complexity of each time step and the accuracy of the scheme. We also discuss how the Hamiltonian structure changes when using a basis set to discretize TDDFT and the challenges this raises for using symplectic split-operator propagation schemes.

physics.comp-ph↗

arXiv2022

All-Electron, Density Functional-Based Method for Angle-Resolved Tunneling Ionization in the Adiabatic Regime

We develop and test a method that integrates many-electron weak-field asymptotic theory (ME-WFAT) [Phys. Rev. A 89, 013421 (2014)] in the integral representation (IR) into the density functional theory (DFT) framework. In particular, we present modifications of the integral formula in the IR ME-WFAT to incorporate the potential terms unique to DFT. By solving an adiabatic rate equation for the angle-resolved ionization yield in our DFT-based ME-WFAT method, we show that the results are in excellent agreement with those of real-time time-dependent density functional theory (RT-TDDFT) simulations for NO, OCS, CH$_3$Br, and CH$_3$Cl interacting with one- and two- color laser fields with a fundamental wavelength of $800$ nm. This agreement is significant because the WFAT calculations take only a small fraction of the time of full TDDFT calculations. These results suggest that in the wavelength region commonly used in strong-field experiments ($800$ nm and longer), our DFT-based WFAT treatment can be used to rapidly screen for the ionization properties of a large number of molecules as a function of alignment or orientation between the molecule and the strong field.

physics.atom-ph↗

arXiv2022

Attochemistry Regulation of Charge Migration

Charge migration (CM) is a coherent attosecond process that involves the movement of localized holes across a molecule. To determine the relationship between a molecule's structure and the CM dynamics it exhibits, we perform systematic studies of para-functionalized bromobenzene molecules (X-C$_6$H$_4$-R) using real-time time-dependent density functional theory. We initiate valence-electron dynamics by emulating rapid strong-field ionization leading to a localized hole on the bromine atom. The resulting CM, which takes on the order of 1 fs, occurs via an X localized to C$_6$H$_4$ delocalized to R localized mechanism. Interestingly, the hole contrast on the acceptor functional group increases with increasing electron donating strength. This trend is well-described by the Hammett sigma value of the group, which is a commonly used metric for quantifying the effect of functionalization on the chemical reactivity of benzene derivatives. These results suggest that simple attochemistry principles and a density-based picture can be used to predict and understand CM.

physics.chem-ph↗

arXiv2022

Characterizing Anomalous High-Harmonic Generation in Solids

Anomalous high-harmonic generation (HHG) arises in certain solids when irradiated by an intense laser field, as the result of a nonlinear perpendicular current akin to a Hall current. Here, we theoretically characterize the anomalous HHG mechanism, via development of an ab-initio methodology for strong-field laser-solid interaction that allows a rigorous decomposition of the total current. We identify two key characteristics of the anomalous harmonic yields: an overall increase with laser wavelength; and pronounced minima at certain intensities or wavelengths around which the emission time profiles drastically change. Such signatures can be exploited to disentangle the anomalous harmonics from the competing interband harmonics, and thus pave way for the experimental identification and time-domain control of pure anomalous harmonics.

physics.optics↗

arXiv2022

Characterizing Particle-Like Charge Migration Dynamics with High-Harmonic Sideband Spectroscopy

We introduce high-harmonic sideband spectroscopy (HHSS) and show that it can be a robust probe of attosecond charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and harmonic-generation (HHG) dynamics using ab initio time-dependent density-functional theory. We find that CM dynamics initiated along the molecular backbone induces sidebands in the HHG spectrum driven by a delayed laser pulse that is polarized perpendicular to the molecular axis. Monitoring the spectrum as either the HHG laser frequency or the relative delay is scanned allows for the extraction of detailed information about the time-domain characteristics of the CM process.

physics.atom-ph↗

arXiv2022

Signatures of multi-band effects in high-harmonic generation in monolayer MoS$_2$

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of high-order harmonics generated in monolayer MoS$_2$, as a function of crystal orientation relative to the mid-infrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. This observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multi-band recombination dipoles.

cond-mat.mtrl-sci↗

arXiv2021

Introduction to theory of high-harmonic generation in solids: tutorial

High-harmonic generation (HHG) in solids has emerged in recent years as a rapidly expanding and interdisciplinary field, attracting attention from both the condensed-matter and the atomic, molecular, and optics communities. It has exciting prospects for the engineering of new light sources and the probing of ultrafast carrier dynamics in solids, and the theoretical understanding of this process is of fundamental importance. This tutorial provides a hands-on introduction to the theoretical description of the strong-field laser-matter interactions in a condensed-phase system that give rise to HHG. We provide an overview ranging from a detailed description of different approaches to calculating the microscopic dynamics and how these are intricately connected to the description of the crystal structure, through the conceptual understanding of HHG in solids as supported by the semiclassical recollision model, and finally a brief description of how to calculate the macroscopic response. We also give a general introduction to the Berry phase, and we discuss important subtleties in the modelling of HHG, such as the choice of structure and laser gauges, and the construction of a smooth and periodic structure gauge for both nondegenerate and degenerate bands. The advantages and drawback of different structure and laser-gauge choices are discussed, both in terms of their ability to address specific questions and in terms of their numerical feasibility.

physics.atom-ph↗

arXiv2021

Expanded view of electron-hole recollisions in solid-state high-order harmonic generation: Full-Brillouin-zone tunneling and imperfect recollisions

We theoretically investigate electron-hole recollisions in high-harmonic generation (HHG) in band-gap solids irradiated by linearly and elliptically polarized drivers. We find that in many cases the emitted harmonics do not originate in electron-hole pairs created at the minimum band gap, where the tunneling probability is maximized, but rather in pairs created across an extended region of the Brillouin zone (BZ). In these situations, the analogy to gas-phase HHG in terms of the short- and long-trajectory categorizations is inadequate. Our analysis methodology comprises three complementary levels of theory: the numerical solutions to the semiconductor Bloch equations, an extended semiclassical recollision model, and a quantum wave packet approach. We apply this methodology to two general material types with representative band structures: a bulk system and a hexagonal monolayer system. In the bulk, the interband harmonics generated using elliptically-polarized drivers are found to originate not from tunneling at the minimum band gap $Γ$, but from regions away from it. In the monolayer system driven by linearly-polarized pulses, tunneling regions near different symmetry points in the BZ lead to distinct harmonic energies and emission profiles. We show that the imperfect recollisions, where an electron-hole pair recollide while being spatially separated, are important in both bulk and monolayer materials. The excellent agreement between our three levels of theory highlights and characterizes the complexity behind the HHG emission dynamics in solids, and expands on the notion of interband HHG as always originating in trajectories tunnelled at the minimum band gap. Our work furthers the fundamental understanding of HHG in periodic systems and will benefit the future design of experiments.

physics.atom-ph↗

arXiv2020

Resonant propagation of x-rays from the linear to the nonlinear regime

We present a theoretical study of temporal, spectral, and spatial reshaping of intense, ultrafast x-ray pulses propagating through a resonant medium. Our calculations are based on the solution of a 3D time-dependent Schrödinger-Maxwell equation, with the incident x-ray photon energy on resonance with the core-level 1s-3p transition in neon. We study the evolution of the combined incident and medium-generated field, including the effects of stimulated emission, absorption, ionization and Auger decay, as a function of the input pulse energy and duration. We find that stimulated Raman scattering between core-excited states $1s^{-1}3p$ and $2p^{-1}3p$ occurs at high x-ray intensity, and that the emission around this frequency is strongly enhanced when also including the similar $1s^{-1}-2p^{-1}$ response of the ion. We also explore the dependence of x-ray self-induced transparency (SIT) and self-focusing on the pulse intensity and duration, and we find that the stimulated Raman scattering plays an important role in both effects. Finally, we discuss how these nonlinear effects may potentially be exploited as control parameters for pulse properties of x-ray free-electron laser sources.

physics.atom-ph↗

arXiv2020

Noncollinear enhancement cavity for record-high out-coupling efficiency of an extreme-UV frequency comb

We demonstrate a femtosecond enhancement cavity with a crossed-beam geometry for efficient generation and extraction of extreme-ultraviolet (XUV) frequency combs at a 154 MHz repetition rate. We achieve a record-high out-coupled power of 600 μW, directly usable for spectroscopy, at a wavelength of 97 nm. This corresponds to a >60% out-coupling efficiency. The XUV power scaling and generation efficiency are similar to that achieved with a single Gaussian-mode fundamental beam inside a collinear enhancement cavity. The noncollinear geometry also opens the door for the generation of isolated attosecond pulses at >100 MHz repetition rate.

physics.optics↗

arXiv2020

Structure- and laser-gauges for the semiconductor Bloch equations in high-harmonic generation in solids

The semiconductor Bloch equations (SBEs) are routinely used for simulations of strong-field laser-matter interactions in condensed matter. In systems without inversion or time-reversal symmetries, the Berry connections and transition dipole phases (TDPs) must be included in the SBEs, which in turn requires the construction of a smooth and periodic structure gauge for the Bloch states. Here, we illustrate a general approach for such a structure-gauge construction for topologically trivial systems. Furthermore, we investigate the SBEs in the length and velocity gauges, and discuss their respective advantages and shortcomings for the high-harmonic generation (HHG) process. We find that in cases where we require dephasing or separation of the currents into interband and intraband contributions, the length gauge SBEs are computationally more efficient. In calculations without dephasing and where only the total current is needed, the velocity gauge SBEs are structure-gauge independent and are computationally more efficient. We employ two systems as numerical examples to highlight our findings: an 1D model of ZnO and the 2D monolayer hexagonal boron nitride (h-BN). The omittance of Berry connections or TDPs in the SBEs for h-BN results in nonphysical HHG spectra. The structure- and laser-gauge considerations in the current work are not restricted to the HHG process, and are applicable to all strong-field matter simulations with SBEs.

physics.atom-ph↗

arXiv2020

Attosecond synchronization of extreme ultraviolet high harmonics from crystals

The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength range. These observations have opened up the possibility of attosecond metrology in solids, which would benefit from a precise measurement of the emission times of individual harmonics with respect to the NIR laser field. Here we show that, when high-harmonics are detected from the input surface of a magnesium oxide crystal, a bichromatic probing of the XUV emission shows a clear synchronization largely consistent with a semiclassical model of electron-hole recollisions in bulk solids. On the other hand, the bichromatic spectrogram of harmonics originating from the exit surface of the 200 $μ$m-thick crystal is strongly modified, indicating the influence of laser field distortions during propagation. Our tracking of sub-cycle electron and hole re-collisions at XUV energies is relevant to the development of solid-state sources of attosecond pulses.

physics.optics↗

arXiv2019

Attosecond time-domain measurement of core-excitonic decay in magnesium oxide

Excitation of ionic solids with extreme ultraviolet pulses creates localized core-excitons, which in some cases couple strongly to the lattice. Here, core-excitonic states of magnesium oxide are studied in the time domain at the Mg $\text{L}_{2,3}$ edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near infrared optical pulses. Combined with a few-state theoretical model, this reveals that the optical pulse shifts the energy of bright core-exciton states as well as induces features arising from dark core-excitons. We report coherence lifetimes for the first two core-excitons of $2.3 \pm 0.2$ and $1.6 \pm 0.5$ femtoseconds and show that these short lifetimes are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process.

cond-mat.mtrl-sci↗