The nature of time as emergent for a system by separating it from its environment has been put forward by Page and Wootters [Phys. Rev. D 27, 2885 (1983)PRVDAQ0556-282110.
View Article and Find Full Text PDFTunable attosecond pulses are necessary for various attosecond resolved spectroscopic applications, which can potentially be obtained through the tuning of high harmonic generation. Here we show theoretically, using the time-dependent Schrödinger equation and strong field approximation, a continuously tunable spectral shift of high-order harmonics by exploiting the interaction of two delayed identical infrared (IR) pulses within the single-atom response. The tuning spans more than twice the driving frequency (∼2ω) range, for several near-cutoff harmonics, with respect to only one control parameter: the change in delay between the two IR pulses.
View Article and Find Full Text PDFFaraday Discuss
September 2022
We elucidate the mechanism of strong laser pulse excitation in pristine graphene with multi-harmonic pulses, linearly polarized parallel to the line connecting the two different Dirac points in the Brillouin zone and with a maximal vector potential given by the distance of those points. The latter two conditions have emerged from our previous work [Kelardeh , , 2022, , L022014] as favorable for large valley polarization. We introduce a novel compacted representation for excitation, locally resolved in the initial conditions for the crystal momenta.
View Article and Find Full Text PDFWe demonstrate a dispersion-free wavefront splitting attosecond resolved interferometric delay line for easy ultrafast metrology of broadband femtosecond pulses. Using a pair of knife-edge prisms, we symmetrically split and later recombine the two wavefronts with a few tens of attosecond resolution and stability and employ a single-pixel analysis of interference fringes with good contrast using a phone camera without any iris or nonlinear detector. Our all-reflective delay line is theoretically analyzed and experimentally validated by measuring 1st and 2nd order autocorrelations and the SHG-FROG trace of a NIR femtosecond pulse.
View Article and Find Full Text PDFWe 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.
View Article and Find Full Text PDFWe predict the existence of a universal class of ultralong-range Rydberg molecular states whose vibrational spectra form trimmed Rydberg series. A dressed ion-pair model captures the physical origin of these exotic molecules, accurately predicts their properties, and reveals features of ultralong-range Rydberg molecules and heavy Rydberg states with a surprisingly small Rydberg constant. The latter is determined by the small effective charge of the dressed anion, which outweighs the contribution of the molecule's large reduced mass.
View Article and Find Full Text PDFIn attosecond science it is assumed that Wigner-Smith time delays, known from scattering theory, are determined by measuring streaking shifts. Despite their wide use from atoms to solids this has never been proven. Analyzing the underlying process-energy absorption from the streaking light-we derive this relation.
View Article and Find Full Text PDFWe introduce an ultra-thin attosecond optical delay line based on controlled wavefront division of a femtosecond infrared pulse after transmission through a pair of micrometer-thin glass plates with negligible dispersion effects. The time delay between the two pulses is controlled by rotating one of the glass plates from absolute zero to several optical cycles, with 2.5 as to tens of attosecond resolution with 2 as stability, as determined by interferometric self-calibration.
View Article and Find Full Text PDFRescattering by electrons on classical trajectories is central to understand photoelectron and high-harmonic emission from isolated atoms or molecules in intense laser pulses. By controlling the cluster size and the quiver amplitude of electrons, we demonstrate how rescattering influences the energy distribution of photoelectrons emitted from noble gas nanoclusters. Our experiments reveal a universal dependence of photoelectron energy distributions on the cluster size when scaled by the field driven electron excursion, establishing a unified rescattering picture for extended systems with the known atomic dynamics as the limit of zero extension.
View Article and Find Full Text PDFPhotoelectron 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.
View Article and Find Full Text PDFWe demonstrate that, by changing the direction of the chirp in vacuum-ultraviolet 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 of rapid adiabatic passage if extended to include transitions to the continuum. The chirp phase locks the linear combination of the two resonantly coupled bound states whose ionization amplitudes interfere constructively or destructively depending on the chirp direction under suitable conditions.
View Article and Find Full Text PDFWe 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.
View Article and Find Full Text PDFWe develop general quantitative criteria for dynamic interference, a manifestation of a double-slit interference in time which should be realizable with brilliant state-of-the-art high-frequency laser sources. Our analysis reveals that the observation of dynamic interference hinges upon maximizing the difference between the dynamic polarization of the initial bound and the final continuum states of the electron during the light pulse while keeping depletion of the initial state small. These two properties, Stark shift and depletion, can be determined from electronic structure calculations avoiding expensive propagation in time.
View Article and Find Full Text PDFThe dynamics of ultraslow electrons in the combined potential of an ionic core and a static electric field is discussed. With state-of-the-art detection it is possible to create such electrons through strong intense-field photoabsorption and to detect them via high-resolution time-of-flight spectroscopy despite their very low kinetic energy. The characteristic feature of their momentum spectrum, which emerges at the same position for different laser orientations, is derived and could be revealed experimentally with an energy resolution of the order of 1 meV.
View Article and Find Full Text PDFWe explore the possibility for orientation recovery in single-molecule coherent diffractive imaging with diffusion map. This algorithm approximates the Laplace-Beltrami operator, which we diagonalize with a metric that corresponds to the mapping of Euler angles onto scattering images. While suitable for images of objects with specific properties we show why this approach fails for realistic molecules.
View Article and Find Full Text PDFObjective: Long-term studies regarding the effect of a structured physical exercise programme (SPEP) during haemodialysis (HD) assessing compliance and clinical benefit are scarce.
Study Design: A single-centre clinical trial, non-randomised, investigating 46 patients with HD (63.2 ± 16.
X-ray photoabsorption from intense short pulses by a molecule triggers complicated electron and subsequently ion dynamics, leading to photoelectron spectra, which are difficult to interpret. Illuminating fullerenes offers a way to separate out the electron dynamics since the cage structure confines spatially the origin of photo- and Auger electrons. Together with the sequential nature of the photoprocesses at intensities available at x-ray free-electron lasers, this allows for a remarkably detailed interpretation of the photoelectron spectra, as we will demonstrate.
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