arXiv subjects

P. H. Bucksbaum

Publications and source records attributed to P. H. Bucksbaum.

At least 19 recordsLinked to original sources

arXiv2024

Orientation-Dependent Enhanced Ionization in Acetylene Revealed by Ultrafast Cross-Polarized Pulse Pairs

We investigate the orientation dependence of Enhanced Ionization (EI) during strong-field-driven nuclear motion in acetylene (C$_2$H$_2$). Here, we both initiate and probe molecular dynamics in acetylene with intense 6-fs cross-polarized pulse pairs, separated by a variable delay. Following multiple ionization by the first pulse, acetylene undergoes simultaneous elongation of the carbon-carbon and carbon-hydrogen bonds, enabling further ionization by the second pulse and the formation of a very highly charged state, [C$_2$H$_2]^{6+}$. At small inter-pulse delays ($<$20 fs), this enhancement occurs when the molecule is aligned to the probe pulse. Conversely, at large delays ($>$40 fs), formation of [C$_2$H$_2]^{6+}$ occurs when the molecule is aligned to the pump pulse. By analyzing the polarization and time dependence of sequentially ionized [C$_2$H$_2]^{6+}$, we resolve two distinct pathways that both contribute to a large increase in the multiple ionization yield. This cross-polarized pulse pair scheme uniquely enables selective probing of deeply bound orbitals, providing new insights on orientation-dependent EI in highly charged hydrocarbons.

physics.atom-ph↗

arXiv2022

Filming Enhanced Ionization in an Ultrafast Triatomic Slingshot

Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e. filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and filmed the rapid "slingshot" motion that enhances ionization and distorts CEI results. Our investigation uncovered both the geometry and mechanism of the enhancement which may inform CEI experiments in many other polyatomic molecules.

physics.chem-ph↗

arXiv2021

Single Particle Detection System for Strong-Field QED Experiments

Measuring signatures of strong-field quantum electrodynamics (SF-QED) processes in an intense laser field is an experimental challenge: it requires detectors to be highly sensitive to single electrons and positrons in the presence of the typically very strong x-ray and $γ$-photon background levels. In this paper, we describe a particle detector capable of diagnosing single leptons from SF-QED interactions and discuss the background level simulations for the upcoming Experiment-320 at FACET-II (SLAC National Accelerator Laboratory). The single particle detection system described here combines pixelated scintillation LYSO screens and a Cherenkov calorimeter. We detail the performance of the system using simulations and a calibration of the Cherenkov detector at the ELBE accelerator. Single 3 GeV leptons are expected to produce approximately 537 detectable photons in a single calorimeter channel. This signal is compared to Monte-Carlo simulations of the experiment. A signal-to-noise ratio of 18 in a single Cherenkov calorimeter detector is expected and a spectral resolution of 2% is achieved using the pixelated LYSO screens.

hep-ex↗

arXiv2021

Correlation Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule

The possibility of suddenly ionized molecules undergoing extremely fast electron hole dynamics prior to significant structural change was first recognized more than 20 years ago and termed charge migration. The accurate probing of ultrafast electron hole dynamics requires measurements that have both sufficient temporal resolution and can detect the localization of a specific hole within the molecule. We report an investigation of the dynamics of inner valence hole states in isopropanol where we use an x-ray pump/x-ray probe experiment, with site and state-specific probing of a transient hole state localized near the oxygen atom in the molecule, together with an ab initio theoretical treatment. We record the signature of transient hole dynamics and make the first observation of dynamics driven by frustrated Auger-Meitner transitions. We verify that the hole lifetime is consistent with our theoretical prediction. This state-specific measurement paves the way to widespread application for observations of transient hole dynamics localized in space and time in molecules and thus to charge transfer phenomena that are fundamental in chemical and material physics.

physics.chem-ph↗

arXiv2021

Strong Field Ionization of Water: Nuclear Dynamics Revealed by Varying the Pulse Duration

Polyatomic molecules in strong laser fields can undergo substantial nuclear motion within tens of femtoseconds. Ion imaging methods based on dissociation or Coulomb explosion therefore have difficulty faithfully recording the geometry dependence of the field ionization that initiates the dissociation process. Here we compare the strong-field double ionization and subsequent dissociation of water (both H$_2$O and D$_2$O) in 10-fs and 40-fs 800-nm laser pulses. We find that 10-fs pulses turn off before substantial internuclear motion occurs, whereas rapid internuclear motion can take place during the double ionization process for 40-fs pulses. The short-pulse measurements are consistent with a simple tunnel ionization picture, whose predictions help interpret the motion observed in the long-pulse measurements.

physics.atom-ph↗

arXiv2019

Multiple Fourier Component Analysis of X-ray Second Harmonic Generation in Diamond

The unprecedented brilliance of X-ray free-electron lasers (XFELs) [1, 2] has enabled first studies of nonlinear interactions in the hard X-ray range. In particular, X-ray-optical mixing [3], X-ray second harmonic generation (XSHG) [4] and nonlinear Compton scattering (NLCS) [5] have been recently observed for the first time using XFELs. The former two experiments as well as X-ray parametric downconversion (XPDC)[6, 7] are well explained by nonlinearities in the impulse approximation[8], where electrons in a solid target are assumed to be quasi free for X-ray interactions far from atomic resonances. However, the energy of the photons generated in NLCS at intensities reaching up to 4 x 1020 W/cm2 exhibit an anomalous red-shift that is in violation with the free-electron model. Here we investigate the underlying physics of X-ray nonlinear interactions at intensities on order of 1016 W/cm2. Specifically, we perform a systematic study of XSHG in diamond. While one phase-matching geometry has been measured in Shwartz et al.[4], we extend these studies to multiple Fourier components and with significantly higher statistics, which allows us to determine the second order nonlinear structure factor. We measure the efficiency, angular dependence, and contributions from different source terms of the process. We find good agreement of our measurements with the quasi-free electron model.

physics.optics↗

arXiv2016

Machine learning applied to single-shot x-ray diagnostics in an XFEL

X-ray free-electron lasers (XFELs) are the only sources currently able to produce bright few-fs pulses with tunable photon energies from 100 eV to more than 10 keV. Due to the stochastic SASE operating principles and other technical issues the output pulses are subject to large fluctuations, making it necessary to characterize the x-ray pulses on every shot for data sorting purposes. We present a technique that applies machine learning tools to predict x-ray pulse properties using simple electron beam and x-ray parameters as input. Using this technique at the Linac Coherent Light Source (LCLS), we report mean errors below 0.3 eV for the prediction of the photon energy at 530 eV and below 1.6 fs for the prediction of the delay between two x-ray pulses. We also demonstrate spectral shape prediction with a mean agreement of 97%. This approach could potentially be used at the next generation of high-repetition-rate XFELs to provide accurate knowledge of complex x-ray pulses at the full repetition rate.

physics.data-an↗

arXiv2016

Self-referenced coherent diffraction x-ray movie of Angstrom- and femtosecond-scale atomic motion

Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with time and space resolution of $30~$fs and $0.3$ Å. The high spatial fidelity is due to interference between the moving excitation and the static initial charge distribution. This x-ray interference has not been employed to image internal motion in molecules before. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on Ångstrom and femtosecond scales. Coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods.

physics.atom-ph↗

arXiv2015

Nonlinear X-ray Compton Scattering

X-ray scattering is a weak linear probe of matter. It is primarily sensitive to the position of electrons and their momentum distribution. Elastic X-ray scattering forms the basis of atomic structural determination while inelastic Compton scattering is often used as a spectroscopic probe of both single-particle excitations and collective modes. X-ray free-electron lasers (XFELs) are unique tools for studying matter on its natural time and length scales due to their bright and coherent ultrashort pulses. However, in the focus of an XFEL the assumption of a weak linear probe breaks down, and nonlinear light-matter interactions can become ubiquitous. The field can be sufficiently high that even non-resonant multiphoton interactions at hard X-rays wavelengths become relevant. Here we report the observation of one of the most fundamental nonlinear X-ray-matter interactions, the simultaneous Compton scattering of two identical photons producing a single photon at nearly twice the photon energy. We measure scattered photons with an energy near 18 keV generated from solid beryllium irradiated by 8.8-9.75 keV XFEL pulses. The intensity in the X-ray focus reaches up to 4x20 W/cm2, which corresponds to a peak electric field two orders of magnitude higher than the atomic unit of field-strength and within four orders of magnitude of the quantum electrodynamic critical field. The observed signal scales quadratically in intensity and is emitted into a non-dipolar pattern, consistent with the simultaneous two-photon scattering from free electrons. However, the energy of the generated photons shows an anomalously large redshift only present at high intensities. This indicates that the instantaneous high-intensity scattering effectively interacts with a different electron momentum distribution than linear Compton scattering, with implications for the study of atomic-scale structure and dynamics of matter

physics.optics↗

arXiv2013

Double core hole production in N2: Beating the Auger clock

We investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a timescale shorter than the core-hole lifetime by using intense x-ray pulses from the Linac Coherent Light Source free electron laser. The production and decay of these states is characterized by photoelectron spectroscopy and Auger electron spectroscopy. In molecules, two types of double core holes are expected, the first with two core holes on the same N atom, and the second with one core hole on each N atom. We report the first direct observations of the former type of core hole in a molecule, in good agreement with theory, and provide an experimental upper bound for the relative contribution of the latter type.

physics.acc-ph↗

arXiv2013

Multiphoton Ionization as a clock to Reveal Molecular Dynamics with Intense Short X-ray Free Electron Laser Pulses

We investigate molecular dynamics of multiple ionization in N2 through multiple core-level photoabsorption and subsequent Auger decay processes induced by intense, short X-ray free electron laser pulses. The timing dynamics of the photoabsorption and dissociation processes is mapped onto the kinetic energy of the fragments. Measurements of the latter allow us to map out the average internuclear separation for every molecular photoionization sequence step and obtain the average time interval between the photoabsorption events. Using multiphoton ionization as a tool of multiple-pulse pump-probe scheme, we demonstrate the modification of the ionization dynamics as we vary the x-ray laser pulse duration.

physics.acc-ph↗

arXiv2013

Delayed Ultrafast X-ray Auger Probing (DUXAP) of Nucleobase Ultraviolet Photoprotection

We present a new method for ultrafast spectroscopy of molecular photoexcited dynamics. The technique uses a pair of femtosecond pulses: a photoexcitation pulse initiating excited state dynamics followed by a soft x-ray (SXR) probe pulse that core ionizes certain atoms inside the molecule. We observe the Auger decay of the core hole as a function of delay between the photoexcitation and SXR pulses. The core hole decay is particularly sensitive to the local valence electrons near the core and shows new types of propensity rules, compared to dipole selection rules in SXR absorption or emission spectroscopy. We apply the delayed ultrafast x-ray Auger probing (DUXAP) method to the specific problem of nucleobase photoprotection to demonstrate its potential. The ultraviolet photoexcited ππ* states of nucleobases are prone to chemical reactions with neighboring bases. To avoid this, the single molecules funnel the ππ* population to lower lying electronic states on an ultrafast timescale under violation of the Born-Oppenheimer approximation. The new type of propensity rule, which is confirmed by Auger decay simulations, allows us to have increased sensitivity on the direct relaxation from the ππ* state to the vibrationally hot electronic ground state. For the nucleobase thymine, we measure a decay constant of 300 fs in agreement with previous quantum chemical simulations.

physics.chem-ph↗

arXiv2010

Influence of Phase Matching on the Cooper Minimum in Ar High Harmonic Spectra

We study the influence of phase matching on interference minima in high harmonic spectra. We concentrate on structures in atoms due to interference of different angular momentum channels during recombination. We use the Cooper minimum (CM) in argon at 47 eV as a marker in the harmonic spectrum. We measure 2d harmonic spectra in argon as a function of wavelength and angular divergence. While we identify a clear CM in the spectrum when the target gas jet is placed after the laser focus, we find that the appearance of the CM varies with angular divergence and can even be completely washed out when the gas jet is placed closer to the focus. We also show that the argon CM appears at different wavelengths in harmonic and photo-absorption spectra measured under conditions independent of any wavelength calibration. We model the experiment with a simulation based on coupled solutions of the time-dependent Schrödinger equation and the Maxwell wave equation, including both the single atom response and macroscopic effects of propagation. The single atom calculations confirm that the ground state of argon can be represented by its field free $p$ symmetry, despite the strong laser field used in high harmonic generation. Because of this, the CM structure in the harmonic spectrum can be described as the interference of continuum $s$ and $d$ channels, whose relative phase jumps by $π$ at the CM energy, resulting in a minimum shifted from the photoionization result. We also show that the full calculations reproduce the dependence of the CM on the macroscopic conditions. We calculate simple phase matching factors as a function of harmonic order and explain our experimental and theoretical observation in terms of the effect of phase matching on the shape of the harmonic spectrum. Phase matching must be taken into account to fully understand spectral features related to HHG spectroscopy.

physics.atom-ph↗

arXiv2006

Information hiding and retrieval in Rydberg wave packets using half-cycle pulses

We demonstrate an information hiding and retrieval scheme with the relative phases between states in a Rydberg wave packet acting as the bits of a data register. We use a terahertz half-cycle pulse (HCP) to transfer phase-encoded information from an optically accessible angular momentum manifold to another manifold which is not directly accessed by our laser pulses, effectively hiding the information from our optical interferometric measurement techniques. A subsequent HCP acting on these wave packets reintroduces the information back into the optically accessible data register manifold which can then be `read' out.

quant-ph↗

arXiv2004

Coherence measurements on Rydberg wave packets kicked by a half-cycle pulse

A kick from a unipolar half-cycle pulse (HCP) can redistribute population and shift the relative phase between states in a radial Rydberg wave packet. We have measured the quantum coherence properties following the kick, and show that selected coherences can be destroyed by applying an HCP at specific times. Quantum mechanical simulations show that this is due to redistribution of the angular momentum in the presence of noise. These results have implications for the storage and retrieval of quantum information in the wave packet.

quant-ph↗

arXiv2004

Extracting quantum dynamics from genetic learning algorithms through principal control analysis

Genetic learning algorithms are widely used to control ultrafast optical pulse shapes for photo-induced quantum control of atoms and molecules. An unresolved issue is how to use the solutions found by these algorithms to learn about the system's quantum dynamics. We propose a simple method based on covariance analysis of the control space, which can reveal the degrees of freedom in the effective control Hamiltonian. We have applied this technique to stimulated Raman scattering in liquid methanol. A simple model of two-mode stimulated Raman scattering is consistent with the results.

quant-ph↗

arXiv2004

Probing the evolution of Stark wave packets by a weak half cycle pulse

We probe the dynamic evolution of a Stark wave packet in cesium using weak half-cycle pulses (HCP's). The state-selective field ionization(SSFI) spectra taken as a function of HCP delay reveal wave packet dynamics such as Kepler beats, Stark revivals and fractional revivals. A quantum-mechanical simulation explains the results as multi-mode interference induced by the HCP.

quant-ph↗

arXiv2004

Control of Raman Lasing in the Nonimpulsive Regime

We explore coherent control of stimulated Raman scattering in the nonimpulsive regime. Optical pulse shaping of the coherent pump field leads to control over the stimulated Raman output. A model of the control mechanism is investigated.

quant-ph↗