arXiv subjects

J. B. Williams

Publications and source records attributed to J. B. Williams.

17 recordsLinked to original sources

arXiv2025

Probing Instantaneous Single-Molecule Chirality in the Planar Ground State of Formic Acid

We experimentally demonstrate that individual molecules of formic acid are chiral even when they are in the vibronic ground state, which has a planar equilibrium structure. We ionize the C 1s shell of the molecule and record the photoelectron in coincidence with positively charged fragments. This provides two consecutive measurements of the structure of one molecule, the first by photoelectron diffraction imaging and the second by Coulomb explosion imaging. We find that both measurements show the same handedness of the specific molecule. The phenomenon of being achiral on average but chiral at the level of individual molecules is general to most prochiral molecules and is a consequence of the three-dimensional zero-point delocalization of the nuclei in the vibrational ground state.

physics.atom-ph↗

arXiv2023

A new route for enantio-sensitive structure determination by photoelectron scattering on molecules in the gas phase

X-ray as well as electron diffraction are powerful tools for structure determination of molecules. Studies on randomly oriented molecules in the gas-phase address cases in which molecular crystals cannot be generated or the interaction-free molecular structure is to be addressed. Such studies usually yield partial geometrical information, such as interatomic distances. Here, we present a complementary approach, which allows obtaining insight to the structure, handedness and even detailed geometrical features of molecules in the gas phase. Our approach combines Coulomb explosion imaging, the information that is encoded in the molecular frame diffraction pattern of core-shell photoelectrons and ab initio computations. Using a loop-like analysis scheme we are able to deduce specific molecular coordinates with sensitivity even to the handedness of chiral molecules and the positions of individual atoms, as, e.g., protons.

physics.chem-ph↗

arXiv2021

Fourfold Differential Photoelectron Circular Dichroism

We report on a joint experimental and theoretical study of photoelectron circular dichroism (PECD) in methyloxirane. By detecting O 1s-photoelectrons in coincidence with fragment ions, we deduce the molecule's orientation and photoelectron emission direction in the laboratory frame. Thereby, we retrieve a fourfold differential PECD clearly beyond 50%. This strong chiral asymmetry is reproduced by ab initio electronic structure calculations. Providing such a pronounced contrast makes PECD of fixed-in-space chiral molecules an even more sensitive tool for chiral recognition in the gas phase.

physics.atm-clus↗

arXiv2020

Revealing the Two-Electron Cusp in the Ground States of He and H2 via Quasifree Double Photoionization

We report on kinematically complete measurements and ab initio non-perturbative calculations of double ionization of He and H2 by a single 800 eV circularly polarized photon. We confirm the quasifree mechanism of photoionization for H2 and show how it originates from the two-electron cusp in the ground state of a two-electron target. Our approach establishes a new method for mapping electrons relative to each other and provides valuable insight into photoionization beyond the electric-dipole approximation.

physics.atom-ph↗

arXiv2019

Tunable Antenna-Coupled Intersubband Terahertz (TACIT) Mixers: The Quantum Limit Without the Quantum Liquid

At present, nearly quantum-limited heterodyne receivers for Terahertz (THz) frequencies require cooling to temperatures below 4K. We are working to build semiconductor-based "tunable antenna-coupled intersubband terahertz" (TACIT) heterodyne mixers for 1-5 THz. We predict that they can achieve single-sideband noise temperatures of a few hundred K with intermediate frequency (IF) bandwidth >10 GHz, while operating at lattice temperatures >20 K and requiring local oscillator (LO) power ~ 1 $μ$W.

physics.ins-det↗

arXiv2018

Separating Dipole and Quadrupole Contributions to Single-Photon Double Ionization

We report on a kinematically complete measurement of double ionization of helium by a single 1100 eV circularly polarized photon. By exploiting dipole selection rules in the two-electron continuum state, we observed the angular emission pattern of electrons originating from a pure quadrupole transition. Our fully differential experimental data and companion ab initio nonperturbative theory show the separation of dipole and quadrupole contributions to photo-double-ionization and provide new insight into the nature of the quasifree mechanism.

physics.atom-ph↗

arXiv2018

Frustrated Coulomb explosion of small helium clusters

Almost ten years ago, energetic neutral hydrogen atoms were detected after a strong-field double ionization of H$_2$. This process, called 'frustrated tunneling ionization', occurs when an ionized electron is recaptured after being driven back to its parent ion by the electric field of a femtosecond laser. In the present study we demonstrate that a related process naturally occurs in clusters without the need of an external field: we observe a charge hopping that occurs during a Coulomb explosion of a small helium cluster, which leads to an energetic neutral helium atom. This claim is supported by theoretical evidence. As an analog to 'frustrated tunneling ionization', we term this process 'frustrated Coulomb explosion'.

physics.atm-clus↗

arXiv2018

Imaging the square of the correlated two-electron wave function of a hydrogen molecule

The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the constituents is decisive and the spatial and the momentum distribution of one electron depends on those of the other electrons and the nuclei. Such correlations have escaped direct observation by imaging techniques so far. Here, we implement an imaging scheme which visualizes correlations between electrons by coincident detection of the reaction fragments after high energy photofragmentation. With this technique, we examine the H2 two-electron wave function in which electron-electron correlation beyond the mean-field level is prominent. We visualize the dependence of the wave function on the internuclear distance. High energy photoelectrons are shown to be a powerful tool for molecular imaging. Our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.

physics.atom-ph↗

arXiv2016

Two-particle interference of electron pairs on a molecular level

We investigate the photo-doubleionization of $H_2$ molecules with 400 eV photons. We find that the emitted electrons do not show any sign of two-center interference fringes in their angular emission distributions if considered separately. In contrast, the quasi-particle consisting of both electrons (i.e. the "dielectron") does. The work highlights the fact that non-local effects are embedded everywhere in nature where many-particle processes are involved.

physics.atom-ph↗

arXiv2016

Imaging the He$_2$ quantum halo state using a free electron laser

We report on coulomb explosion imaging of the wavefunction of the quantum halo system He$_2$. Each atom of this system is ionized by tunnelionization in a femto second laser pulse and in a second experiment by single photon ionization employing a free electron laser. We visualize the exponential decay of the probability density of the tunneling particle over distance for over two orders of magnitude up to an internuclear distance of 250 Å. By fitting the slope of the density in the tunneling regime we obtain a binding energy of 151.9 $\pm$ 13.3 neV, which is in agreement with most recent calculations.

physics.atom-ph↗

arXiv2016

Electron localization in dissociating $H_2^+$ by retroaction of a photoelectron onto its source

We investigate the dissociation of $H_2^+$ into a proton and a $H^0$ after single ionization with photons of an energy close to the threshold. We find that the $p^+$ and the $H^0$ do not emerge symmetrically in case of the $H_2^+$ dissociating along the $1sσ_g$ ground state. Instead, a preference for the ejection of the $p^+$ in the direction of the escaping photoelectron can be observed. This symmetry breaking is strongest for very small electron energies. Our experiment is consistent with a recent prediction by Serov and Kheifets [Phys. Rev. A 89, 031402 (2014)]. In their model, which treats the photoelectron classically, the symmetry breaking is induced by the retroaction of the long range Coulomb potential onto the dissociating $H_2^+$.

physics.atom-ph↗

arXiv2015

Agreement at last: an experimental and theoretical study on the single ionization of helium by fast proton impact

Even though ion/atom-collision is a mature field of atomic physics great discrepancies between experiment and theoretical calculations are still common. Here we present experimental results with highest momentum resolution on single ionization of helium induced by 1\,MeV protons and compare these to different theoretical calculations. The overall agreement is strikingly good and already the first Born approximation yields good agreement between theory and experiment. This has been expected since several decades, but so far has not been accomplished. The influence of projectile coherence effects on the measured data is shortly discussed in line with an ongoing dispute on the existence of nodal structures in the electron angular emission distributions.

physics.atom-ph↗

arXiv2014

Interatomic-Coulombic-decay-induced recapture of photoelectrons in helium dimers

We investigate the onset of photoionization shakeup induced interatomic Coulombic decay (ICD) in He2 at the He+*(n = 2) threshold by detecting two He+ ions in coincidence. We find this threshold to be shifted towards higher energies compared to the same threshold in the monomer. The shifted onset of ion pairs created by ICD is attributed to a recapture of the threshold photoelectron after the emission of the faster ICD electron.

physics.atm-clus↗

arXiv2014

Absolute cross sections for photoionization of Xe$^{q+}$ ions (1 $\le$ q $\le$ 5) at the 3d ionization threshold

The photon-ion merged-beams technique has been employed at the new Photon-Ion spectrometer at PETRA III (PIPE) for measuring multiple photoionization of Xe$^{q+}$ (q=1-5) ions. Total ionization cross sections have been obtained on an absolute scale for the dominant ionization reactions of the type hν+ Xe$^{q+}$ $\to$ Xe$^{r+}$ + (q-r) e$^-$ with product charge states q+2 $\le$ r $\le$ q+5. Prominent ionization features are observed in the photon-energy range 650-750 eV, which are associated with excitation or ionization of an inner-shell 3d electron. Single-configuration Dirac-Fock calculations agree quantitatively with the experimental cross sections for non-resonant photoabsorption, but fail to reproduce all details of the measured ionization resonance structures.

physics.atom-ph↗

arXiv2013

Vibrationally Resolved Decay Width of Interatomic Coulombic Decay in HeNe

We investigate the ionization of HeNe from below the He 1s3p excitation to the He ionization threshold. We observe HeNe$^+$ ions with an enhancement by more than a factor of 60 when the He side couples resonantly to the radiation field. These ions are an experimental proof of a two-center resonant photoionization mechanism predicted by Najjari et al. [Phys. Rev. Lett. 105, 153002 (2010)]. Furthermore, our data provide electronic and vibrational state resolved decay widths of interatomic Coulombic decay (ICD) in HeNe dimers. We find that the ICD lifetime strongly increases with increasing vibrational state.

physics.atm-clus↗

arXiv2013

A measurement of the evolution of Interatomic Coulombic Decay in the time domain

During the last 15 years a novel decay mechanism of excited atoms has been discovered and investigated. This so called ''Interatomic Coulombic Decay'' (ICD) involves the chemical environment of the electronically excited atom: the excitation energy is transferred (in many cases over long distances) to a neighbor of the initially excited particle usually ionizing that neighbor. It turned out that ICD is a very common decay route in nature as it occurs across van-der-Waals and hydrogen bonds. The time evolution of ICD is predicted to be highly complex, as its efficiency strongly depends on the distance of the atoms involved and this distance typically changes during the decay. Here we present the first direct measurement of the temporal evolution of ICD using a novel experimental approach.

physics.atom-ph↗

arXiv2010

Auger decay of 1σg and 1σu hole states of N2 molecule: disentangling decay routes from coincidence measurements

Results of the most sophisticated measurements in coincidence of the angular resolved K-shell photo- and Auger-electrons, and of two atomic ions produced by dissociation of N2 molecule, are analyzed. Detection of photoelectrons at certain angles allows separating the Auger decay processes of the 1σg and 1σu core hole states. The Auger electron angular distributions for each of these hole states are measured as a function of the kinetic energy release of two atomic ions and are compared with the corresponding theoretical angular distributions. From that comparison one can disentangle the contributions of different repulsive doubly charged molecular ion states to the Auger decay. Different kinetic energy release values are directly related to the different internuclear distances. In this way one can trace experimentally the behavior of the potential energy curves of dicationic final states inside the Frank-Condon region. Presentation of the Auger electron angular distributions as a function of kinetic energy release of two atomic ions opens a new dimension in the study of Auger decay.

physics.atom-ph↗