K. Kreidi

Bio: K. Kreidi is an academic researcher from Goethe University Frankfurt. The author has contributed to research in topics: Interatomic Coulombic decay & Electron. The author has an hindex of 19, co-authored 32 publications receiving 1513 citations.

Ultrafast energy transfer between water molecules

Abstract: Analysis of the electrons ionized from water dimers suggests that the energy absorbed by one molecule is rapidly transmitted to the second molecule from which the electron is ejected. This process, referred to as intermolecular Coulombic decay, is a qualitatively different source of low-energy electrons to conventional direct ionization processes. At the transition from the gas to the liquid phase of water, a wealth of new phenomena emerge, which are absent for isolated H2O molecules. Many of those are important for the existence of life, for astrophysics and atmospheric science. In particular, the response to electronic excitation changes completely as more degrees of freedom become available. Here we report the direct observation of an ultrafast transfer of energy across the hydrogen bridge in (H2O)2 (a so-called water dimer). This intermolecular coulombic decay leads to an ejection of a low-energy electron from the molecular neighbour of the initially excited molecule. We observe that this decay is faster than the proton transfer that is usually a prominent pathway in the case of electronic excitation of small water clusters and leads to dissociation of the water dimer into two H2O+ ions. As electrons of low energy (∼0.7–20 eV) have recently been found to efficiently break-up DNA constituents1,2, the observed decay channel might contribute as a source of electrons that can cause radiation damage in biological matter.

Experimental Observation of Interatomic Coulombic Decay in Neon Dimers

Abstract: Recently Cederbaum et al. [Phys. Rev. Lett. 79, 4778 (1997)] predicted a new decay channel of excited atoms and molecules termed interatomic Coulombic decay (ICD). In ICD the deexcitation energy is transferred via virtual photon exchange to a neighboring atom, which releases it by electron emission. We report on an experimental observation of ICD in $2s$ ionized neon dimers. The process is unambiguously identified by detecting the energy of two ${\mathrm{N}\mathrm{e}}^{1+}$ fragments and the ICD electron in coincidence, yielding a clean, background free experimental spectral distribution of the ICD electrons.

The Simplest Double Slit: Interference and Entanglement in Double Photoionization of H2

Abstract: The wave nature of particles is rarely observed, in part because of their very short de Broglie wavelengths in most situations. However, even with wavelengths close to the size of their surroundings, the particles couple to their environment (for example, by gravity, Coulomb interaction, or thermal radiation). These couplings shift the wave phases, often in an uncontrolled way, and the resulting decoherence, or loss of phase integrity, is thought to be a main cause of the transition from quantum to classical behavior. How much interaction is needed to induce this transition? Here we show that a photoelectron and two protons form a minimum particle/slit system and that a single additional electron constitutes a minimum environment. Interference fringes observed in the angular distribution of a single electron are lost through its Coulomb interaction with a second electron, though the correlated momenta of the entangled electron pair continue to exhibit quantum interference.

Single Photon-Induced Symmetry Breaking of H2 Dissociation

Abstract: H2, the smallest and most abundant molecule in the universe, has a perfectly symmetric ground state. What does it take to break this symmetry? We found that the inversion symmetry can be broken by absorption of a linearly polarized photon, which itself has inversion symmetry. In particular, the emission of a photoelectron with subsequent dissociation of the remaining H +2 fragment shows no symmetry with respect to the ionic H+ and neutral H atomic fragments. This lack of symmetry results from the entanglement between symmetric and antisymmetric H +2 states that is caused by autoionization. The mechanisms behind this symmetry breaking are general for all molecules.

Single photon induced symmetry breaking of H2 dissociation - eScholarship

Abstract: Single photon induced symmetry breaking of H 2 dissociation F. Mart´ 1 , J. Fern´ ndez 1 , T. Havermeier 2 , L. Foucar 2 , Th. Weber 2 , in a K. Kreidi 2 , M. Sch¨ ffler 2 , L. Schmidt 2 , T. Jahnke 2 , O. Jagutzki 2 , A. o Czasch 2 , E.P. Benis 4 , T. Osipov 5 , A. L. Landers 3 , A. Belkacem 5 , M. H. Prior 5 , H. Schmidt-B¨ cking 2 , C. L. Cocke 4 , and R. D¨ rner 2 o o Departamento de Qu´ mica, C-9, Universidad Aut´ noma de Madrid, 28049-Madrid, Spain o Institut f¨ r Kernphysik, University Frankfurt, u Max von Laue Str 1, D-60438 Frankfurt Germany Department of Physics, Auburn University Auburn AL-36849 Dept of Physics, Kansas State Univ, Cardwell Hall, Manhattan KS 66506 Lawrence Berkeley National Lab., Berkeley CA 94720 Abstract H 2 , the smallest and most abundant molecule in the universe, has a perfectly symmetric ground state. What does it take to break this symmetry? Here we show that the inversion symmetry can be broken by absorption of a linearly polarized photon, which itself has inversion symmetry. In particular, the emission of a photoelectron with subsequent dissociation of the remaining H + fragment shows no symmetry with respect to the ionic H + and neutral H atomic fragments. This result is the consequence of the entanglement between symmetric and antisymmetric H + states resulting from autoionization. The mechanisms behind this symmetry breaking are general for all molecules.

Double-slit photoelectron interference in strong-field ionization of the neon dimer.

Abstract: Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.

Attosecond Physics

Abstract: Summary form only given. Fundamental processes in atoms, molecules, as well as condensed matter are triggered or mediated by the motion of electrons inside or between atoms. Electronic dynamics on atomic length scales tends to unfold within tens to thousands of attoseconds (1 attosecond [as] = 10-18 s). Recent breakthroughs in laser science are now opening the door to watching and controlling these hitherto inaccessible microscopic dynamics. The key to accessing the attosecond time domain is the control of the electric field of (visible) light, which varies its strength and direction within less than a femtosecond (1 femtosecond = 1000 attoseconds). Atoms exposed to a few oscillations cycles of intense laser light are able to emit a single extreme ultraviolet (XUV) burst lasting less than one femtosecond. Full control of the evolution of the electromagnetic field in laser pulses comprising a few wave cycles have recently allowed the reproducible generation and measurement of isolated sub-femtosecond XUV pulses, demonstrating the control of microscopic processes (electron motion and photon emission) on an attosecond time scale. These tools have enabled us to visualize the oscillating electric field of visible light with an attosecond "oscilloscope", to control single-electron and probe multi-electron dynamics in atoms, molecules and solids. Recent experiments hold promise for the development of an attosecond X-ray source, which may pave the way towards 4D electron imaging with sub-atomic resolution in space and time.

Laser-Induced Electron Tunneling and Diffraction

Abstract: Molecular structure is usually determined by measuring the diffraction pattern the molecule impresses on x-rays or electrons. We used a laser field to extract electrons from the molecule itself, accelerate them, and in some cases force them to recollide with and diffract from the parent ion, all within a fraction of a laser period. Here, we show that the momentum distribution of the extracted electron carries the fingerprint of the highest occupied molecular orbital, whereas the elastically scattered electrons reveal the position of the nuclear components of the molecule. Thus, in one comprehensive technology, the photoelectrons give detailed information about the electronic orbital and the position of the nuclei.

Electron localization following attosecond molecular photoionization

Abstract: For the past several decades, we have been able to directly probe the motion of atoms that is associated with chemical transformations and which occurs on the femtosecond (10(-15)-s) timescale. However, studying the inner workings of atoms and molecules on the electronic timescale has become possible only with the recent development of isolated attosecond (10(-18)-s) laser pulses. Such pulses have been used to investigate atomic photoexcitation and photoionization and electron dynamics in solids, and in molecules could help explore the prompt charge redistribution and localization that accompany photoexcitation processes. In recent work, the dissociative ionization of H(2) and D(2) was monitored on femtosecond timescales and controlled using few-cycle near-infrared laser pulses. Here we report a molecular attosecond pump-probe experiment based on that work: H(2) and D(2) are dissociatively ionized by a sequence comprising an isolated attosecond ultraviolet pulse and an intense few-cycle infrared pulse, and a localization of the electronic charge distribution within the molecule is measured that depends-with attosecond time resolution-on the delay between the pump and probe pulses. The localization occurs by means of two mechanisms, where the infrared laser influences the photoionization or the dissociation of the molecular ion. In the first case, charge localization arises from quantum mechanical interference involving autoionizing states and the laser-altered wavefunction of the departing electron. In the second case, charge localization arises owing to laser-driven population transfer between different electronic states of the molecular ion. These results establish attosecond pump-probe strategies as a powerful tool for investigating the complex molecular dynamics that result from the coupling between electronic and nuclear motions beyond the usual Born-Oppenheimer approximation.

Photoelectron angular distributions from strong-field ionization of oriented molecules

Abstract: An experimental study shows how a polar molecule can be oriented in three dimensions by using a combination of laser and electrostatic fields. The approach should help to obtain molecular-frame information about strong-field ionization processes in molecules for which the orientation cannot be determined after ionization.