Localization and loss of coherence in molecular double-slit experiments

Zimmermann, B.; Rolles, Daniel; Langer, Burkhard; Hentges, Rainer; Braune, Markus; Cvejanović, S; Geßner, Oliver; Heiser, Franz; Korica, Sanja; Lischke, T.; Reinköster, Axel; Viefhaus, Jens; Dørner, R.; McKoy, Vincent; Becker, Uwe

doi:10.1038/nphys993

Cited by 117 publications

(91 citation statements)

References 43 publications

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“…Regarding photoionization this was even more recently [12]. The showcase example exhib-iting oscillations over several periods is the core electron photoionization of N2 [13]. The oscillation frequency is proportional to the bond length R in the same respect as the oscillation frequency is proportional to the diameter D of C60.…”

Section: Introduktionmentioning

confidence: 99%

Partial photoionization cross sections of C60 and C70: A gas versus adsorbed phase comparison

et al. 2010

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We have performed high resolution measurements of the photoelectrons emitted from the valence shell of C70, in the gas and adsorbed phase on a metal surface, in order to derive branching ratios and the partial photoionization cross sections of the two highest occupied molecular orbitals, HOMO and HOMO-1. The comparison between the two phases and the adsorbed phase shows an interesting and unexpected difference that can be attributed to a small orbital shift in solid C70. Density Functional Theory calculations within the Local Density Approximation (LDA) show good agreement for both data sets and give a plausible explanation for the observed difference. IntroduktionThe discovery of the family of carbon molecules dubbed the 'fullerenes' [1] and the breakthrough in their synthesis [2] have stimulated an extensive research activity in this field. The best known among the fullerenes is the C60 molecule, which consists of 60 carbon atoms arranged on a nearly spherical shell with the highest possible symmetry, point group Ih. Recently, we have studied some of its particularly interesting properties by photoelectron spectroscopy [3]. Our results revealed strong oscillations in the partial photoionization cross sections of the two highest occupied molecular orbitals, HOMO and HOMO-1, reflecting the molecular geometry and symmetry of the electronic charge distribution.These oscillations, which were for the first time discovered in solid C60 and interpreted as a solid state effect [4,5], were later also observed for free C60 molecules [6]. Their interpretation was basically interpreted within a standing wave model of the photoelectron wave in a box like potential [7] being extended to a jellium like potential in a subsequent experimental and theoretical study [8]. It is the spherical like structure of the C60 molecule which gives rise to shell like distribution of the delocalized carbon valence electrons. However, one may look to the problem also from the view point of symmetry. The valence hole states HOMO and HOMO-1 have different symmetry gerade (g) and ungerade (u), a situation which may be compared to homonuclear diatomic molecules. Here the g and u states show also pronounced oscillations in their partial photoionization cross sections and even more pronounced oscillations in their photoelectron diffraction intensity behavior in the molecular frame. These oscillations which were predicted more than forty years ago by Cohen and Fano [9] have been experimentally corroborated since the last ten years only [10,11]. Regarding photoionization this was even more recently [12]. The showcase example exhib-

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Section: Introduktionmentioning

confidence: 99%

Partial photoionization cross sections of C60 and C70: A gas versus adsorbed phase comparison

et al. 2010

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“…Different recent studies have realized the probably smallest double slits and analogs to this Einstein-Bohr debate using diatomic molecules as the diffraction elements in a photoionization process [24][25][26]. They were destroyed in the diffraction process and therefore were capable of car- rying away path information.…”

Section: Resultsmentioning

confidence: 99%

An atomically thin matter-wave beamsplitter

et al. 2015

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Matter-wave interferometry has become an essential tool in studies on the foundations of quantum physics [1] and for precision measurements [2][3][4][5][6]. Mechanical gratings have played an important role as coherent beamsplitters for atoms [7], molecules and clusters [8,9] since the basic diffraction mechanism is the same for all particles. However, polarizable objects may experience van der Waals shifts when they pass the grating walls [10,11] and the undesired dephasing may prevent interferometry with massive objects [12]. Here we explore how to minimize this perturbation by reducing the thickness of the diffraction mask to its ultimate physical limit, i.e. the thickness of a single atom. We have fabricated diffraction masks in single-layer and bilayer graphene as well as in 1 nm thin carbonaceous biphenyl membrane. We identify conditions to transform an array of single layer graphene nanoribbons into a grating of carbon nanoscrolls. We show that all these ultra-thin nanomasks can be used for high-contrast quantum diffraction of massive molecules. They can be seen as a nanomechanical answer to the question debated by Bohr and Einstein [13] whether a softly suspended double slit would destroy quantum interference. In agreement with Bohr's reasoning we show that quantum coherence prevails even in the limit of atomically thin gratings.

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“…N 2 represents one of the simplest few-electron diatomic systems, and its interaction with light has been extensively studied experimentally as well as theoretically. A wealth of results has been reported for single-photon interactions (see, e.g., [86,[112][113][114][115][116][117][118][119], fragmentation by intense laser fields [83,84], two-colour time-resolved studies [73], and highresolution electron impact coincidence measurements [120]. Recently, several experiments on multiple ionization of N 2 by few EUV photons have been performed at FLASH and SCSS.…”

Section: Multiple Fragmentation Of N 2 Moleculementioning

confidence: 99%

Exploring few-photon, few-electron reactions at FLASH: from ion yield and momentum measurements to time-resolved and kinematically complete experiments

Rudenko

Jiang

Курка

et al. 2010

J. Phys. B: At. Mol. Opt. Phys.

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Abstract:In this contribution we briefly review a series of recent pioneering experiments on fewphoton-induced multiple fragmentation of atoms and molecules performed at the Free electron LASer at Hamburg (FLASH) using a "Reaction Microscope", i.e., a coincident momentum imaging technique. For atoms we consider the most basic non-linear process, namely direct or sequential two-photon double ionization (TPDI). In particular benchmark data for theory are presented such as recoil-ion momentum distributions for direct TPDI of He and Ne, and fully differential data for sequential TPDI of Ne. For molecules we show how one can identify contributions from different reaction channels by inspecting the measured kinetic energy and angular distributions of ionic fragments, and even infer the time-delay between the two photon absorption events in TPDI by detailed comparison with theory.Finally, we describe a novel split mirror arrangement for EUV-pump -EUV-probe experiments, and present the very first time-resolved data on the dynamics of N 2 molecules irradiated by the FLASH light.

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Localization and loss of coherence in molecular double-slit experiments

Abstract: For emission out of the molecule along the molecular axis, the direct wave interferes with an electron wave that is scattered an odd number of times and dominated by singlescattering (66% back-scattering), whereas for emission into the molecule, the direct

Cited by 117 publications

References 43 publications

Partial photoionization cross sections of C60 and C70: A gas versus adsorbed phase comparison

Partial photoionization cross sections of C60 and C70: A gas versus adsorbed phase comparison

An atomically thin matter-wave beamsplitter

Exploring few-photon, few-electron reactions at FLASH: from ion yield and momentum measurements to time-resolved and kinematically complete experiments

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