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Markus Arndt

Publications and source records attributed to Markus Arndt.

At least 55 records · Page 3Linked to original sources

Matter-wave interference with particles selected from a molecular library with masses exceeding 10000 amu

The quantum superposition principle, a key distinction between quantum physics and classical mechanics, is often perceived as a philosophical challenge to our concepts of reality, locality or space-time since it contrasts our intuitive expectations with experimental observations on isolated quantum systems. While we are used to associating the notion of localization with massive bodies, quantum physics teaches us that every individual object is associated with a wave function that may eventually delocalize by far more than the body's own extension. Numerous experiments have verified this concept at the microscopic scale but intuition wavers when it comes to delocalization experiments with complex objects. While quantum science is the uncontested ideal of a physics theory, one may ask if the superposition principle can persist on all complexity scales. This motivates matter-wave diffraction and interference studies with large compounds in a three-grating interferometer configuration which also necessitates the preparation of high-mass nanoparticle beams at low velocities. Here we demonstrate how synthetic chemistry allows us to prepare libraries of fluorous porphyrins which can be tailored to exhibit high mass, good thermal stability and relatively low polarizability, which allows us to form slow thermal beams of these high-mass compounds, which can be detected in electron ionization mass spectrometry. We present successful superposition experiments with selected species from these molecular libraries in a quantum interferometer, which utilizes the diffraction of matter waves at an optical phase grating. We observe high-contrast quantum fringe patterns with molecules exceeding a mass of 10 000 amu and 810 atoms in a single particle.

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Cavity cooling of free silicon nanoparticles in high-vacuum

Laser cooling has given a boost to atomic physics throughout the last thirty years since it allows one to prepare atoms in motional states which can only be described by quantum mechanics. Most methods, such as Doppler cooling, polarization gradient cooling or sub-recoil laser cooling rely, however, on a near-resonant and cyclic coupling between laser light and well-defined internal states. Although this feat has recently even been achieved for diatomic molecules, it is very hard for mesoscopic particles. It has been proposed that an external cavity may compensate for the lack of internal cycling transitions in dielectric objects and it may thus provide assistance in the cooling of their centre of mass state. Here, we demonstrate cavity cooling of the transverse kinetic energy of silicon nanoparticles propagating in genuine high-vacuum (< 10^8 mbar). We create and launch them with longitudinal velocities even down to v < 1 m/s using laser induced thermomechanical stress on a pristine silicon wafer. The interaction with the light of a high-finesse infrared cavity reduces their transverse kinetic energy by more than a factor of 30. This is an important step towards new tests of recent proposals to explore the still speculative non-linearities of quantum mechanics with objects in the mass range between 10^7 and 10^10 amu.

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Colloquium: Quantum interference of clusters and molecules

We review recent progress and future prospects of matter wave interferometry with complex organic molecules and inorganic clusters. Three variants of a near-field interference effect, based on diffraction by material nanostructures, at optical phase gratings, and at ionizing laser fields are considered. We discuss the theoretical concepts underlying these experiments and the experimental challenges. This includes optimizing interferometer designs as well as understanding the role of decoherence. The high sensitivity of matter wave interference experiments to external perturbations is demonstrated to be useful for accurately measuring internal properties of delocalized nanoparticles. We conclude by investigating the prospects for probing the quantum superposition principle in the limit of high particle mass and complexity.

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Testing spontaneous localization theories with matter-wave interferometry

We propose to test the theory of continuous spontaneous localization (CSL) in an all-optical time-domain Talbot-Lau interferometer for clusters with masses exceeding 1000000 amu. By assessing the relevant environmental decoherence mechanisms, as well as the growing size of the particles relative to the grating fringes, we argue that it will be feasible to test the quantum superposition principle in a mass range excluded by recent estimates of the CSL effect.

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Concept of an ionizing time-domain matter-wave interferometer

We discuss the concept of an all-optical and ionizing matter-wave interferometer in the time domain. The proposed setup aims at testing the wave nature of highly massive clusters and molecules, and it will enable new precision experiments with a broad class of atoms, using the same laser system. The propagating particles are illuminated by three pulses of a standing ultraviolet laser beam, which detaches an electron via efficient single photon-absorption. Optical gratings may have periods as small as 80 nm, leading to wide diffraction angles for cold atoms and to compact setups even for very massive clusters. Accounting for the coherent and the incoherent parts of the particle-light interaction, we show that the combined effect of phase and amplitude modulation of the matter waves gives rise to a Talbot-Lau-like interference effect with a characteristic dependence on the pulse delay time.

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New prospects for de Broglie interferometry

We consider various effects that are encountered in matter wave interference experiments with massive nanoparticles. The text-book example of far-field interference at a grating is compared with diffraction into the dark field behind an opaque aperture, commonly designated as Poisson's spot or the spot of Arago. Our estimates indicate that both phenomena may still be observed in a mass range exceeding present-day experiments by at least two orders of magnitude. They both require, however, the development of sufficiently cold, intense and coherent cluster beams. While the observation of Poisson's spot offers the advantage of non-dispersiveness and a simple distinction between classical and quantum fringes in the absence of particle wall interactions, van der Waals forces may severely limit the distinguishability between genuine quantum wave diffraction and classically explicable spots already for moderately polarizable objects and diffraction elements as thin as 100 nm.

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Master Equation for the Motion of a Polarizable Particle in a Multimode Cavity

We derive a master equation for the motion of a polarizable particle weakly interacting with one or several strongly pumped cavity modes. We focus here on massive particles with complex internal structure such as large molecules and clusters, for which we assume a linear scalar polarizability mediating the particle-light interaction. The predicted friction and diffusion coefficients are in good agreement with former semiclassical calculations for atoms and small molecules in weakly pumped cavities, while the current rigorous quantum treatment and numerical assessment sheds a light on the feasibility of experiments that aim at optically manipulating beams of massive molecules with multimode cavities.

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Wave and Particle in Molecular Interference Lithography

The wave-particle duality of massive objects is a cornerstone of quantum physics and a key property of many modern tools such as electron microscopy, neutron diffraction or atom interferometry. Here we report on the first experimental demonstration of quantum interference lithography with complex molecules. Molecular matter-wave interference patterns are deposited onto a reconstructed Si(111) 7x7 surface and imaged using scanning tunneling microscopy. Thereby both the particle and the quantum wave character of the molecules can be visualized in one and the same image. This new approach to nanolithography therefore also represents a sensitive new detection scheme for quantum interference experiments.

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Quantum physics meets biology

Quantum physics and biology have long been regarded as unrelated disciplines, describing nature at the inanimate microlevel on the one hand and living species on the other hand. Over the last decades the life sciences have succeeded in providing ever more and refined explanations of macroscopic phenomena that were based on an improved understanding of molecular structures and mechanisms. Simultaneously, quantum physics, originally rooted in a world view of quantum coherences, entanglement and other non-classical effects, has been heading towards systems of increasing complexity. The present perspective article shall serve as a pedestrian guide to the growing interconnections between the two fields. We recapitulate the generic and sometimes unintuitive characteristics of quantum physics and point to a number of applications in the life sciences. We discuss our criteria for a future quantum biology, its current status, recent experimental progress and also the restrictions that nature imposes on bold extrapolations of quantum theory to macroscopic phenomena.

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Theory and experimental verification of Kapitza-Dirac-Talbot-Lau interferometry

Kapitza-Dirac-Talbot-Lau interferometry (KDTLI) has recently been established for demonstrating the quantum wave nature of large molecules. A phase space treatment permits us to derive closed equations for the near-field interference pattern, as well as for the Moire-type pattern that would arise if the molecules were to be treated as classical particles. The model provides a simple and elegant way to account for the molecular phase shifts related to the optical dipole potential as well as for the incoherent effect of photon absorption at the second grating. We present experimental results for different molecular masses, polarizabilities and absorption cross sections using fullerenes and fluorofullerenes and discuss the alignment requirements. Our results with C60 and C70, C60F36 and C60F48 verify the theoretical description to a high degree of precision.

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Quantum interferometry with complex molecules

This chapter reviews recent experiments on matter wave interferometry with large molecules. Starting from an elementary introduction to matter wave physics we discuss far-field diffraction and near-field interferometry with thermally excited many-body systems. We describe the constraints imposed by decoherence and dephasing effects, and present an outlook to the future challenges in macromolecule and cluster interferometry.

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Absolute absorption spectroscopy based on molecule interferometry

We propose a new method to measure the absolute photon absorption cross section of neutral molecules in a molecular beam. It is independent of our knowledge of the particle beam density, nor does it rely on photo-induced fragmentation or ionization. The method is based on resolving the recoil resulting from photon absorption by means of near-field matter-wave interference, and it thus applies even to very dilute beams with low optical densities. Our discussion includes the possibility of internal state conversion as well as fluorescence. We assess the influence of various experimental uncertainties and show that the measurement of absolute absorption cross sections is conceivable with high precision and using existing technologies.

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A Kapitza-Dirac-Talbot-Lau interferometer for highly polarizable molecules

Research on matter waves is a thriving field of quantum physics and has recently stimulated many investigations with electrons, neutrons, atoms, Bose-condensed ensembles, cold clusters and hot molecules. Coherence experiments with complex objects are of interest for exploring the transition to classical physics, for measuring molecular properties and they have even been proposed for testing new models of space-time. For matter-wave experiments with complex molecules, the strongly dispersive effect of the interaction between the diffracted molecule and the grating wall is a major challenge because it imposes enormous constraints on the velocity selection of the molecular beam. We here describe the first experimental realization of a new interferometer that solves this problem by combining the advantages of a Talbot-Lau setup with the benefits of an optical phase grating and we show quantum interference with new large molecules.

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Optical polarizabilities of large molecules measured in near-field interferometry

We discuss a novel application of matter wave interferometry to characterize the scalar optical polarizability of molecules at 532 nm. The interferometer presented here consists of two material absorptive gratings and one central optical phase grating. The interaction of the molecules with the standing light wave is determined by the optical dipole force and is therefore directly dependent on the molecular polarizability at the wavelength of the diffracting laser light. By comparing the observed matter-wave interference contrast with a theoretical model for several intensities of the standing light wave and molecular velocities we can infer the polarizability in this first proof-of-principle experiment for the fullerenes C60 and C70 and we find a good agreement with literature values.

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Gas phase sorting of nanoparticles

We discuss Stark deflectometry of micro-modulated molecular beams for the enrichment of biomolecular isomers as well as single-wall carbon nanotubes and we demonstrate the working principle of this idea with fullerenes. The sorting is based on the species-dependent polarizability-to-mass ratio $α/m$. The device is compatible with a high molecular throughput, and the spatial micro-modulation of the beam permits to obtain a fine spatial resolution and a high sorting sensitivity.

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Slow beams of massive molecules

Slow beams of neutral molecules are of great interest for a wide range of applications, from cold chemistry through precision measurements to tests of the foundations of quantum mechanics. We report on the quantitative observation of thermal beams of perfluorinated macromolecules with masses up to 6000 amu, reaching velocities down to 11 m/s. Such slow, heavy and neutral molecular beams are of importance for a new class of experiments in matter-wave interferometry and we also discuss the requirements for further manipulation and cooling schemes with molecules in this unprecedented mass range.

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Polarizability measurements in a molecule near-field interferometer

We apply near-field matter-wave interferometry to determine the absolute scalar polarizability of the fullerenes C$_{60}$ and C$_{70}$. A key feature of our experiment is the combination of good transmission and high spatial resolution, gained by wide molecular beams passing through sub-micron gratings. This allows to significantly facilitate the observation of field-dependent beam shifts. We thus measure the polarizability to be $α=88.9 \pm 0.9 \pm 5.1 \rm Å^{3}$ for C$_{60}$ and to $α= 108.5 \pm 2.0 \pm 6.2 \rm Å^{3}$ for C$_{70}$.

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A scalable optical detection scheme for matter wave interferometry

Imaging of surface adsorbed molecules is investigated as a novel detection method for matter wave interferometry with fluorescent particles. Mechanically magnified fluorescence imaging turns out to be an excellent tool for recording quantum interference patterns. It has a good sensitivity and yields patterns of high visibility. The spatial resolution of this technique is only determined by the Talbot gratings and can exceed the optical resolution limit by an order of magnitude. A unique advantage of this approach is its scalability: for certain classes of nano-sized objects, the detection sensitivity will even increase significantly with increasing size of the particle.

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