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New Journal of Physics

Isotope-selective high-order interferometry with large organic molecules in free fall

Jonas Rodewald, Nadine Dörre, Andrea Grimaldi, Philipp Geyer, Lukas Felix, Marcel Mayor, Armin Shayeghi, Markus Arndt

Published Feb 8, 2018• 13 citations
Publisher

Abstract

Interferometry in the time domain has proven valuable for matter-wave based measurements.This concept has recently been generalized to cold molecular clusters using short-pulse standing light waves which realized photo-depletion gratings, arranged in a time-domain Talbot-Lau interferometer (OTIMA).Here we extend this idea further to large organic molecules and demonstrate a new scheme to scan the emerging molecular interferogram in position space.The capability of analyzing different isotopes of the same monomer under identical conditions opens perspectives for studying the interference fringe shift as a function of time in gravitational free fall.The universality of OTIMA interferometry allows one to handle a large variety of particles.In our present work, quasi-continuous laser evaporation allows transferring fragile organic molecules into the gas phase, covering more than an order of magnitude in mass between 614 amu and 6509 amu, i.e. 300% more massive than in previous OTIMA experiments.For all masses, we find about 30% fringe visibility.

DOI
10.1088/1367-2630/aaade2

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•Jan 1, 2012•0 citations
Interferometry in the time domain has proven valuable for matter-wave based measurements.This concept has recently been generalized to cold molecular clusters using short-pulse standing light waves which realized photo-depletion gratings, arranged in a time-domain Talbot-Lau interferometer (OTIMA).Here we extend this idea further to large organic molecules and demonstrate a new scheme to scan the emerging molecular interferogram in position space.The capability of analyzing different isotopes of the same monomer under identical conditions opens perspectives for studying the interference fringe shift as a function of time in gravitational free fall.The universality of OTIMA interferometry allows one to handle a large variety of particles.In our present work, quasi-continuous laser evaporation allows transferring fragile organic molecules into the gas phase, covering more than an order of magnitude in mass between 614 amu and 6509 amu, i.e. 300% more massive than in previous OTIMA experiments.For all masses, we find about 30% fringe visibility.
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.
We discuss modern developments in quantum optics with organic molecules, clusters and nanoparticles -- in particular recent realizations of near-field matter-wave interferometry. A unified theoretical description in phase space allows us to describe quantum interferometry in position space and in the time domain on an equal footing. In order to establish matter-wave interferometers as a universal tool, which can accept and address a variety of nanoparticles, we elaborate on new quantum optical elements, such as diffraction gratings made of matter and light, as well as their absorptive and dispersive interaction with complex materials. We present Talbot-Lau interferometry (TLI), the Kapitza-Dirac-Talbot-Lau interferometer (KDTLI) and interferometry with pulsed optical gratings (OTIMA) as the most advanced devices to study the quantum wave nature of composite matter. These experiments define the current mass and complexity record in interferometric explorations of quantum macroscopicity and they open new avenues to quantum assisted metrology with applications in physical chemistry and biomolecular physics.
We demonstrate a near-field Talbot-Lau interferometer for C70 fullerene molecules. Such interferometers are particularly suitable for larger masses. Using three free-standing gold gratings of 1 microm period and a transversally incoherent but velocity-selected molecular beam, we achieve an interference fringe visibility of 40% with high count rate. Both the high visibility and its velocity dependence are in good agreement with a quantum simulation that takes into account the van der Waals interaction of the molecules with the gratings and are in striking contrast to a classical moiré model.
We discuss new de Broglie coherence experiments in a near-field molecule interferometer with a variety of large organic molecules. While de Broglie coherence is to first order only associated with the center-of-mass motion of the diffracted particle, we here investigate the question as to which extent the internal molecular property is relevant for, compatible with or detrimental for maintaining coherence in the translational degree of freedom. External perturbations, such as inhomogeneous external electric fields, may influence the delocalized molecules inside the matter wave interferometer and they allow us to access the molecular polarizabilities, permanent or even fluctuating electric dipole moments. We extract information about the molecular states from the interference phase shifts as well as from the observed dephasing in a Kapitza-Dirac Talbot-Lau-Stark-deflectometer. We discuss the relevance of our experiments with regard to both molecule metrology and the foundations of quantum mechanics, i.e. the preservation of coherence for highly complex particles in external fields.
This thesis describes theoretical work carried out in connection with the high-mass matter-wave interference experiments at the University of Vienna. Its scope ranges from the simulation and analysis of experimental data to the proposal of a trapped interference scheme applicable to a variety of matter-wave platforms. The first main result of the thesis is the phase-space description of a near-field interferometer with any number of gratings. This theory is used to analyze a four-grating Talbot-Lau interferometer, in which passive compensation of low-frequency vibrations and of the Coriolis force are expected. The compensation is numerically confirmed and its effectiveness is compared to existing techniques. The second main result is the demonstration of Bragg diffraction of complex molecules on optical gratings, to which the author contributed the basic experimental design, simulations, and the interpretation of the data. This demonstration is a first step towards applying large momentum transfer coherent manipulation techniques to the interference of heavy molecules and clusters. The third main result is a new interference scheme for matter waves in toroidal confinement. The beam splitting and recombination in this scheme rely on the free evolution in the waveguide and require no interaction with the matter waves. The scheme is within reach of state-of-the-art experiments with Bose-Einstein condensates, where it could be used to measure weak atom-atom interactions or magnetic field gradients.
In order to explore the quantum-to-classical transition, the ambition of this thesis was the design and synthesis of tailor-made molecules for matter-wave interference experiments. Firstly, the focus was set on a deeper understanding of the influence of a molecule’s internal structure, especially its polarizability, on quantum interference. Furthermore, the limits of quantum mechanics were addressed by increasing the size of the interfering objects. The metrological aspect of molecule interferometry - to measure influences of molecule properties on the wave nature - is described in the first part of this thesis. Two fourfold perfluorohexyl functionalized constitutional isomers were synthesized in order to demonstrate that different molecular conformations can be distinguished in quantum interference experiments. A tetrahedral isomer and a rod-like oligo(phenylene ethynylene) derivative were applied in a near-field Kapitza-Dirac-Talbot-Lau interferometer. Although de Broglie quantum interference describes the center of mass motion of a massive body, it was shown to be sensitive to the internal molecular structure of the constitutional isomers. The different total susceptibilities of both isomers lead to different de Broglie interference shifts in the presence of external electric fields. The isomers thus become distinguishable in spite of their identical mass and chemical sum formula. Besides metrological applications, a main goal of this thesis was to synthesize model compounds for molecule interferometry to increase the preexisting mass record for quantum interferometry, which was held by the fluorofullerene C60F48 with a molecular weight of 1 633 g/mol. Near-field interferometry is a promising concept to set new records and thus to approach the quantum-to-classical transition. To meet the requirements of quantum studies with complex organic molecules in a Kapitza-Dirac-Talbot-Lau near-field interferometer – high volatility, high stability, and high molecular mass – we chose the functionalization of tetraarylporphyrins with perfluoroalkyl moieties. A modular synthesis of seven perfluoroalkyl-substituted porphyrin derivatives with up to 16 fluorous alkyl chains was presented. With this series in hand, it was possible to observe interference patterns for three of the seven derivatives. The heaviest molecule of this series for which the wave nature has been observed has a 3.3 fold higher molecular weight than the preexisting mass record for quantum interference. These experiments open a new window for quantum experiments with nanoobjects in a complexity class comparable to that of small proteins. The experimental setup of the near-field Kapitza-Dirac-Talbot-Lau interferometer is not restricted to monodisperse and pure starting compounds. It also allows for experiments with compound mixtures because individual components of compound libraries can be detected in the mass spectrometric detection unit. The preparation of porphyrin libraries gave access to compounds in a new mass region (> 10 000 g/mol). Preliminary investigations in near-field interferometers with these structures revealed suitable molecule beam properties. With these porphyrin libraries in hand, it is expected to exceed for the first time the ceiling of 10 000 g/mol for an interfering object in the future. Large, stable, highly volatile and fluorescent molecules were the goal of synthetic work that was performed for novel far-field interference experiments in a setup based on fluorescence detection. For this purpose three fluorescent fluorous phthalocyanine derivatives were prepared. With the help of a new laser-controlled micro-evaporation source it was possible to produce a beam of molecules with the required intensity and coherence. The observation of the wave nature of a free base phthalocyanine having a molecular weight of 1 299 g/mol set a new mass record for far-field molecule interferometry. The preexisting record for far-field interferometry was held by the fullerene C70 with a mass of 841 g/mol. To conclude, major contributions to the exploration of the frontiers of quantum mechanics were achieved by matter-wave interferometry using the perfluoroalkyl-functionalized molecules described in this thesis. \n