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Angewandte Chemie International Edition

The Wave Property of Heavy Molecules—Its Use in Mass Spectrometry

Karl‐Otto Greulich

Published Sep 11, 2008• 2 citations
Publisher

Abstract

The perfect wave: The wave properties of large molecules have been used for mass spectrometry. A perfluoroalkylated palladium complex has been investigated by this method and its mass and polarizability determined from the visibility of the molecules interferogram. This method allows the differentiation of molecule fragments in the source from those generated in the detector. Applications based on matter waves are now conceivable.

DOI
10.1002/anie.200803290

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The perfect wave: The wave properties of large molecules have been used for mass spectrometry. A perfluoroalkylated palladium complex has been investigated by this method and its mass and polarizability determined from the visibility of the molecules interferogram. This method allows the differentiation of molecule fragments in the source from those generated in the detector. Applications based on matter waves are now conceivable.
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Matter-wave interferometry with large molecules is partially limited by the inefficiency of the commonly used ionization detection schemes. Here we discuss the possibility of employing a surface imaging method in which molecular interferograms with periods in the micron range are adsorbed on a surface and subsequently read using fluorescence microscopy. Our preliminary experiments show that the detection efficiency can be significantly increased compared to electron impact ionization and quadrupole mass spectrometry. However the interpretation of fluorescent molecular patterns requires a good understanding and control of the molecular mobility, the bleaching behavior, and the coverage dependence of the fluorescence intensity.
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
Matter-wave dualism is a fundamental concept in quantum physics. The observation of wave properties of heavy organic molecules can be used to approach the borderline between classical and quantum physics. Up to which mass and size do particles or molecules still have wave properties? This question is subject to be answered within this thesis and as part of the international nanoquestfit-project where many researchers of different disciplines are involved. \nThis thesis is a summary of the work done within a research collaboration between the group of Prof. Dr. Marcel Mayor (University of Basel) and the group of Prof. Dr. Markus Arndt (University of Vienna). The work is mainly focused on the development of novel quantum interference experiments that imply the development of new synthetic strategies towards tailor-made molecules. Novel interferometers have been developed by the Arndt group and therefore the molecular requirements changed strongly within the past years. The syntheses of these tailor-made molecules were performed by the author in the laboratories of Prof. Mayor in Basel. Quantum interference experiments and the preliminary investigations described within this work, namely the thermal stability test, the desorption studies and the laser-induced acoustic desorption have been performed by the Arndt group in Vienna. \nInvestigations at the interface of quantum and classical physics are a fascinating part of the research. The final goal is to approach the quantum-to-classical transition by the observation of quantum properties of large and complex molecules. In order to study the wave nature of such particles—a purely quantum mechanical phenomenon—synthetic procedures towards tailor-made compounds are developed to improve the observation of this phenomenon through matter-wave experiments. \nAt the starting point of this work, a series of highly fluorinated porphyrin-monomers set a new benchmark in high-mass quantum interference experiments. The highest masses of particles used in quantum interference experiments were around 10’000 g/mol. Thus, our objective was to reach masses up to 25’000 g/mol with the suitable features for the quantum interferometry experiments. \nIn the first chapter of this thesis, the principle of interferometry, the development and evolution of this technology are presented. In the subsequent chapters, the different synthetic approaches of the tailor-made molecules designed to improve the measurements and achieve the goal of this thesis are described. \nThe main part of this thesis is focused on the synthesis of tailor-made molecules for quantum interference experiments. In a first part, the synthesis of a novel, more massive fluorinated phthalocyanine is presented. That phthalocyanine was used in far-field quantum interference experiments. Unfortunately, the molecular requirements could not been tuned to observe wave-particle duality in these experiments. The second part focuses on the synthesis of three different molecular libraries. Molecular libraries are mixtures of molecules having the same core but a to some extent random number of long perfluorinated chains. The individual members within the library were observable in MALDI-TOF mass spectrometry. We attached the chains to three different cores to obtain three different molecular libraries. To produce a first generation of libraries we used diacetylene bond porphyrin-dimer. The rather limited reaction scope of diacetylene bond porphyrins was enhanced by the second generation of tetramers and pentamers. To compare the modularity of the synthesis of oligo-porphyrin systems two additional cores, a porphyrin-dimer and a porphyrin-trimer, have also been synthesized. The possibility to produce a molecular beam with the three molecular-libraries has been investigated by thermal studies, desorption experiments and laser-induced acoustic desorption. \nThe last part of the thesis is focused on the synthesis of photocleavable tags that can be attached to model compounds. These tags are synthesized since novel quantum interference experiments are based on light gratings where a mass difference is supposed to be observed at the detector level upon cleavage. The final idea is, in the near future, to attach these molecules to large particles, such as metal-nanoparticles, clusters or proteins. It is expected to enable the detection of mass differences of the intact clusters and the clusters with the cleaved tags. Three different model compounds have been synthesized. The cleavage of the tags was proven in solution upon irradiation of UV-light in solution, where a constant and reproducible decay was observed. In future quantum interference experiments, the cleavage should be performed in gas-phase as a final prove of concept. The molecules are currently under investigations in the Arndt group.