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Matter-wave interferometry with molecules is intriguing both because it demonstrates a fundamental quantum phenomenon and because it opens avenues to quantum-enhanced measurements in physical chemistry. One great challenge in such experiments is to establish matter-wave beam splitting mechanisms that are efficient and applicable to a wide range of particles. In the past, continuous standing light waves in the visible spectral range were used predominantly as phase gratings, while pulsed vacuum ultraviolet light found applications in photo-ionisation gratings. Here, we explore the regime of continuous, intense deep-ultraviolet ($\rm >1 MW/cm^2$, $\rm 266\,nm$) light masks, where a rich variety of photo-physical and photo-chemical phenomena and relaxation pathways must be considered. The improved understanding of the mechanisms in this interaction opens new potential pathways to protein interferometry and to matter-wave enhanced sensing of molecular properties., Comment: 11 pages, 8 figures. Supplemental information is included

Probing the universal low temperature magnetic field scaling of Kondo-correlated quantum dots via electrical conductance has proved to be experimentally challenging. Here, we show how to probe this in nonlinear thermocurrent spectroscopy applied to a molecular quantum dot in the Kondo regime. Our results demonstrate that the bias-dependent thermocurrent is a sensitive probe of universal Kondo physics, directly measures the splitting of the Kondo resonance in a magnetic field, and opens up possibilities for investigating nanosystems far from thermal and electrical equilibrium., Comment: Published version, including Supplementary Material main text:6 pages, 4 figures. SI: 55 pages, 22 figures

Single molecules are nanoscale thermodynamic systems with few degrees of freedom. Thus, the knowledge of their entropy can reveal the presence of microscopic electron transfer dynamics, that are difficult to observe otherwise. Here, we apply thermocurrent spectroscopy to directly measure the entropy of a single free radical molecule in a magnetic field. Our results allow us to uncover the presence of a singlet to triplet transition in one of the redox states of the molecule, not detected by conventional charge transport measurements. This highlights the power of thermoelectric measurements which can be used to determine the difference in configurational entropy between the redox states of a nanoscale system involved in conductance without any prior assumptions about its structure or microscopic dynamics.

The appealing feature of molecular electronics is the possibility of exploiting functionality built within a single molecule. This functionality can be employed, for example, for sensing or switching purposes. Thus, ideally, the associated conductance changes should be sizable upon application of external stimuli. Here, we show that a molecular spring can be mechanically compressed or elongated to tune its conductance by up to an order of magnitude by controlling the quantum interference between electronic pathways. Oscillations in the conductance occur when the stress built up in the molecule is high enough to allow the anchoring groups to move along the surface in a stick-slip-like fashion. The mechanical control of quantum interference effects and the resulting large change in molecular conductance open the door for applications in, e.g., a minute mechanosensitive sensing device functional at room temperature., Comment: 23 pages, 6 figures

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.

Matter waves, as introduced by de Broglie in 1923, are a fundamental quantum phenomenon, describing the delocalized center of mass motion of massive bodies and we show here their sensitivity to the molecular structure of constitutional isomers., Comment: 4 pages, 3 figures

We investigate the influence of thermally activated internal molecular dynamics on the phase shifts of matter waves inside a molecule interferometer. While de Broglie physics generally describes only the center-of-mass motion of a quantum object, our experiment demonstrates that the translational quantum phase is sensitive to dynamic conformational state changes inside the diffracted molecules. The structural flexibility of tailor-made hot organic particles is sufficient to admit a mixture of strongly fluctuating dipole moments. These modify the electric susceptibility and through this the quantum interference pattern in the presence of an external electric field. Detailed molecular dynamics simulations combined with density functional theory allow us to quantify the time-dependent structural reconfigurations and to predict the ensemble-averaged square of the dipole moment which is found to be in good agreement with the interferometric result. The experiment thus opens a new perspective on matter wave interferometry as it demonstrates for the first time that it is possible to collect structural information about molecules even if they are delocalized over more than hundred times their own diameter., Comment: 5 pages, 3 figures

The observation of interference patterns in double-slit experiments with massive particles is generally regarded as the ultimate demonstration of the quantum nature of these objects. Such matter-wave interference has been observed for electrons, neutrons, atoms and molecules and it differs from classical wave-physics in that it can even be observed when single particles arrive at the detector one by one. The build-up of such patterns in experiments with electrons has been described as the "most beautiful experiment in physics". Here we show how a combination of nanofabrication and nanoimaging methods allows us to record the full two-dimensional build-up of quantum diffraction patterns in real-time for phthalocyanine molecules PcH2 and their tailored derivatives F24PcH2 with a mass of 1298 amu. A laser-controlled micro-evaporation source was used to produce a beam of molecules with the required intensity and coherence and the gratings were machined in 10 nm thick silicon nitride membranes to reduce the effect of van der Waals forces. Wide-field fluorescence microscopy was used to detect the position of each molecule with an accuracy of 10 nm and to reveal the build-up of a deterministic ensemble interference pattern from stochastically arriving and internally hot single molecules., Comment: Related video: http://www.youtube.com/watch?v=wDx8tu-iX8U

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., Comment: 6 pages, 3 figures

The Kondo effect arises due to the interaction between a localized spin and the electrons of a surrounding host. Studies of individual magnetic impurities by scanning tunneling spectroscopy have renewed interest in Kondo physics; however, a quantitative comparison with theoretical predictions remained challenging. Here we show that the zero-bias anomaly detected on an organic radical weakly coupled to a Au (111) surface can be described with astonishing agreement by perturbation theory as originally developed by Kondo 60 years ago. Our results demonstrate that Kondo physics can only be fully conceived by studying both temperature and magnetic field dependence of the resonance. The identification of a spin 1/2 Kondo system is of relevance not only as a benchmark for predictions for Kondo physics but also for correlated electron materials in general., Comment: 6 pages, 4 figures, published article PDF

We analyze quantum interference and decoherence effects in single-molecule junctions both experimentally and theoretically by means of the mechanically controlled break junction technique and density-functional theory. We consider the case where interference is provided by overlapping quasi-degenerate states. Decoherence mechanisms arising from the electronic-vibrational coupling strongly affect the electrical current flowing through a single-molecule contact and can be controlled by temperature variation. Our findings underline the all-important relevance of vibrations for understanding charge transport through molecular junctions., Comment: 5 pages, 4 figures

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., Comment: 13 pages, 4 figures