Imaging the Renner-Teller effect using laser-induced electron diffraction.

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS2) in the [Formula: see text] excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS2 molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the [Formula: see text] excited state in neutral CS2, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS2, which is known to appear as a two-center scatterer.

An atomically thin matter-wave beamsplitter.

Matter-wave interferometry has become an essential tool in studies on the foundations of quantum physics and for precision measurements. Mechanical gratings have played an important role as coherent beamsplitters for atoms, molecules and clusters, because 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, and the undesired dephasing may prevent interferometry with massive objects. Here, we explore how to minimize this perturbation by reducing the thickness of the diffraction mask to its ultimate physical limit, that is, the thickness of a single atom. We have fabricated diffraction masks in single-layer and bilayer graphene as well as in a 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 ultrathin 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 of 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.

Cavity-Assisted Manipulation of Freely Rotating Silicon Nanorods in High Vacuum.

Optical control of nanoscale objects has recently developed into a thriving field of research with far-reaching promises for precision measurements, fundamental quantum physics and studies on single-particle thermodynamics. Here, we demonstrate the optical manipulation of silicon nanorods in high vacuum. Initially, we sculpture these particles into a silicon substrate with a tailored geometry to facilitate their launch into high vacuum by laser-induced mechanical cleavage. We manipulate and trace their center-of-mass and rotational motion through the interaction with an intense intracavity field. Our experiments show that the anisotropy of the nanorotors leads to optical forces that are three times stronger than on silicon nanospheres of the same mass. The optical torque experienced by the spinning rods will enable cooling of the rotational motion and torsional optomechanics in a dissipation-free environment.

Sensitivity of a superconducting nanowire detector for single ions at low energy.

We report on the characterization of a superconducting nanowire detector for ions at low kinetic energies. We measure the absolute single-particle detection efficiency η and trace its increase with energy up to η = 100%. We discuss the influence of noble gas adsorbates on the cryogenic surface and analyze their relevance for the detection of slow massive particles. We apply a recent model for the hot-spot formation to the incidence of atomic ions at energies between 0.2 and 1 keV. We suggest how the differences observed for photons and atoms or molecules can be related to the surface condition of the detector and we propose that the restoration of proper surface conditions may open a new avenue for SSPD-based optical spectroscopy on molecules and nanoparticles.

A superconducting NbN detector for neutral nanoparticles.

We present a proof-of-principle study of superconducting single photon detectors (SSPD) for the detection of individual neutral molecules/nanoparticles at low energies. The new detector is applied to characterize a laser desorption source for biomolecules and allows retrieval of the arrival time distribution of a pulsed molecular beam containing the amino acid tryptophan, the polypeptide gramicidin as well as insulin, myoglobin and hemoglobin. We discuss the experimental evidence that the detector is actually sensitive to isolated neutral particles.

UV and VUV ionization of organic molecules, clusters, and complexes.

The generation of organic particle beams is studied in combination with photoionization using UV radiation at 266 nm and vacuum ultraviolet (VUV) light at 157 nm. Single-photon ionization with pulsed VUV light turns out to be sensitive enough to detect various large neutral biomolecular complexes ranging from metal-amino acid complexes to nucleotide clusters and aggregates of polypeptides. Different biomolecular clusters are shown to exhibit rather specific binding characteristics with regard to the various metals that are codesorbed in the source. We also find that the ion signal of gramicidin can be increased by a factor of 15 when the photon energy is increased from 4.66 to 7.9 eV.

Gas-phase formation of large neutral alkaline-earth metal tryptophan complexes.

We report on the first observation of isolated large neutral metal amino acid complexes such as Trp(n)Me(k), with Me=Ca, Ba, Sr, cluster combinations covering n=1...33, k=0..2 and masses beyond 6500 u. The cluster beam is generated using UV laser desorption from a mixed powder of alkaline-earth metal salts and tryptophan inside a cluster mixing channel. The particles are detected using VUV photoionization followed by time-of-flight mass spectroscopy. The enhanced stability of metal amino acid clusters over pure amino acid clusters is substantiated in molecular dynamics simulations by determining the gain in binding energy related to the inclusion of the metal atoms.

Hydration dependent dynamics in sol-gel encapsulated myoglobin.

In this work we study the effect of hydration on the dynamics of a protein in confined geometry, i.e. encapsulated in a porous silica matrix. Using elastic neutron scattering we investigate the temperature dependence of the mean square displacements of non-exchangeable hydrogen atoms of sol-gel encapsulated met-myoglobin. The study is extended to samples at 0.2, 0.3 and 0.5 g water/g protein fractions and comparison is made with met-myoglobin powders at the same average hydration and with a dry powder sample. Elastic data are analysed using a model of dynamical heterogeneity to take into account deviations of elastic intensity from gaussian behaviour in a large momentum transfer range and reveal a specific, model independent, effect of sol-gel confinement on protein dynamics, consisting mainly in a reduction of large-scale motions that are activated at temperatures larger than approximately 230 K. Surprisingly, the effect of confinement depends markedly on hydration and has a maximum at about 35% water/protein fraction corresponding to full first shell hydration. The presence of hydration-dependent MSD also in encapsulated met-Mb strongly supports the idea that the effect of sol-gel confinement on protein dynamics involves a modification of the structural/dynamical properties of the co-encapsulated solvent more than direct protein-matrix interactions.