Emerging beam resonances in atom diffraction from a reflection grating

We report on the observation of emerging beam resonances, well known as Rayleigh-Wood anomalies and threshold resonances in photon and electron diffraction, respectively, in an atom-optical diffraction experiment. Diffraction of He atom beams reflected from a blazed ruled grating at grazing incidence has been investigated. The total reflectivity of the grating as well as the intensities of the diffracted beams reveal anomalies at the Rayleigh angles of incidence, i.e., when another diffracted beam merges parallel to the grating surface. The observed anomalies are discussed in terms of the classical wave-optical model of Rayleigh and Fano.Comment: 4 pages, 3 figure

Second-harmonic phonon spectroscopy of α\alpha-quartz

We demonstrate midinfrared second-harmonic generation as a highly sensitive phonon spectroscopy technique that we exemplify using $\alpha$-quartz (SiO$_2$) as a model system. A midinfrared free-electron laser provides direct access to optical phonon resonances ranging from $350\ \mathrm{cm}^{-1}$ to $1400\ \mathrm{cm}^{-1}$. While the extremely wide tunability and high peak fields of an free-electron laser promote nonlinear spectroscopic studies---complemented by simultaneous linear reflectivity measurements---azimuthal scans reveal crystallographic symmetry information of the sample. Additionally, temperature-dependent measurements show how damping rates increase, phonon modes shift spectrally and in certain cases disappear completely when approaching$T_c=846\ \mathrm{K}$where quartz undergoes a structural phase transition from trigonal$\alpha$-quartz to hexagonal$\beta$-quartz, demonstrating the technique's potential for studies of phase transitions

Second Harmonic Generation from Critically Coupled Surface Phonon Polaritons

Mid-infrared nanophotonics can be realized using sub-diffractional light localization and field enhancement with surface phonon polaritons in polar dielectric materials. We experimentally demonstrate second harmonic generation due to the optical field enhancement from critically coupled surface phonon polaritons at the 6H-SiC-air interface, employing an infrared free-electron laser for intense, tunable, and narrowband mid-infrared excitation. Critical coupling to the surface polaritons is achieved using a prism in the Otto geometry with adjustable width of the air gap, providing full control over the excitation conditions along the polariton dispersion. The calculated reflectivity and second harmonic spectra reproduce the full experimental data set with high accuracy, allowing for a quantification of the optical field enhancement. We also reveal the mechanism for low out-coupling efficiency of the second harmonic light in the Otto geometry. Perspectives on surface phonon polariton-based nonlinear sensing and nonlinear waveguide coupling are discussed

AC electric trapping of neutral atoms

We study the dynamic behavior of ultracold neutral atoms in a macroscopic ac electric trap. Confinement in such a trap is achieved by switching between two saddle-point configurations of the electric field. The gradual formation of a stably trapped cloud is observed and the trap performance is studied versus the switching frequency and the symmetry of the switching cycle. Additionally, the electric field in the trap is mapped out by imaging the atom cloud while the fields are still on. Finally, the phase-space acceptance of the trap is probed by introducing a modified switching cycle. The experimental results are reproduced using full three-dimensional trajectory calculations.Comment: 10 pages, 13 figures, updated version, added journal referenc

Direct Identification of Acetaldehyde Formation and Characterization of the Active Site in the [VPO4].+/C2H4 Couple by Gas‐Phase Vibrational Spectroscopy

The gas‐phase reaction of the heteronuclear oxide cluster [VPO4].+ with C2H4 is studied under multiple collision conditions at 150 K using cryogenic ion‐trap vibrational spectroscopy combined with electronic structure calculations. The exclusive formation of acetaldehyde is directly identified spectroscopically and discussed in the context of the underlying reaction mechanism. In line with computational predictions it is the terminal P=O and not the V=O unit that provides the oxygen atom in the barrier‐free thermal C2H4→CH3CHO conversion. Interestingly, in the course of the reaction, the emerging CH3CHO product undergoes a rather complex intramolecular migration, coordinating eventually to the vanadium center prior to its liberation. Moreover, the spectroscopic structural characterization of neutral C2H4O deserves special mentioning as in most, if not all, ion/molecule reactions, the neutral product is usually only indirectly identified.DFG, 390540038, EXC 2008: UniSysCatDFG, 234149247, SFB 1109: Molekulare Einblicke in Metalloxid-Wasser-Systeme: Strukturelle Evolution, Grenzflächen und AuflösungTU Berlin, Open-Access-Mittel - 201

Trapping of Rb atoms by ac electric fields

We demonstrate trapping of an ultracold gas of neutral atoms in a macroscopic ac electric trap. Three-dimensional confinement is obtained by switching between two saddle-point configurations of the electric field. Stable trapping is observed in a narrow range of switching frequencies around 60 Hz. The dynamic confinement of the atoms is directly visualized at different phases of the ac switching cycle. We observe about 10^5 Rb atoms in the 1 mm^3 large and several microkelvins deep trap with a lifetime of approximately 5 s.Comment: 4 pages, 4 figures; updated version, added journal referenc

Resonant enhancement of second harmonic generation in the mid-infrared using localized surface phonon polaritons in sub-diffractional nanostructures

We report on strong enhancement of mid-infrared second harmonic generation (SHG) from SiC nanopillars due to the resonant excitation of localized surface phonon-polaritons within the Reststrahlen band. The magnitude of the SHG peak at the monopole mode experiences a strong dependence on the resonant frequency beyond that described by the field localization degree and the dispersion of linear and nonlinear-optical SiC properties. Comparing the results for the identical nanostructures made of 4H and 6H SiC polytypes, we demonstrate the interplay of localized surface phonon polaritons with zone-folded weak phonon modes of the anisotropic crystal. Tuning the monopole mode in and out of the region where the zone-folded phonon is excited in 6H-SiC, we observe a prominent increase of the already monopole-enhanced SHG output when the two modes are coupled. Envisioning this interplay as one of the showcase features of mid-infrared nonlinear nanophononics, we discuss its prospects for the effective engineering of nonlinear-optical materials with desired properties in the infrared spectral range.Comment: 16 pages, 3 figure

Quantum reflection of helium atom beams from a microstructured grating

We observe high-resolution diffraction patterns of a thermal-energy helium-atom beam reflected from a microstructured surface grating at grazing incidence. The grating consists of 10-$\mu$m-wide Cr strips patterned on a quartz substrate and has a periodicity of 20 $\mu$m. Fully-resolved diffraction peaks up to the $7^{\rm th}$ order are observed at grazing angles up to 20 mrad. With changes in de Broglie wavelength or grazing angle the relative diffraction intensities show significant variations which shed light on the nature of the atom-surface interaction potential. The observations are explained in terms of quantum reflection at the long-range attractive Casimir-van der Waals potential.Comment: 4 pages, 4 figure

Observation of the Efimov state of the helium trimer

Quantum theory dictates that upon weakening the two-body interaction in a three-body system, an infinite number of three-body bound states of a huge spatial extent emerge just before these three-body states become unbound. Three helium atoms have been predicted to form a molecular system that manifests this peculiarity under natural conditions without artificial tuning of the attraction between particles by an external field. Here we report experimental observation of this long predicted but experimentally elusive Efimov state of $^{4}$He$_{3}$ by means of Coulomb explosion imaging. We show spatial images of an Efimov state, confirming the predicted size and a typical structure where two atoms are close to each other while the third is far away

Gas phase structures and charge localization in small aluminum oxide anions: Infrared photodissociation spectroscopy and electronic structure calculations

We use cryogenic ion trap vibrational spectroscopy in combination with quantum chemical calculations to study the structure of mono- and dialuminum oxide anions. The infrared photodissociation spectra of D2-tagged AlO1-4 − and Al2O3-6 − are measured in the region from 400 to 1200 cm−1. Structures are assigned based on a comparison to simulated harmonic and anharmonic IR spectra derived from electronic structure calculations. The monoaluminum anions contain an even number of electrons and exhibit an electronic closed-shell ground state. The Al2O3-6 − anions are oxygen-centered radicals. As a result of a delicate balance between localization and delocalization of the unpaired electron, only the BHLYP functional is able to qualitatively describe the observed IR spectra of all species with the exception of AlO3 −. Terminal Al–O stretching modes are found between 1140 and 960 cm−1. Superoxo and peroxo stretching modes are found at higher (1120-1010 cm−1) and lower energies (850-570 cm−1), respectively. Four modes in-between 910 and 530 cm−1 represent the IR fingerprint of the common structural motif of dialuminum oxide anions, an asymmetric four-member Al–(O)2–Al ring