Fano interference in quantum resonances from angle-resolved elastic scattering

Asymmetric spectral line shapes are a hallmark of interference of a quasi-bound state with a continuum of states. Such line shapes are well known for multichannel systems, for example, in photoionization or Feshbach resonances in molecular scattering. On the other hand, in resonant single channel scattering, the signature of such interference may disappear due to the orthogonality of partial waves. Here, we show that probing the angular dependence of the cross section allows us to unveil asymmetric Fano profiles also in a single channel shape resonance. We observe a shift in the peak of the resonance profile in the elastic collisions between metastable helium and deuterium molecules with detection angle, in excellent agreement with theoretical predictions from full quantum scattering calculations. Using a model description for the partial wave interference, we can disentangle the resonant and background contributions and extract the relative phase responsible for the characteristic Fano-like profiles from our experimental measurements.

Light Scattering by Pure Water and Seawater: Recent Development

Light scattering by pure water and seawater is a fundamental optical property that plays a critical role in ocean optics and ocean color studies. We briefly review the theory of molecular scattering in liquid and electrolyte solutions and focus on the recent developments in modeling the effect of pressure, extending to extreme environments, and evaluating the effect of salinity on the depolarization ratio. We demonstrate how the modeling of seawater scattering can be applied to better understand spectral absorption and attenuation of pure water and seawater. We recommend future efforts should be directed at measuring the polarized components of scattering by pure water over a greater range of wavelengths, temperature, salinity, and pressure to constrain and validate the model and to improve our knowledge of the water’s depolarization ratio.

Exploiting Aeolus Level-2B Winds to Better Characterize Atmospheric Motion Vector Bias and Uncertainty

The need for highly accurate atmospheric wind observations is a high priority in the science community, and in particular numerical weather prediction (NWP). To address this requirement, this study leverages Aeolus wind LIDAR Level-2B data provided by the European Space Agency (ESA) to better characterize atmospheric motion vector (AMV) bias and uncertainty, with the eventual goal of potentially improving AMV algorithms. AMV products from geostationary (GEO) and low-Earth polar orbiting (LEO) satellites are compared with reprocessed Aeolus horizontal line-of-sight (HLOS) global winds observed in August and September 2019. Winds from two of the four Aeolus observing modes are utilized for comparison with AMVs: Rayleigh-clear (derived from the molecular scattering signal) and Mie-cloudy (derived from particle scattering). For the most direct comparison, quality controlled (QC’d) Aeolus winds are collocated with quality controlled AMVs in space and time, and the AMVs are projected onto the Aeolus HLOS direction. Mean collocation differences (MCD) and standard deviation (SD) of those differences (SDCD) are determined from comparisons based on a number of conditions, and their relation to known AMV bias and uncertainty estimates is discussed. GOES-16 and LEO AMV characterizations based on Aeolus winds are described in more detail. Overall, QC’d AMVs correspond well with QC’d Aeolus HLOS wind velocities (HLOSV) for both Rayleigh-clear and Mie-cloudy observing modes, despite remaining biases in Aeolus winds after reprocessing. Comparisons with Aeolus HLOSV are consistent with known AMV bias and uncertainty in the tropics, NH extratropics, and in the Arctic, and at mid- to upper-levels in both clear and cloudy scenes. SH comparisons generally exhibit larger than expected SDCD, which could be attributed to height assignment errors in regions of high winds and enhanced vertical wind shear. GOES-16 water vapor clear-sky AMVs perform best relative to Rayleigh-clear winds, with small MCD (-0.6 m s-1 to 0.1 m s-1) and SDCD (5.4–5.6 m s-1) in the NH and tropics that fall within the accepted range of AMV error values relative to radiosonde winds. Compared to Mie-cloudy winds, AMVs exhibit similar MCD and smaller SDCD (~4.4–4.8 m s-1) throughout the troposphere. In polar regions, Mie-cloudy comparisons have smaller SDCD (5.2 m s-1 in the Arctic, 6.7 m s-1 in the Antarctic) relative to Rayleigh-clear comparisons, which are larger by 1–2 m s-1. The level of agreement between AMVs and Aeolus winds varies per combination of conditions including the Aeolus observing mode coupled with AMV derivation method, geographic region, and height of the collocated winds. It is advised that these stratifications be considered in future comparison studies and impact assessments involving 3D winds. Additional bias corrections to the Aeolus dataset are anticipated to further refine the results.

A Bi-Axial Quantum State That Controls Molecular Collisions Like a Double-Slit Interferometer

To control molecular scattering, we consider hydrogen molecules prepared in a coherent superposition of m states within a single rovibrational (v, j) energy eigenstate using Stark-induced adiabatic Raman passage (SARP). Specifically, SARP can prepare a bi-axial state of the HD molecule in which the HD bond axis exists simultaneously in two possible alignments at right angles to one another with a well-defined relative phase. We show that scattering from this biaxial state will interfere, resulting in a φ -dependent scattering intensity distribution, where φ is the azimuthal angle about the collision velocity direction. Using the scattering matrix extracted from our experiments on the rotationally inelastic collisions of quantum state prepared HD at low temperatures, we calculate the differential scattering cross-section dσ/dΩ, which shows an interference pattern as function of θ and φ in the image plane perpendicular to the collision velocity. The calculated scattering image shows that scattering from the bi-axial state directs molecules along well-defined angles, corresponding to interference maxima. Thus, the bi-axial state behaves like a double slit for molecular scattering. Moreover, by rotating the polarizations of the SARP preparation lasers, we can control the interference thereby altering the scattering angular distribution. This molecular interferometer, which experimentally measures the relative phases of the scattering matrix elements, allows a direct test of theoretical calculations on important, fundamental collision processes.

Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.