Uptake of ammonia by ice surfaces at atmospheric temperatures.

We present an ambient pressure X-ray photoelectron spectroscopy investigation of the adsorption of ammonia on ice over the temperature range -23 °C to -50 °C. Previous flow tube studies have shown significant uptake of ammonia to ice at these temperatures, which was linked to the incorporation of ammonium into the ice crystal lattice. Our present investigation shows a significant uptake of ammonia to the ice interface, with ammonia concentrations exceeding those measured in past studies for the case of bulk snow and ice.

Multiphase Chemistry in the Atmosphere.

Earth's atmosphere comprises a complex mix of gas and condensed phases, where condensed phases facilitate multiphase chemical reactions that would not occur in the gas phase alone. These reactions drive dynamic physical and chemical processes across various spatial and temporal scales, playing a crucial role in the cycling of atmospheric trace constituents. Multiphase chemistry significantly influences geochemical cycles, human health, and climate.

A sub-100 nm thickness flat jet for extreme ultraviolet to soft X-ray absorption spectroscopy.

Experimental characterization of the structural, electronic and dynamic properties of dilute systems in aqueous solvents, such as nanoparticles, molecules and proteins, are nowadays an open challenge. X-ray absorption spectroscopy (XAS) is probably one of the most established approaches to this aim as it is element-specific. However, typical dilute systems of interest are often composed of light elements that require extreme-ultraviolet to soft X-ray photons.

Deconvolution of the X-ray absorption spectrum of -1,3-butadiene with resonant Auger spectroscopy.

High-resolution carbon K-edge X-ray photoelectron, X-ray absorption, non-resonant and resonant Auger spectra are presented of gas phase -1,3-butadiene alongside a detailed theoretical analysis utilising nuclear ensemble approaches and vibronic models to simulate the spectroscopic observables. The resonant Auger spectra recorded across the first pre-edge band reveal a complex evolution of different electronic states which remain relatively well-localised on the edge or central carbon sites. The results demonstrate the sensitivity of the resonant Auger observables to the weighted contributions from multiple electronic states.

Jahn-Teller effects in initial and final states: high-resolution X-ray absorption, photoelectron and Auger spectroscopy of allene.

Carbon K-edge resonant Auger spectra of gas-phase allene following excitation of the pre-edge 1s → π* transitions are presented and analysed with the support of EOM-CCSD/cc-pVTZ calculations. X-Ray absorption (XAS), X-ray photoelectron (XPS), valence band and non-resonant Auger spectra are also reanalysed with a series of computational approaches. The results presented demonstrate the importance of including nuclear ensemble effects for simulating X-ray observables and as an effective strategy for capturing Jahn-Teller effects in spectra.

Charge-transfer and impulsive electronic-to-vibrational energy conversion in ferricyanide: ultrafast photoelectron and transient infrared studies.

The photophysics of ferricyanide in HO, DO and ethylene glycol was studied upon excitation of ligand-to-metal charge transfer (LMCT) transitions by combining ultrafast photoelectron spectroscopy (PES) of liquids and transient vibrational spectroscopy. Upon 400 nm excitation in water, the PES results show a prompt reduction of the Fe to Fe and a back electron transfer in ∼0.5 ps concomitant with the appearance and decay of a strongly broadened infrared absorption at ∼2065 cm.

Harmonium: An Ultrafast Vacuum Ultraviolet Facility.

Harmonium is a vacuum ultraviolet (VUV) photon source built within the Lausanne Centre for Ultrafast Science (LACUS). Utilising high harmonic generation, photons from 20-110 eV are available to conduct steady-state or ultrafast photoelectron and photoion spectroscopies (PES and PIS). A pulse preserving monochromator provides either high energy resolution (70 meV) or high temporal resolution (40 fs).