Experiments
We use photoemission spectroscopy of liquids. The experimental technique has been enabled by introducing liquid microjets into the vacuum, establishing a method called liquid-jet photoelectron spectroscopy (LJ-PES). Both the light source and the electron analyzer are focused near the injection point, enabling measurements of photoemission spectra just before the liquid rapidly evaporates and freezes down the stream. Since establishing a reliable approach to absolute energy calibration in 2021, we can now measure binding energies with high precision. This enables us to detect smaller changes arising from various interactions in the liquid.
The need for a high-quality soft X-ray light source for our experiments brings us to synchrotron facilities. There, we perform the measurements several times per semester. We also use their custom-made LJ-PE spectrometers. We have collaborations with the facilities of BESSY II (Germany), DESY (Germany), MAX IV (Sweden), and SOLEIL (France).
We use quantum-chemical computations to accompany some of our experimental data. In many cases, they help us to fully interpret the underlying processes or even predict the magnitude of the effect that we want to study.
Research areas
ESCA (Electron Spectroscopy for Chemical Analysis, also known as X-ray photoelectron spectroscopy) has become a powerful conventional analytical method for solids and gases. We are expanding the technique to the realm of liquids. We focus on establishing the method as an analytical tool in chemistry, highlighting its surface-sensitivity, ultrafast nature, and ability to provide a full electronic structure of liquid-phase molecules.
The world of liquids exhibits various X-ray-initiated electronic relaxation processes that lead to electron emission and can be, therefore, also recorded in our measurements. Some of these processes are unique to liquids. Moreover, they are extremely specific, as they involve the nearest neighboring molecules. This provides us with an unprecedented analytical probe of coordination and a weakly bonded environment. We use these processes to study biological interactions and the solvation of molecules.
Using photoemission spectroscopy, we study ion pairing in solutions. This is important in various fields, ranging from biological sensing via receptors to processes in ion batteries. We systematically explore the effect of the size, charge, geometry, and concentration on forming ion pairs. The topic is closely connected to studying solvation shells around molecules or ions. We focus on disentangling specific solvation patterns and their effect on the measured binding energies.
We study biologically interesting acid–base systems in pH-dependent measurements. Specifically, we utilize the ultrafast nature of the photoionization process to probe the proton sharing and localization vs. delocalization. This is important in enzyme-driven metabolic pathways such as the citric acid cycle.