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Marco De Pas

Publications and source records attributed to Marco De Pas.

5 recordsLinked to original sources

Non-equilibrium state during proton-deuteron exchange at a liquid-liquid interface

Proton-deuteron exchange is a very fast process, even across macroscopic length scales. Here we directly and quantitatively measure the formation of HDO within the first 100 microseconds of the reaction at the liquid-liquid interface between D$_2$O and H$_2$O, using a fast-flowing liquid flat jet combined with infrared spectroscopic imaging. We demonstrate that, at early stages HDO formation is reaction-limited, set by the low concentration of the hydroxide and hydronium ions that mediate the exchange. As the ion concentration rises, the rate rapidly approaches the diffusion limit. The reaction rate constant we extract is consistent with the picosecond timescale of the elementary proton-deuteron exchange. Access to these microsecond kinetics reveals a non-equilibrium state in the early H$_2$O/D$_2$O interface: the two liquids are fully mixed by diffusion, yet the HDO concentration remains well below equilibrium. Quantitative imaging of reactant and product concentrations at well-defined liquid-liquid interfaces, as introduced here, will enable the study of fast kinetics across a wide range of chemical reactions.

physics.chem-ph

A two-color dual-oscillator infrared free-electron laser

We report on the design and performance of a two-color dual-oscillator infrared free-electron laser (FEL). The mid-infrared (MIR) FEL at the Fritz Haber Institute (FHI FEL) has been upgraded to include a second oscillator FEL beamline that permits lasing in the far-infrared (FIR) regime from 4.5 μm to 175 μm. In addition, a 500 MHz kicker cavity has been installed downstream of the electron accelerator. It allows to deflect electron bunches of up to 50 MeV energy alternately left and right by an angle of {\pm}2°. It can, thus, split the high-repetition-rate (1 GHz) electron bunch train from the accelerator into two bunch trains of 500 MHz repetition rate each; one is steered to the MIR FEL and the other one to the new FIR FEL. In this two-color mode of simultaneous, synchronized operation the wavelengths in both FELs can be tuned independently over wide ranges of up to a factor of four each by undulator-gap variation. In addition, two-color operation is also available at reduced repetition rates (e.g. 55.6 MHz of both MIR and FIR pulses), as needed for some applications. This unique two-color mode opens up a wealth of novel user applications such as, MIR-FIR pump-probe experiments.

physics.acc-ph

Controlling isomer population using a dual-oscillator infrared free-electron laser

We report on the control and characterization of the isomer population of ions inside superfluid helium nanodroplets, using two-color operation of a dual-oscillator infrared free-electron laser. The timing of both lasers is highly synchronized, and their frequencies (or "colors") can be tuned independently over a wide range. Interaction of the singly deuterated proton-bound dimer of dihydrogen phosphate and formate inside helium nanodroplets with both colors enables the control over its isomer population and the recording of - one-color hidden - infrared spectra of individual isomers.

physics.chem-ph

Infrared super-resolution wide-field microscopy using sum-frequency generation

Super-resolution microscopy in the visible is an established powerful tool in several disciplines. In the infrared (IR) spectral range, however, no comparable schemes have been demonstrated to date. In this work, we experimentally demonstrate super-resolution microscopy in the IR range ($λ_{IR}\approx 10-12\,μ$m) using IR-visible sum-frequency generation. We operate our microscope in a wide-field scheme and image localized surface phonon polaritons in 4H-SiC nanostructures as a proof-of-concept. With this technique, we demonstrate an enhanced spatial resolution of $\simλ_{IR}/9$, enabling to resolve the polariton resonances in individual sub-diffractional nanostructures with sub-wavelength spacing. Furthermore we show, that this resolution allows to differentiate between spatial patterns associated with different polariton modes within individual nanostructures.

physics.optics

A compact radiofrequency drive based on interdependent resonant circuits for precise control of ion traps

Paul traps are widely used to confine electrically charged particles like atomic and molecular ions by using an intense radiofrequency (RF) field, typically obtained by a voltage drop on capacitative electrodes placed in vacuum. We present a RF drive realized on a compact printed circuit board (PCB) and providing a high-voltage RF signal to a quadrupole Paul trap. The circuit is formed by four interdependent resonant circuits $-$ each of which connected to an electrode of a Paul trap $-$ fed by low-noise amplifiers, leading to an output voltage of peak-to-peak amplitude up to 200 V at 3.23 MHz. The presence of a single resonant circuit for each electrode ensures a strong control on the voltage drop on each electrode, e.g. by applying a DC field through a bias tee. Additionally, the moderate quality factor Q = 67 of the resonant circuits ensures a fast operation of the drive, which can be turned on and off in less than 10 $μ$s. Finally, the RF lines are equipped with pick-ups that sample the RF in phase and amplitude, thus providing a signal that can be used to actively control the voltage drop at the trap's electrodes. Thanks to its features, this drive is particularly suited for experiments in which high trap stability and excellent micromotion compensation are required.

physics.atom-ph