ABSTRACT
TEMPUS is a new detector system being developed for photon science. It is based on the Timepix4 chip and, thus, it can be operated in two distinct modes: a photon-counting mode, which allows for conventional full-frame readout at rates up to 40â kfps; and an event-driven time-stamping mode, which allows excellent time resolution in the nanosecond regime in measurements with moderate X-ray flux. In this paper, the initial prototype, a single-chip device, is introduced, and the readout system described. Moreover, and in order to evaluate its capabilities, some tests were performed at PETRAâ III and ESRF for which results are also presented.
ABSTRACT
Water dimer (H2O)2âa vital component of the earth's atmosphereâis an important prototypical hydrogen-bonded system. It provides direct insights into fundamental chemical and biochemical processes, e.g., proton transfer and ionic supramolecular dynamics, occurring in astro- and atmospheric chemistry. Exploiting a purified molecular beam of water dimer and multimass ion imaging, we report the simultaneous detection of all generated ion products of (H2O)2+ fragmentation following single ionization. Detailed information about ion yields and reaction energetics of 13 ion-radical pathways, 6 of which are new, of (H2O)2+ are presented, including strong 18O-isotope effects.
ABSTRACT
Recent developments in X-ray free-electron lasers have enabled a novel site-selective probe of coupled nuclear and electronic dynamics in photoexcited molecules, time-resolved X-ray photoelectron spectroscopy (TRXPS). We present results from a joint experimental and theoretical TRXPS study of the well-characterized ultraviolet photodissociation of CS2, a prototypical system for understanding non-adiabatic dynamics. These results demonstrate that the sulfur 2p binding energy is sensitive to changes in the nuclear structure following photoexcitation, which ultimately leads to dissociation into CS and S photoproducts. We are able to assign the main X-ray spectroscopic features to the CS and S products via comparison to a first-principles determination of the TRXPS based on ab initio multiple-spawning simulations. Our results demonstrate the use of TRXPS as a local probe of complex ultrafast photodissociation dynamics involving multimodal vibrational coupling, nonradiative transitions between electronic states, and multiple final product channels.
ABSTRACT
We modulate the atomic structure of bilayer graphene by driving its lattice at resonance with the in-plane E_{1u} lattice vibration at 6.3 µm. Using time- and angle-resolved photoemission spectroscopy (tr-ARPES) with extreme-ultraviolet (XUV) pulses, we measure the response of the Dirac electrons near the K point. We observe that lattice modulation causes anomalous carrier dynamics, with the Dirac electrons reaching lower peak temperatures and relaxing at faster rate compared to when the excitation is applied away from the phonon resonance or in monolayer samples. Frozen phonon calculations predict dramatic band structure changes when the E_{1u} vibration is driven, which we use to explain the anomalous dynamics observed in the experiment.
ABSTRACT
We report the first demonstration of a solid state laser passively mode-locked through the saturable absorption of short-wavelength intersubband transitions in doped quantum wells: a continuous wave Ti:sapphire laser end-pumped Tm,Ho:YAG laser at the center wavelength of 2.091 mum utilizing intersubband transitions in narrow In(0.53)Ga(0.47)As/Al(0.53)As(0.47)Sb quantum wells. Stable passive mode-locking operation with maximum average output power of up to 160 mW for 2.9 W of the absorbed pump power could last for hours without external interruption and a mode-locked pulse with duration of 60 ps at repetition rate of 106.5 MHz was generated.