Fs Temporal Resolution Research Articles

Probing quantum optical excitations with fast electrons

Probing optical excitations with nanometer resolution is important for understanding their dynamics and interactions down to the atomic scale. Electron microscopes currently offer the unparalleled ability of rendering spatially-resolved electron spectra with combined meV and sub-nm resolution, while the use of ultrafast optical pulses enables fs temporal resolution and exposure of the electrons to ultraintense confined optical fields. Here, we theoretically investigate fundamental aspects of the interaction of fast electrons with localized optical modes that are made possible by these advances. We use a quantum-optics description of the optical field to predict that the resulting electron spectra strongly depend on the statistics of the sample excitations (bosonic or fermionic) and their population (Fock, coherent, or thermal), whose autocorrelation functions are directly retrieved from the ratios of electron gain intensities. We further explore feasible experimental scenarios to probe the quantum characteristics of the sampled excitations and their populations.

Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment.

We present a general experimental concept for jitter-free pump and probe experiments at free electron lasers. By generating pump and probe pulse from one and the same X-ray pulse using an optical split-and-delay unit, we obtain a temporal resolution that is limited only by the X-ray pulse lengths. In a two-color X-ray pump and X-ray probe experiment with sub 70 fs temporal resolution, we selectively probe the response of orbital and charge degree of freedom in the prototypical functional oxide magnetite after photoexcitation. We find electronic order to be quenched on a time scale of (30 ± 30) fs and hence most likely faster than what is to be expected for any lattice dynamics. Our experimental result hints to the formation of a short lived transient state with decoupled electronic and lattice degree of freedom in magnetite. The excitation and relaxation mechanism for X-ray pumping is discussed within a simple model leading to the conclusion that within the first 10 fs the original photoexcitation decays into low-energy electronic excitations comparable to what is achieved by optical pump pulse excitation. Our findings show on which time scales dynamical decoupling of degrees of freedom in functional oxides can be expected and how to probe this selectively with soft X-ray pulses. Results can be expected to provide crucial information for theories for ultrafast behavior of materials and help to develop concepts for novel switching devices.

Concept of a laser-plasma-based electron source for sub-10-fs electron diffraction

We propose a new concept of an electron source for ultrafast electron diffraction with sub-10~fs temporal resolution. Electrons are generated in a laser-plasma accelerator, able to deliver femtosecond electron bunches at 5 MeV energy with kHz repetition rate. The possibility of producing this electron source is demonstrated using Particle-In-Cell simulations. We then use particle tracking simulations to show that this electron beam can be transported and manipulated in a realistic beamline, in order to reach parameters suitable for electron diffraction. The beamline consists of realistic static magnetic optics and introduces no temporal jitter. We demonstrate numerically that electron bunches with 5~fs duration and containing 1.5~fC per bunch can be produced, with a transverse coherence length exceeding 2~nm, as required for electron diffraction.

Imaging energy-, momentum-, and time-resolved distributions of photoinjected hot electrons in GaAs.

Using time-and angle-resolved photoemission spectroscopy, we determine directly energy-, momentum-, and time-resolved distributions of hot electrons photoinjected into the conduction band of GaAs, a prototypical direct-gap semiconductor. The nascent distributions of photoinjected electrons are captured for different pump photon energies and polarization. The evolutions of hot electron distributions in ultrafast intervalley scattering processes are resolved in momentum space with fs-temporal resolution, revealing an intervalley transition time as short as 20fs.

Mapping multidimensional excited state dynamics using pump-impulsive-vibrational-spectroscopy and pump-degenerate-four-wave-mixing

Pump-impulsive vibrational spectroscopy (pump-IVS) is used to record excited state vibrational dynamics following photoexcitation of two carotenoids, β-carotene and lycopene, with <30 fs temporal resolution, and covering the full vibrational spectrum of the investigated chromophores. The results record the course of S2-S1 internal conversion, followed by vibrational relaxation and decay to the electronic ground state. This interpretation is corroborated by comparison with pump-degenerate-four-wave-mixing (pump-DFWM) experiments on the same systems. The results demonstrate the potential of both time-domain spectroscopic techniques to resolve photochemical dynamics, including fingerprint frequencies which directly reflect changes in bonding and structure in the nascent sample. The exclusive strengths and limitations of these two methods are compared with those presented by the frequency-domain Femtosecond Stimulated Raman Scattering (FSRS) technique, highlighting the complementary nature of the three, and the benefits of using them in concert to investigate vibrational dynamics in reactive species.