Tracking primary radiation-induced processes in matter requires ultrafast sources and high precision timing. While compact laser-driven ion accelerators are seeding the development of novel high instantaneous flux applications, combining the ultrashort ion and laser pulse durations with their inherent synchronicity to trace the real-time evolution of initial damage events has yet to be realized. Here we report on the absolute measurement of proton bursts as short as 3.5±0.7 ps from laser solid target interactions for this purpose. Our results verify that laser-driven ion acceleration can deliver interaction times over a factor of hundred shorter than those of state-of-the-art accelerators optimized for high instantaneous flux. Furthermore, these observations draw ion interaction physics into the field of ultrafast science, opening the opportunity for quantitative comparison with both numerical modelling and the adjacent fields of ultrafast electron and photon interactions in matter.

High order harmonics generated at relativistic intensities have long been recognized as a route to the most powerful extreme ultraviolet pulses. Reliably generating isolated attosecond pulses requires gating to only a single dominant optical cycle, but techniques developed for lower power lasers have not been readily transferable. We present a novel method to temporally gate attosecond pulse trains by combining noncollinear and polarization gating. This scheme uses a split beam configuration which allows pulse gating to be implemented at the high beam fluence typical of multi-TW to PW class laser systems. Scalings for the gate width demonstrate that isolated attosecond pulses are possible even for modest pulse durations achievable for existing and planned future ultrashort high-power laser systems. Experimental results demonstrating the spectral effects of temporal gating on harmonic spectra generated by a relativistic laser plasma interaction are shown.

Energy coupling during relativistically intense laser-matter interactions is encoded in the attosecond motion of strongly driven electrons at the pre-formed plasma-vacuum boundary. Studying and controlling this motion can reveal details about the microscopic processes that govern a vast array of light-matter interaction physics and applications. These include research areas right at the forefront of extreme laser-plasma science such as laser-driven ion acceleration 1 , bright attosecond pulse generation 2,3 and efficient energy coupling for the generation and study of warm dense matter 4 . Here we demonstrate attosecond control over the trajectories of relativistic electron bunches formed during such interactions by studying the emission of extreme ultraviolet (XUV) harmonic radiation. We describe how the precise addition of a second laser beam operating at the second harmonic of the driving laser pulse can significantly transform the interaction by modifying the accelerating potential provided by the fundamental frequency to drive strong coherent emission. Numerical particle-in-cell code simulations and experimental observations demonstrate that this modification is extremely sensitive to the relative phase of the two beams and can lead to significant enhancements in the resulting harmonic yield. This work also reveals that the ability to control these extreme interactions

We report direct experimental measurements with picosecond time resolution of how high energy protons interact with water at extreme dose levels (kGy), delivered in a single pulse with the duration of less than 80 ps. The unique synchronisation possibilities of laser accelerated protons with an optical probe pulse were utilized to investigate the energy deposition of fast protons in water on a time scale down to only a few picoseconds. This was measured using absorbance changes in the water, induced by a population of solvated electrons created in the tracks of the high energy protons. Our results indicate that for sufficiently high doses delivered in short pulses, intertrack effects will affect the yield of solvated electrons. The experimental scheme allows for investigation of the ultrafast mechanisms occurring in proton water radiolysis, an area of physics especially important due to its relevance in biology and for proton therapy.

Recently, measurements of few-picosecond (ps, 10−12 s) pulses of laser-driven protons were realised by the observation of transient opacity in SiO2. This ultrafast response could be understood by the formation of self-trapped excitonic states in the material, creating a rapid de-excitation channel for conduction band electrons. Here we extend this work to examine the onset and evolution of an ion-induced opacity in transparent dielectrics, namely multicomponent variants of SiO2. The fast recovery observed in SiO2 is in sharp contrast to borosilicate (BK7) and soda-lime glasses. We find that the opacity decay timescales for BK7 and soda-lime glass are orders of magnitude greater than the 3.5 ps proton pump pulse duration and discuss the underlying processes which may be affecting the extended recovery of the material. Simultaneous probing with 2nd harmonic radiation allows estimates of ultrafast electron dynamics due to proton interactions in matter to be investigated, this indicates that a rapid evolution of an initially unstructured ion-induced dose distribution seeds the longer term recovery pathways in the irradiated dielectrics. When combined, these results demonstrate the efficacy of utilising ultrafast laser-driven ionising radiation along with highly synchronised probe pulses to enable the study of ion-induced damage in matter on ultrafast timescales in real time.