Yb:YAG-Pumped, Few-Cycle Optical Parametric Amplifiers

In this chapter, the principle, design, and characteristics of high-efficiency, short-pulse-pumped, few-cycle optical parametric chirped-pulse amplification (OPCPA) systems are reviewed. To this end, the feasibility of two techniques to increase the conversion efficiency of few-cycle OPCPA systems is demonstrated and discussed. The techniques result in 2.5 mJ, 7.5 W pulses and correspond to a pump-to-signal conversion efficiency of 30%. The broadband amplified spectrum supports 5.7 fs. Finally, the feasibility of extending the amplified spectrum to a near-single-cycle regime by using the combination of different crystals and phase matching is shown

Third-generation femtosecond technology

Chirped pulse amplification in solid-state lasers is currently the method of choice for producing high-energy ultrashort pulses, having surpassed the performance of dye lasers over 20 years ago. The third generation of femtosecond technology based on short-pulse-pumped optical parametric chirped pulse amplification (OPCPA) holds promise for providing few-cycle pulses with terawatt-scale peak powers and kilowatt-scale-average powers simultaneously, heralding the next wave of attosecond and femtosecond science. OPCPA laser systems pumped by near-1-ps pulses support broadband and efficient amplification of few-cycle pulses due to their unrivaled gain per unit length. This is rooted in the high threshold for dielectric breakdown of the nonlinear crystals for even shorter pump pulse durations. Concomitantly, short pump pulses simplify dispersion management and improve the temporal contrast of the amplified signal. This thesis covers the main experimental and theoretical steps required to design and operate a high-power, high-energy, few-cycle OPCPA. This includes the generation of a broadband, high-contrast, carrier envelope phase (CEP)-stable seed, the practical use of a high-power thin-disk regenerative amplifier, its efficient use for pumping a multi-stage OPCPA chain and compression of the resulting pulses. A theoretical exploration of the concept and its extension to different modes of operation, including widely-tunable, high-power multi-cycle pulse trains, and ultrabroadband waveform synthesis is presented. Finally, a conceptual design of a field synthesizer with multi-terawatt, multi-octave light transients is discussed, which holds promise for extending the photon energy attainable via high harmonic generation to several kiloelectronvolts, nourishing the hope for attosecond spectroscopy at hard-x-ray wavelengths

Third-generation femtosecond technology

Chirped pulse amplification in solid-state lasers is currently the method of choice for producing high-energy ultrashort pulses, having surpassed the performance of dye lasers over 20 years ago. The third generation of femtosecond technology based on short-pulse-pumped optical parametric chirped pulse amplification (OPCPA) holds promise for providing few-cycle pulses with terawatt-scale peak powers and kilowatt-scale-average powers simultaneously, heralding the next wave of attosecond and femtosecond science. OPCPA laser systems pumped by near-1-ps pulses support broadband and efficient amplification of few-cycle pulses due to their unrivaled gain per unit length. This is rooted in the high threshold for dielectric breakdown of the nonlinear crystals for even shorter pump pulse durations. Concomitantly, short pump pulses simplify dispersion management and improve the temporal contrast of the amplified signal. This thesis covers the main experimental and theoretical steps required to design and operate a high-power, high-energy, few-cycle OPCPA. This includes the generation of a broadband, high-contrast, carrier envelope phase (CEP)-stable seed, the practical use of a high-power thin-disk regenerative amplifier, its efficient use for pumping a multi-stage OPCPA chain and compression of the resulting pulses. A theoretical exploration of the concept and its extension to different modes of operation, including widely-tunable, high-power multi-cycle pulse trains, and ultrabroadband waveform synthesis is presented. Finally, a conceptual design of a field synthesizer with multi-terawatt, multi-octave light transients is discussed, which holds promise for extending the photon energy attainable via high harmonic generation to several kiloelectronvolts, nourishing the hope for attosecond spectroscopy at hard-x-ray wavelengths

Theoretical Study: High Harmonic Generation by Light Transients

The dynamic of electron densities in matter upon the interaction with an intense, few-cycle electric field of light causes variety of nonlinear phenomena. Capturing the spatiotemporal dynamics of electrons calls for isolated attosecond pulses in the X-ray regime, with sufficient flux to allow for: (i) attosecond pump-attosecond probe spectroscopy;or (ii) four-dimensional imaging. Light field synthesizers generate arbitrary sub-cycle, non-sinusoidal waveforms. They have a great potential to overcome the limitations of current laser sources and to extend attosecond pulses towards the X-ray regime. In this paper, we show theoretically how the achievable high-energy, high-power waveforms from current light field synthesizers can be optimized to enhance the harmonic yield at high photon energies and can serve as a promising source for scaling the photon energies of attosecond pulses. We demonstrate that the simulated optimized, non-sinusoidal waveform in this work can increase the photon flux of keV, attosecond pulses by five orders of magnitude compared to the achievable flux from longer wavelength sources and at similar photon energies

Near-Petahertz Fieldoscopy of Liquid

Measuring transient optical field is pivotal not only for understanding ultrafast phenomena but also for quantitative detection of various molecular species in a sample. In this work, we demonstrate near-petahertz electric field detection of a few femtosecond pulses with 2oo attosecond temporal resolution, 10$^8$ detection dynamic range in electric field and sub-femtojoule detection sensitivity, exceeding those reported by the current methods. By field-resolved detection of the impulsively excited molecules in the liquid phase, termed 'femtosecond fieldoscopy', we demonstrate temporal isolation of the response of the target molecules from those of the environment and the excitation pulse. In a proof-of-concept analysis of aqueous and liquid samples, we demonstrate field-sensitive detection of combination bands of 4.13 {\mu}mol ethanol for the first time. This method expands the scope of aqueous sample analysis to higher detection sensitivity and dynamic range, while the simultaneous direct measurements of phase and intensity information pave the path towards high-resolution biological spectro-microscop

Highly Nonlinear Dynamics of In Vivo Deep-Tissue Interaction with Femtosecond Laser Pulses at 1030 nm

We report on the highly nonlinear behavior observed in the central nervous system tissue of zebrafish (Danio rerio) when exposed to femtosecond pulses at 1030 nm. At this irradiation wavelength, photo damage becomes detectable only after exceeding a specific peak intensity threshold, which is independent of the photon flux and irradiation time, distinguishing it from irradiation at shorter wavelengths. Furthermore, we investigate and quantify the role of excessive heat in reducing the damage threshold, particularly during high-repetition-rate operations, which are desirable for label-free and multi-dimensional microscopy techniques. To verify our findings, we examined cellular responses to tissue damage, including apoptosis and the recruitment of macrophages and fibroblasts at different time points post-irradiation. These findings substantially contribute to advancing the emerging nonlinear optical microscopy techniques and provide a strategy for inducing deep-tissue, precise and localized injuries using near-infrared femtosecond laser pulses

Time-domain Compressed Sensing

Ultrashort time-domain spectroscopy, particularly field-resolved spectroscopy, are established methods for identifying the constituents and internal dynamics of samples. However, these techniques are often encumbered by the Nyquist criterion, leading to prolonged data acquisition and processing times as well as sizable data volumes. To mitigate these issues, we have successfully implemented the first instance of time-domain compressed sensing, enabling us to pinpoint the primary absorption peaks of atmospheric water vapor in response to tera-hertz light transients that exceed the Nyquist limit. Our method demonstrates successful identification of water absorption peaks up to 2.5 THz, even for sampling rates where the Nyquist frequency is as low as 0.75 THz, with a mean squared error of 12*10-4. Time-domain sparse sampling achieves considerable data compression while also expediting both the measurement and data processing time, representing a significant stride towards the realm of real-time spectroscop

Multi-octave, CEP-stable source for high-energy field synthesis

The development of high-energy, high-power, multi-octave light transients is currently the subject of intense research driven by emerging applications in attosecond spectroscopy and coherent control. We report on a phase-stable, multi-octave source based on a Yb:YAG amplifier for light transient generation. We demonstrate the amplification of a two-octave spectrum to 25 mu J of energy in two broadband amplification channels and their temporal compression to 6 and 18 fs at 1 and 2 mu m, respectively. In this scheme, due to the intrinsic temporal synchronization between the pump and seed pulses, the temporal jitter is restricted to long-term drift. We show that the intrinsic stability of the synthesizer allows subcycle detection of an electric field at 0.15 PHz. The complex electric field of the 0.15-PHz pulses and their free induction decay after interaction with water molecules are resolved by electro-optic sampling over 2 ps. The scheme is scalable in peak and average power