Phillip D. Keathley

High-energy, phase-stable, ultrabroadband kHz OPCPA at 2.1 μm pumped by a picosecond cryogenic Yb:YAG laser

We report on a kHz, mJ-level, carrier-envelope phase (CEP)-stable ultrabroadband optical parametric chirped-pulse amplifier (OPCPA) at 2.1-μm wavelength, pumped by a high-energy, 14 ps, cryogenic Yb:YAG pump laser, and its application to high-order harmonic generation (HHG) with Xe. The pre-amplifier chain is pumped by a 12-ps Nd:YLF pump laser and both pump lasers are optically synchronized to the signal pulse of the OPCPA. An amplified pulse energy of 0.85 mJ was obtained at the final OPCPA stage with good beam profile. The pulse is compressed to 4.5 optical cycles (<32 fs) with a spectral bandwidth of 474 nm supporting 3.5 optical cycles. The CEP stability was measured to be 194 mrad and the super-fluorescence noise is estimated to be ~9%. First HHG results are demonstrated with Xe showing significant cutoff extension to >85 eV with an efficiency of ~10-10 per harmonic, limited by the maximum gas pressure and flow into the chamber. This demonstrates the potential of this 2.1-μm source for scaling of photon energy and flux in the water-window range when applied to Ne and He at kHz repetition rate.

Nanostructured Ultrafast Silicon-Tip Optical Field-Emitter Arrays

Femtosecond ultrabright electron sources with spatially structured emission are an enabling technology for free-electron lasers, compact coherent X-ray sources, electron diffractive imaging, and attosecond science. In this work, we report the design, modeling, fabrication, and experimental characterization of a novel ultrafast optical field emission cathode comprised of a large (>100,000 tips), dense (4.6 million tips·cm(-2)), and highly uniform (<1 nm tip radius deviation) array of nanosharp high-aspect-ratio silicon columns. Such field emitters offer an attractive alternative to UV photocathodes while providing a direct means of structuring the emitted electron beam. Detailed measurements and simulations show pC electron bunches can be generated in the multiphoton and tunneling regime within a single optical cycle, enabling significant advances in electron diffractive imaging and coherent X-ray sources on a subfemtosecond time scale, not possible before. At high charge emission yields, a slow rollover in charge is explained as a combination of the onset of tunneling emission and the formation of a virtual cathode.

Toward a terahertz-driven electron gun

Femtosecond electron bunches with keV energies and eV energy spread are needed by condensed matter physicists to resolve state transitions in carbon nanotubes, molecular structures, organic salts, and charge density wave materials. These semirelativistic electron sources are not only of interest for ultrafast electron diffraction, but also for electron energy-loss spectroscopy and as a seed for x-ray FELs. Thus far, the output energy spread (hence pulse duration) of ultrafast electron guns has been limited by the achievable electric field at the surface of the emitter, which is 10 MV/m for DC guns and 200 MV/m for RF guns. A single-cycle THz electron gun provides a unique opportunity to not only achieve GV/m surface electric fields but also with relatively low THz pulse energies, since a single-cycle transform-limited waveform is the most efficient way to achieve intense electric fields. Here, electron bunches of 50 fC from a flat copper photocathode are accelerated from rest to tens of eV by a microjoule THz pulse with peak electric field of 72 MV/m at 1 kHz repetition rate. We show that scaling to the readily-available GV/m THz field regime would translate to monoenergetic electron beams of ~100 keV.

High-energy, kHz, picosecond hybrid Yb-doped chirped-pulse amplifier.

We report on a diode-pumped, hybrid Yb-doped chirped-pulse amplification (CPA) laser system with a compact pulse stretcher and compressor, consisting of Yb-doped fiber preamplifiers, a room-temperature Yb:KYW regenerative amplifier (RGA), and cryogenic Yb:YAG multi-pass amplifiers. The RGA provides a relatively broad amplification bandwidth and thereby a long pulse duration to mitigate B-integral in the CPA chain. The ~1030-nm laser pulses are amplified up to 70 mJ at 1-kHz repetition rate, currently limited by available optics apertures, and then compressed to ~6 ps with high efficiency. The near-diffraction-limited beam focusing quality is demonstrated with M(x)(2) = 1.1 and M(y)(2) = 1.2. The shot-to-shot energy fluctuation is as low as ~1% (rms), and the long-term energy drift and beam pointing stability for over 8 hours measurement are ~3.5% and <6 μrad (rms), respectively. To the best of our knowledge, this hybrid laser system produces the most energetic picosecond pulses at kHz repetition rates among rod-type laser amplifiers. With an optically synchronized Ti:sapphire seed laser, it provides a versatile platform optimized for pumping optical parametric chirped-pulse amplification systems as well as driving inverse Compton scattered X-rays.

High-density Au nanorod optical field-emitter arrays

We demonstrate the design, fabrication, characterization, and operation of high-density arrays of Au nanorod electron emitters, fabricated by high-resolution electron beam lithography, and excited by ultrafast femtosecond near-infrared radiation. Electron emission characteristic of multiphoton absorption has been observed at low laser fluence, as indicated by the power-law scaling of emission current with applied optical power. The onset of space-charge-limited current and strong optical field emission has been investigated so as to determine the mechanism of electron emission at high incident laser fluence. Laser-induced structural damage has been observed at applied optical fields above 5 GV m(-1), and energy spectra of emitted electrons have been measured using an electron time-of-flight spectrometer.

Direct longitudinal laser acceleration of electrons in free space

Compact laser-driven accelerators are versatile and powerful tools of unarguable relevance on societal grounds for the diverse purposes of science, health, security, and technology because they bring enormous practicality to state-of-the-art achievements of conventional radio-frequency accelerators. Current benchmarking laser-based technologies rely on a medium to assist the light-matter interaction, which impose material limitations or strongly inhomogeneous fields. The advent of few cycle ultra-intense radially polarized lasers has materialized an extensively studied novel accelerator that adopts the simplest form of laser acceleration and is unique in requiring no medium to achieve strong longitudinal energy transfer directly from laser to particle. Here we present the first observation of direct longitudinal laser acceleration of non-relativistic electrons that undergo highly-directional multi-GeV/m accelerating gradients. This demonstration opens a new frontier for direct laser-driven particle acceleration capable of creating well collimated and relativistic attosecond electron bunches and x-ray pulses.

Water-window soft x-ray high-harmonic generation up to the nitrogen K-edge driven by a kHz, 2.1 mu m OPCPA source

We report the generation of coherent water-window soft x-ray harmonics in a neon-filled semi-infinite gas cell driven by a femtosecond multi-mJ mid-infrared optical parametric chirped-pulse amplification (OPCPA) system at a 1 kHz repetition rate. The cutoff energy was extended to ~450 eV with a 2.1 μm driver wavelength and a photon flux of photons/s/1% bandwidth was obtained at 350 eV. A comparable photon flux of photons/s/1% bandwidth was observed at the nitrogen K-edge of 410 eV. This is the first demonstration of water-window harmonic generation up to the nitrogen K-edge from a kHz OPCPA system. Finally, this system is suitable for time-resolved soft x-ray near-edge absorption spectroscopy. Further scaling of the driving pulses energy and repetition rate is feasible due to the availability of high-power picosecond Yb-doped pump laser technologies, thereby enabling ultrafast, tabletop water-window x-ray imaging.

Cut-off scaling of high-harmonic generation driven by a femtosecond visible optical parametric amplifier

We studied high-harmonic generation (HHG) in Ar, Ne and He gas jets using a broadly tunable, high-energy optical parametric amplifier (OPA) in the visible wavelength range. We optimized the noncollinear OPA to deliver tunable, femtosecond pulses with 200–500 μJ energy at the 1 kHz repetition rate with excellent spatiotemporal properties, suitable for HHG experiments. By tuning the central wavelength of the OPA while keeping other parameters (energy, duration and beam size) constant, we experimentally studied the scaling law of cut-off energy with the driver wavelength in helium. Our measurements show a λ 1.7 + 0.2 dependence of the HHG cut-off photon energy over the full visible range in agreement with previous experiments of near- and mid-IR wavelengths. By tuning the central wavelength of the driver source, the high-order harmonic spectra in the extreme ultraviolet cover the full range of photon energy between ∼25 and ∼100 eV. Due to the high coherence intrinsic in HHG, as well as the broad and continuous tunability in the extreme UV range, a high energy, high repetition rate version of this source might be an ideal seed for free electron lasers. (Some figures may appear in colour only in the online journal)

Multi-mJ mid-infrared kHz OPCPA and Yb-doped pump lasers for tabletop coherent soft x-ray generation

We present our recent progress on the development of a mid-infrared (mid-IR), multi-mJ, kHz optical parametric chirped-pulse amplification (OPCPA) system, pumped by a homebuilt picosecond cryogenic Yb:YAG chirped-pulse amplifier, and its application to soft x-ray high-order harmonic generation. The cryogenic Yb:YAG laser operating at 1 kHz repetition rate delivers 42 mJ, 17 ps, 1.03 μm pulses to pump the OPCPA system. Efficient second and fourth harmonic generations from the Yb:YAG system are demonstrated, which provide the pumping capability for OPCPA at various wavelengths. The mid-IR OPCPA system produces 2.6 mJ, 39 fs, 2.1 μm pulses with good beam quality (M 2 = ~1.5) at 1 kHz repetition rate. The output pulses of the OPCPA are used to generate high-order harmonics in both gas cell and hollow-core fiber targets. A photon flux of ~2 × 108 photon/s/1% bandwidth at 160 eV in Ar is measured while the cutoff is 190 eV. The direct measurements of the photon flux from x-ray photodiodes have confirmed the generation of water-window soft x-ray photons with a flux ~106 photon/s/1% bandwidth at 330 eV in Ne. The demonstrated OPCPA and Yb:YAG pump laser technologies provide an excellent platform of energy and power scalable few-cycle mid-IR sources that are suitable for high-flux tabletop coherent soft x-ray generation.

Nanostructured silicon photo-cathodes for x-ray generation

We report the fabrication and characterization of ultrafast laser triggered nanostructured silicon photo-cathodes for x-ray generation via inverse Compton scattering. A highly uniform array of ~2200 silicon pillars with 5 μm array pitch, where each pillar is capped by a nanosharp tip, shows stable current emission using 35 fs, 800 nm laser pulses. The cathodes can emit at 3.6 nA average current over 8-million 1.2 pC electron bunches when excited with 9.5 μJ laser pulses with no degradation of the emission characteristic of the cathode, showing that silicon-based photon-triggered cathodes processed with standard CMOS processes and operated at high vacuum can function for extended periods without performance degradation.