Ultrafast plasmonic photoemission in the single-cycle and few-cycle regimes.

Due to the highly increased interest in the development of state-of-the-art applications of photoemission in ultrafast electron microscopy, development of photocathodes and many more applications, a correct theoretical understanding of the underlying phenomena is needed. Within the framework of the single active electron approximation the most accurate results can be obtained by the direct solution of the time-dependent Schrödinger equation (TDSE). In this work, after a brief presentation of a numerically improved version of a mixed 1D-TDSE method, we investigated the characteristics of electron spectra obtained from the surface of metal nanoparticles irradiated with ultrashort laser pulses. During our investigation different decay lengths of the plasmonic-enhanced incident field in the vicinity of the metal were considered. Using the simulated spectra we managed to identify the behavior of the cutoff energy as a function of decay length in the strong-field, multiphoton and transition regimes.

Attosecond pulse generation with an optimization loop in a light-field-synthesizer.

We developed an efficient, tailored optimization method for attopulse generation using a light-field-synthesizer [M. Hassan et al., Nature 530, 66 (2016)]. We adapted genetic optimization of single-cycle and sub-cycle waveforms to attosecond pulse generation and achieved significantly improved convergence to many target attosecond pulse shapes. Importantly, we show that the single-atom approach (based on strong field approximation) gives similar results to the more complex and numerically intensive 3D model of the attopulse generation process and that spectrally tunable attosecond pulses can be produced with a light-field synthesizer.

Direct comparison of kilohertz- and megahertz-repetition-rate femtosecond damage threshold.

We performed femtosecond laser-induced damage threshold (fs LIDT) measurements with substantially different repetition rate Ti:sapphire laser systems: a 1 kHz regenerative amplifier and a 4.3 MHz long-cavity oscillator. All other pulse parameters are kept the same. Comparative measurements of a dielectric high reflector, a chirped mirror, and metallic mirrors show at least a factor of 2.7 lower fs LIDT at megahertz repetition rates. We attribute this to thermally assisted damage mechanisms supported by complex heat transfer simulations.

Strong-field plasmonic photoemission in the mid-IR at <1†GW/cm² intensity.

We investigated nonlinear photoemission from plasmonic films with femtosecond, mid-infrared pulses at 3.1 µm wavelength. Transition between regimes of multi-photon-induced and tunneling emission is demonstrated at an unprecedentedly low intensity of <1 GW/cm(2). Thereby, strong-field nanophysics can be accessed at extremely low intensities by exploiting nanoscale plasmonic field confinement, enhancement and ponderomotive wavelength scaling at the same time. Results agree well with quantum mechanical modelling. Our scheme demonstrates an alternative paradigm and regime in strong-field physics.

Observation of few-cycle, strong-field phenomena in surface plasmon fields.

We present experimental evidence of the generation of few-cycle propagating surface plasmon polariton wavepackets. These ultrashort plasmonic pulses comprised of only 2-3 field oscillations were characterized by an autocorrelation measurement based on electron photoemission. By exploiting plasmonic field enhancement, we achieved plasmon-induced tunnelling emission from the metal surface at low laser intensity, opening perspectives for strong-field experiments with low pulse energies. All-optical electron acceleration up to keV kinetic energy is also demonstrated in these surface-confined, few-cycle fields with only 1.35×10(12) W/cm2 focused laser intensity. The experimental results are found to be in excellent agreement with the model.

Scalable Yb-MOPA-driven carrier-envelope phase-stable few-cycle parametric amplifier at 1.5 microm.

Carrier-envelope phase-stable 4 microJ pulses at approximately 1.5 microm are obtained from a femtosecond Yb:KGW-MOPA-pumped two-stage optical parametric amplifier. This novel technology represents a highly attractive alternative to traditional Ti:sapphire front-ends for seeding multimillijoule-level optical parametric chirped-pulse amplifiers. For this task, we demonstrate stretching of the OPA output to approximately 40 ps and recompression to 33 fs pulse duration. As a stand-alone system, our tunable two-stage OPA might find numerous applications in time-resolved spectroscopy and micromachining.

Nonlinear processes induced by the enhanced, evanescent field of surface plasmons excited by femtosecond laser pulses.

Evanescent fields of surface plasmon polaritons (SPP) above metal surfaces can reach 1-2 orders of magnitude higher, nearly atomic field strengths in comparison to the relatively weak exciting laser fields of a femtosecond Ti:sapphire laser oscillator. We used these high plasmonic fields to study the characteristic SPP phenomena of intense field optics experimentally. It was found that both the intensity and the angular distribution of SPP emitted light depend nonlinearly on the exciting laser intensity in the higher-intensity, non-perturbative range of the interactions. These results are supported by our theory. At these strong excitations, an additional, depolarized, diffuse spectrum also appeared which can be attributed either to the fluorescence of Au, or to the non-equlibrium Planck radiation, originating from the fast cooling of the conduction electron cloud of Au excited by the femtosecond laser pulse.

Solitonic dynamics of ultrashort pulses in a highly nonlinear photonic-crystal fiber visualized by spectral interferometry.

A linear technique of phase measurement based on spectral interferometry is employed to visualize the fine details in the spectral phase of a soliton produced in a highly nonlinear photonic crystal fiber (PCF) with a resolution better than 0.1 nm. Gigahertz features have been resolved in the spectral phase of the soliton PCF output, allowing the accuracy of time-domain soliton envelope reconstruction to be improved on the timescale of a few femtoseconds.

Influence of the carrier-envelope phase of few-cycle pulses on ponderomotive surface-plasmon electron acceleration.

Control over basic processes through the electric field of a light wave can lead to new knowledge of fundamental light-matter interaction phenomena. We demonstrate, for the first time, that surface-plasmon (SP) electron acceleration can be coherently controlled through the carrier-envelope phase (CEP) of an excitation optical pulse. Analysis indicates that the physical origin of the CEP sensitivity arises from the electron's ponderomotive interaction with the oscillating electromagnetic field of the SP wave. The ponderomotive electron acceleration mechanism provides sensitive (nJ energies), high-contrast, single-shot CEP measurement capability of few-cycle laser pulses.

Pulse compression with time-domain optimized chirped mirrors.

Dispersive optical interference coatings (chirped mirrors - CMs) are designed by computer optimization of an analytically calculated initial multilayer. Traditionally, the relevant properties of the CM (reflectance and the frequency-dependence of the phase shift upon reflection) are optimized to match frequency-domain targets. We propose a novel target function that quantifies directly the capability of a multilayer to control the temporal shape of the reflected optical pulse. Employing this time-domain analysis/optimization one can design dispersive multilayers having air as medium of incidence and supporting the generation of pulses with durations in the sub-5-fs-range, as demonstrated in a proof-of-principle compression experiment.

Observation of light-phase-sensitive photoemission from a metal.

We demonstrate that multiphoton-induced photoelectron emission from a gold surface caused by low-energy (unamplified) 4-fs, 750-nm laser pulses is sensitive to the timing of electric field oscillations with respect to the pulse peak. This observation confirms recent theoretical predictions and opens the door to measuring the absolute value of the carrier-envelope phase difference of few-cycle light pulses with a solid-state detector.

Efficient generation of large diffraction gratings with a grating interferometer.

The advantages of a grating interferometer for the generation of large diffraction gratings are demonstrated. In a one- and a two-stage process, high-quality gratings of 120 and 200 mm, respectively, were made with optics no larger than 50 mm together with an argon-ion laser with no line narrowing or beam stabilization and a rotating diffuser for improved beam uniformity.