Few-cycle Laser Pulses Research Articles

Carrier-envelope phase effects on the reflectance of diamond films irradiated by ultrashort single-cycle light pulses: A comparison study in attosecond and femtosecond regimes

Diamond films irradiated with few-cycle laser pulses are emerging as a all-optical information processing device with high-speed and low-power-consumption. The possibility to steer, control or switch such few-cycle laser pulses with diamond films is expected to pave the way towards ultrafast all-optical switching. Here, we show theoretically the effect of the carrier-envelope phase (CEP) of the ultrashort single-cycle light pulses on the reflectance of diamond films within the framework of multi-scale theory. We observe clear variations in the reflectance behavior of femtosecond pulses and attosecond pulses. Our most important finding is that the reflectivity difference of attosecond pulses with different waveforms and the same spectrum on diamond films exhibits a perfect quadratic relationship with the CEP. This observation suggests that the nonlinearity of attosecond pulses is different from that of femtosecond pulses. Analysis of these results allows us to gain new insights in the interaction between attosecond light pulses and matter. This opens fascinating avenues for all-optical information processing over ultrashort lengths and timescales.

Generation of optical-terahertz solitons by a few-cycle laser pulse

The generation of broadband terahertz radiation using an extremely short laser pulse of high intensity is considered. Using numerical simulation of the generalized Yajima-Oikawa system, it is shown that in the generation of an optical-terahertz soliton, in contrast to the quasi-monochromatic case, Kerr nonlinearity plays an important role for a low-period pulse, considering its dispersion.

Unforeseen advantage of looser focusing in vacuum laser acceleration

Acceleration of electrons in vacuum directly by intense laser fields holds great promise for the generation of high-charge, ultrashort, relativistic electron bunches. While the energy gain is expected to be higher with tighter focusing, this does not account for the reduced acceleration range, which is limited by diffraction. Here, we present the results of an experimental investigation that exposed nanotips to relativistic few-cycle laser pulses. We demonstrate the vacuum laser acceleration of electron beams with 100s pC charge and 15 MeV energy. Two different focusing geometries, with normalized vector potential a0 of 9.8 and 3.8, produced comparable overall charge and electron spectra, despite a factor of almost ten difference in peak intensity. Our results are in good agreement with 3D particle-in-cell simulations, which indicate the importance of dephasing.

Efficient laser wakefield accelerator in pump depletion dominated bubble regime.

With the usage of the postcompression technique, few-cycle joule-class laser pulses are nowadays available extending the state of the art of 100 TW-class laser working at 10Hz repetition. In this Letter, we explore the potential of wakefield acceleration when driven with such pulses. The numerical modeling predicts that 50% of the laser pulse energy can be transferred into electrons with energy above 15 MeV, and with charge exceeding several nanocoulombs for the electrons at hundreds of MeV energy. In such a regime, the laser pulse depletes its energy to plasma rapidly driving a strong cavitated wakefield. The self-steepening effect induces a continuous prolongation of a bubble resulting in a massive continuous self-injection that explains the extremely high charge of the beam rending this approach suitable for promoting Bremsstrahlung emitter and generator of tertiary particles, including neutrons released through photonuclear reactions.

Carrier-envelope phase-stabilized ultrashort pulses from a gas-filled multi-pass cell

Few-cycle laser pulses at a high repetition rate with a stable carrier-envelope phase are required for next-generation attosecond time-resolved spectroscopies. One way to generate these pulses is the nonlinear compression of laser pulses via gas-filled hollow-core fibers. Recently, an alternative approach based on multi-pass cells (MPCs) has been shown to be very efficient for post-compression of turn-key, industrial-grade, high average power Yb-doped solid-state laser amplifiers. However, to expand the system for exploring strong-field laser applications, its carrier-envelope phase stability needs to be demonstrated in the compressed pulses. In this Letter, we present the generation of carrier-envelope phase-stabilized 40 fs pulses with 380 μJ energy at 50 kHz by compressing the output of a Yb:KGW amplifier in a gas-filled MPC. Comparable short-term carrier-envelope phase errors of 412 and 435 mrad root mean square were observed from the amplifier and MPC, respectively, indicating that the phase stability of the amplified pulses is well-maintained during pulse compression in the MPC.

Characterization of the polarization state of few-cycle laser pulses using d-scan: D-TURTLE

We characterize the polarization state of few-femtosecond laser pulses by implementing the dispersion scan technique in combination with the tomographic ultrafast retrieval of transverse light E-fields procedure (D-TURTLE). We demonstrate, both numerically and experimentally, that D-TURTLE unambiguously identifies the pulse ellipticity, its handedness and which polarization component travels ahead. Given the robustness of this technique, and its self-referenced and in-line nature, D-TURTLE can be extremely useful to characterize polarized few-cycle laser pulses.

Detangling the quantum tapestry of intrachannel interference in below-threshold nonsequential double ionization with few-cycle laser pulses

We perform a systematic analysis of single-channel quantum interference in laser-induced nonsequential double ionization with few-cycle pulses, using the strong-field approximation. We focus on a below-threshold intensity for which the recollision-excitation with subsequent ionization (RESI) mechanism is prevalent. We derive and classify several analytic interference conditions for single-channel RESI in arbitrary driving fields and address specific issues for few-cycle pulses. Since the cycles in a short pulse are no longer equivalent, there are several events whose dominance varies. We quantify this dominance for single excitation channels by proposing a dominance parameter. Moreover, there will be many types of superimposed interference fringes that must be taken into consideration. We find an intricate tapestry of patterns arising from phase differences related to symmetrization, temporal shifts and a combination of exchange and event interference. Published by the American Physical Society 2024

Gouy phase effects on photocurrents in plasmonic nanogaps driven by single-cycle pulses.

The investigation of optical phenomena in the strong-field regime requires few-cycle laser pulses at field strengths exceeding gigavolts per meter (GV/m). Surprisingly, such conditions can be reached by tightly focusing pJ-level pulses with nearly octave spanning optical bandwidth onto plasmonic nanostructures, exploiting the field-enhancement effect. In this situation, the Gouy phase of the focused beam can deviate significantly from the monochromatic scenario. Here, we study the effect of the Gouy phase of a pulse exploited to drive coherent strong-field photocurrents within a plasmonic gap nanoantenna. While the influence of the specific Gouy phase profile in the experiment approaches the monochromatic case closely, this scheme may be utilized to identify more intricate phase profiles at sub-diffraction scale. Our results pave the way for Gouy phase engineering at picojoule (pJ) pulse energy levels, enabling the optimization of strong-field optical phenomena.

Systematic comparison of commercial devices for temporal characterization of few-cycle laser pulses in the 500-1000 nm spectral range

We compare multiple temporal pulse characterization techniques in three different pulse duration regimes from 15 fs to sub-5 fs, as there are no available standards yet for measuring such ultrashort pulses. To accomplish this, a versatile post-compression platform was developed, where the 100 fs near infrared pulses were post-compressed to the sub-two-cycle regime in a hybrid, three-stage configuration. After each stage, the duration of the compressed pulse was measured with the d-scan, TIPTOE and SRSI techniques and the retrieved temporal intensity profiles, spectrum and spectral phases were compared. Spectral homogeneity was also measured with an imaging spectrometer to understand the input coupling conditions of the temporal measurements. Our findings suggest that the different devices give similar results in terms of temporal intensity profile, however they are extremely sensitive to alignment and to beam quality, especially in the case of the shortest pulses. We address specific steps of measurement procedures, which paves the way towards the standardization of pulse characterization in the near future.

Femtosecond Collisional Dissipation of Vibrating D_{2}^{+} in Helium Nanodroplets.

We explored the collision-induced vibrational decoherence of singly ionized D_{2} molecules inside a helium nanodroplet. By using the pump-probe reaction microscopy with few-cycle laser pulses, we captured in real time the collision-induced ultrafast dissipation of vibrational nuclear wave packet dynamics of D_{2}^{+} ion embedded in the droplet. Because of the strong coupling of excited molecular cations with the surrounding solvent, the vibrational coherence of D_{2}^{+} in the droplet interior only lasts for a few vibrational periods and completely collapses within 140fs. The observed ultrafast coherence loss is distinct from that of isolated D_{2}^{+} in the gas phase, where the vibrational coherence persists for a long time with periodic quantum revivals. Our findings underscore the crucial role of ultrafast collisional dissipation in shaping the molecular decoherence and solvation dynamics during solution chemical reactions, particularly when the solute molecules are predominantly in ionic states.

Loss-free shaping of few-cycle terawatt laser pulses.

We demonstrate loss-free generation of 3 mJ, 1 kHz, few-cycle (5 fs at 750 nm central wavelength) double pulses with a pulse peak separation from 10 to 100 fs, using a helium-filled hollow core fiber (HCF) and chirped mirror compressor. Crucial to our scheme are simulation-based modifications to the spectral phase and amplitude of the oscillator seed pulse to eliminate the deleterious effects of self-focusing and nonlinear phase pickup in the chirped pulse amplifier. The shortest pulse separations are enabled by tunable nonlinear pulse splitting in the HCF compressor.

Spatiotemporal dispersion compensation for a 200-THz noncollinear optical parametric amplifier.

A noncollinear optical parametric amplifier (NOPA) can produce few-cycle femtosecond laser pulses that are ideally suited for time-resolved optical spectroscopy measurements. However, the nonlinear-optical process giving rise to ultrabroadband pulses is susceptible to spatiotemporal dispersion problems. Here, we detail refinements, including chirped-pulse amplification (CPA) and pulse-front matching (PFM), that minimize spatiotemporal dispersion and thereby improve the properties of ultrabroadband pulses produced by a NOPA. The description includes a rationale behind the choices of optical and optomechanical components, as well as assessment protocols. We demonstrate these techniques using a 1kHz, second-harmonic Ti:sapphire pump configuration, which produces ∼5-fs duration pulses that span from about 500 to 800nm with a bandwidth of about 200THz. To demonstrate the utility of the CPA-PFM-NOPA, we measure vibrational quantum beats in the transient-absorption spectrum of methylene blue, a dye molecule that serves as a reference standard.

Field-free orientation of 7LiH steered by a few-cycle nonlinearly chirped pulse

We demonstrate theoretically that an efficient field-free molecular orientation of 7LiH molecule steered by a few-cycle nonlinearly chirped laser pulse with frequency in the terahertz regime can be achieved. The frequency modulation parameter β plays an important role in the molecular orientation, the maximum molecular orientation |〈cosθ〉|max is 0.848 and the orientation duration is 150 fs when β=7.25. In the range of electric-field peak intensity E0=[0.1,4.0] MV/cm, we can find the maximum orientation degree in both positive and negative directions. Compared to the scheme steered by a normal laser pulse, we can find that a more efficient molecular orientation and a smaller difference in population between the adjacent states can be realized by using the nonlinearly chirped laser pulse under the same near-single-period conditions. In addition, at the same temperature, a higher molecular orientation and a smaller decrease rate of orientation with temperature can be obtained by the nonlinearly chirped laser pulse.

Control of the spider-like interference structure in photoelectron momentum distributions of a helium atom in a few-cycle nonlinear chirped laser pulse.

We investigate theoretically the photoelectron momentum distributions (PMDs) of the helium atom in the few-cycle nonlinear chirped laser pulse. The numerical results show that the direction of the spider-like interference structure in PMDs exhibits periodic variations with the increase of the chirp parameter. It is illustrated that the direction of the spider-like interference structure is related to the direction of the electron motion by tracking the trajectories of the electrons. We also demonstrate that the carrier-envelope phase can precisely control the opening of the ionization channel. In addition, we investigate the PMDs when a chirp-free second harmonic (SH) laser pulse is added to the chirped laser field, the numerical results show that the interference patterns can change from only spider-like interference structure to both spider-like and ring-like interference structures.

Few-cycle laser pulse characterization on-target using high-harmonic generation from nano-scale solids.

We demonstrate high-harmonic generation for the time-domain observation of the electric field (HHG-TOE) and use it to measure the waveform of ultrashort mid-infrared (MIR) laser pulses interacting with ZnO thin-films or WS2 monolayers. The working principle relies on perturbing HHG in solids with a weak replica of the pump pulse. We measure the duration of few-cycle pulses at 3200 nm, in reasonable agreement with the results of established pulse characterization techniques. Our method provides a straightforward approach to accurately characterize femtosecond laser pulses used for HHG experiments right at the point of interaction.

Time-resolved subcycle and intercycle interference influenced momentum shift in nonadiabatic tunnelling ionization

Momentum shift is an important sign of nonadiabatic tunnelling ionization process. To investigate the mechanism of momentum shift, we use the strong-field approximation theory to track the formation of ionization momentum spectra of hydrogen atom under the action of different laser pulses in the time domain. By observing the ionization momentum spectra of different structures over time, we find that the momentum shift is formed by the continuous interference and evolution of ionization signals. Meanwhile, we further analyze how subcycle and intercycle interference influence the formation of momentum shift. Before the duration is long enough for intercycle interference to emerge, momentum shift grows smoothly. Our findings reveal different intrinsic mechanisms for the formation of momentum shift in many-cycle and few-cycle laser pulses, showing that subcycle interference plays a dominant role in the former while intercycle interference is critical in the latter. This work lays the foundation for a deeper understanding of the nonadiabatic tunnelling process and makes the regulation of momentum shift possible.

Application of Electro-Optic Sampling Detection Technology Based on BBO Crystals in Detecting Near-Infrared Few-Cycle Laser Pulses

Application of Electro-Optic Sampling Detection Technology Based on BBO Crystals in Detecting Near-Infrared Few-Cycle Laser Pulses

Refining the Performance of mid-IR CPA Laser Systems Based on Fe-Doped Chalcogenides for Nonlinear Photonics

The chirped pulse amplification (CPA) systems based on transition-metal-ion-doped chalcogenide crystals are promising powerful ultrafast laser sources providing access to sub-TW laser pulses in the mid-IR region, which are highly relevant for essential scientific and technological tasks, including high-field physics and attosecond science. The only way to obtain high-peak power few-cycle pulses is through efficient laser amplification, maintaining the gain bandwidth ultrabroad. In this paper, we report on the approaches for mid-IR broadband laser pulse energy scaling and the broadening of the gain bandwidth of iron-doped chalcogenide crystals. The multi-pass chirped pulse amplification in the Fe:ZnSe crystal with 100 mJ level nanosecond optical pumping provided more than 10 mJ of output energy at 4.6 μm. The broadband amplification in the Fe:ZnS crystal in the vicinity of 3.7 μm supports a gain band of more than 300 nm (FWHM). Spectral synthesis combining Fe:ZnSe and Fe:CdSe gain media allows the increase in the gain band (~500 nm (FWHM)) compared to using a single active element, thus opening the route to direct few-cycle laser pulse generation in the prospective mid-IR spectral range. The features of the nonlinear response of carbon nanotubes in the mid-IR range are investigated, including photoinduced absorption under 4.6 μm excitation. The study intends to expand the capabilities and improve the output characteristics of high-power mid-IR laser systems.

Twin-Capture Rydberg State Excitation Enhanced with Few-Cycle Laser Pulses

Quantum excitation is usually regarded as a transient process occurring instantaneously, leaving the underlying physics shrouded in mystery. Recent research shows that Rydberg-state excitation with ultrashort laser pulses can be investigated and manipulated with state-of-the-art few-cycle pulses. We theoretically find that the efficiency of Rydberg state excitation can be enhanced with a short laser pulse and modulated by varying the laser intensities. We also uncover new facets of the excitation dynamics, including the launching of an electron wave packet through strong-field ionization, the re-entry of the electron into the atomic potential and the crucial step where the electron makes a U-turn, resulting in twin captures into Rydberg orbitals. By tuning the laser intensity, we show that the excitation of the Rydberg state can be coherently controlled on a sub-optical-cycle timescale. Our work paves the way toward ultrafast control and coherent manipulation of Rydberg states, thus benefiting Rydberg-state-based quantum technology.

High-harmonic generation in liquids with few-cycle pulses: effect of laser-pulse duration on the cut-off energy.

High-harmonic generation (HHG) in liquids is opening new opportunities for attosecond light sources and attosecond time-resolved studies of dynamics in the liquid phase. In gas-phase HHG, few-cycle pulses are routinely used to create isolated attosecond pulses and to extend the cut-off energy. Here, we study the properties of HHG in liquids, including heavy water, ethanol and isopropanol, by continuously tuning the pulse duration of a mid-infrared driver from the multi- to the two-cycle regime. Similar to the gas phase, we observe the transition from discrete odd-order harmonics to continuous extreme-ultraviolet emission. However, the cut-off energy is shown to be entirely independent of the pulse duration. These observations are confirmed by ab-initio simulations of HHG in large liquid clusters. Our results support the notion that the cut-off energy is a fundamental property of the liquid, independent of the driving-pulse properties. Our work implies that few-cycle mid-infrared laser pulses are suitable drivers for generating isolated attosecond pulses from liquids and confirm the capability of high-harmonic spectroscopy to determine the mean-free paths of slow electrons in liquids.