Propagation-assisted generation of intense few-femtosecond high-harmonic pulses
B. Major, M. Kretschmar, O. Ghafur, A. Hoffmann, K. Kovács, K. Varjú, B. Senfftleben, J. Tümmler, I. Will, T. Nagy, D. Rupp, M. J. J. Vrakking, V. Tosa, B. Schütte
The ongoing development of intense high-harmonic generation (HHG) sources has recently enabled highly nonlinear ionization of atoms by the absorption of at least 10 extreme-ultraviolet (XUV) photons within a single atom [Senfftleben \textit{et al.}, arXiv1911.01375]. Here we investigate the role that reshaping of the fundamental, few-cycle, near-infrared (NIR) driving laser within the 30-cm-long HHG Xe medium plays in the generation of the intense HHG pulses. Using an incident NIR intensity that is higher than what is required for phase-matched HHG, signatures of reshaping are found by measuring the NIR blueshift and the fluorescence from the HHG medium along the propagation axis. These results are well reproduced by numerical calculations that show temporal compression of the NIR pulses in the HHG medium. The simulations predict that after refocusing an XUV beam waist radius of 320 nm and a clean attosecond pulse train can be obtained in the focal plane, with an estimated XUV peak intensity of 9x10^15 W/cm^2. Our results show that XUV intensities that were previously only available at large-scale facilities can now be obtained using moderately powerful table-top light sources.
We report on the generation of intense extreme ultraviolet (EUV) supercontinuum with photon energies spanning from 35 eV to 50 eV (i. e., supporting an isolated attosecond pulse with a duration of ~271 as) by loosely focusing 35 fs, 11 mJ pulses from a femtosecond laser amplifier into a 10-mm long gas cell filled with krypton gas. The dramatic change of spectral and temporal properties of the driver pulses after passing through the gas cell indicates that propagation effects play a significant role in promoting the generation of the EUV supercontinuum.
We report on generation of a rotational wavepacket in the ground vibronic state (v = 0) of excited electronic B2Σu+ state of N2+ in a femtosecond laser induced plasma spark. Decoding of the rotational wavepacket is achieved with the frequency-resolved seed-amplified air laser spectrum resulting from the population inversion between the B2Σu+-X2Σg+ states of N2+ in the plasma. We also observe that the rotational wave-packet leads to modulation of the amplified seed signals in the time domain using a pump-probe scheme, which can be well reproduced by theoretical calculation. Our results demonstr…
We investigate the self-phase modulation of intense femtosecond laser pulses propagating in an ionizing gas and its effects on collective properties of high-order harmonics generated in the medium. Plasmas produced in the medium are shown to induce a positive frequency chirp on the leading edge of the propagating laser pulse, which subsequently drives high harmonics to become positively chirped. In certain parameter regimes, the plasma-induced positive chirp can help to generate sharply peaked high harmonics, by compensating for the dynamically-induced negative chirp that is caused by the stee…
We present the generation of high order harmonics in crystalline silicon subjected to intense near-infrared 30fs laser pulse. The harmonic spectrum extends from the near infrared to the extreme ultraviolet spectral region. Depending on the pulsed laser intensity, we distinguish two regimes of harmonic generation: (i) perturbative regime: electron-hole pairs born during each half-cycle of the laser pulse via multiphoton and tunnel transitions are accelerated in the laser electric field and gain kinetic energy; the electron-hole pairs then recombine in the ground state by emitting a single high-…
Synchronising ultra-short (~fs) and focussed laser pulses is a particularly difficult task, as this timescale lies orders of magnitude below the typical range of fast electronic devices. Here we present an optical technique that allows for femtosecond-scale synchronisation of the focal planes of two focussed laser pulses. This technique is virtually applicable to any focussing geometry and relative intensity of the two lasers. Experimental implementation of this technique provides excellent quantitative agreement with theoretical expectations. The proposed technique will prove highly beneficia…
We investigate the prospects of creating broad rotational wave packets by means of molecular interaction with long sequences of intense femtosecond pulses. Using state-resolved rotational Raman spectroscopy of oxygen, subject to a sequence of more than 20 laser pulses with peak intensities exceeding $10^{13}$ W/cm$^{2}$ per pulse, we show that the centrifugal distortion is the main obstacle on the way to reaching high rotational states. We demonstrate that the timing of the pulses can be optimized to partially mitigate the centrifugal limit. The cumulative effect of a long pulse sequence resul…
We present the effect of a nanostructured surface on the emission of ions and electrons from intense (5-36 Petwatt per sq.cm) femtosecond laser produced plasmas. Electrons from optically polished copper targets coated with copper nanoparticles (CuNP) are observed to be hotter than those from uncoated polished targets. A nearly two-fold enhancement is observed for ions in the range 14-74 keV, while ion yield decreases by a factor of 2 in the 74-2000 keV range. The total ion yields measured using a large area Faraday cup are more from CuNP targets than those from polished Cu targets, indicating …
The effect of femtosecond laser irradiation on bulk and single-layer MoS2 on silicon oxide is studied. Optical, Field Emission Scanning Electron Microscopy (FESEM) and Raman microscopies were used to quantify the damage. The intensity of A1g and E2g1 vibrational modes was recorded as a function of the number of irradiation pulses. The observed behavior was attributed to laser-induced bond breaking and subsequent atoms removal due to electronic excitations. The single-pulse optical damage threshold was determined for the monolayer and bulk under 800nm and 1030nm pulsed laser irradiation and the…
We report fabrication of a multifunctional photonic integrated chip on lithium niobate on insulate (LNOI), which is achieved by femtosecond laser assisted chemo-mechanical polish. We demonstrate a high extinction ratio beam splitter, a 1 * 6 optical switch, and a balanced 3 * 3 interferometer on the fabricated chip by reconfiguring the microelectrode array integrated with the multifunctional photonic circuit.
We demonstrate integrating a high quality factor lithium niobate microdisk resonator with a free-standing membrane waveguide. Our technique is based on femtosecond laser direct writing which produces the pre-structure, followed by focused ion beam milling which reduces the surface roughness of sidewall of the fabricated structure to nanometer scale. Efficient light coupling between the integrated waveguide and microdisk was achieved, and the quality factor of the microresonator was measured as high as 1.67*10^5.
Nanosphere-on-mirror plasmonic antennas, each having a monolayer graphene or MoS2 sheet in the gap, were pumped with a femtosecond laser. Abrupt turnings in the scattering linewidth and peak intensity trends as the laser power changed were experimentally observed. Theoretical modelling of dynamic plasmon evolvement attributes the turning to transitioning between two plasmon states, with a universal switching threshold of four-wave mixing efficiency around 0.14%. This bistability is rendered by a strong feedback from the nonlinear gap current to the gap plasmons, and involvement of both four an…
We experimentally investigate the generation of above-threshold harmonics completely from argon atoms on an excited state using mid-infrared femtosecond laser pulses. The highly nonlinear dependences of the observed signal on the pulse energy and polarization of the driver laser pulses indicate its non-perturbative characteristic.
Bright Ar K-shell x-ray with very little background has been generated using an Ar clustering gas jet target irradiated with an 800 mJ, 30 fs ultra-high contrast laser, with the measured flux of 1.1 x 10^4 photons/mrad^2/pulse. This intense x-ray source critically depends on the laser contrast and the laser energy and the optimization of this source with interaction is addressed. Electron driven by laser electric field directly via nonlinear resonant is proved in simulation, resulting in effective electron heating and the enhancement of x-ray emission. The x-ray pulse duration is demonstrated …
We experimentally investigate generation of backward 357 nm N2 laser in a gas mixture of N2/Ar using 800-nm femtosecond laser pulses, and examine the involved gain dynamics based on pump-probe measurements. Our findings show that a minimum lifetime of population inversion in the excited N2 molecules is required for generating intense backward nitrogen lasers, which is ~0.8 ns under our experimental conditions. The results shed new light on the mechanism for generating intense backward lasers from ambient air, which are highly in demand for high sensitivity remote atmospheric sensing applicatio…
Ultra-intense laser-matter interaction experiments (>10$^{18}$ W/cm$^{2}$) with dense targets are highly sensitive to the effect of laser "noise" (in the form of pre-pulses) preceding the main ultra-intense pulse. These system-dependent pre-pulses in the nanosecond and/or picosecond regimes are often intense enough to modify the target significantly by ionizing and forming a plasma layer in front of the target. Time resolved interferometry offers a robust way to characterize the expanding plasma during this period. We have developed a novel pump-probe interferometry system for an ultra-intense…
We report a novel scheme to generate laser-induced, ultrafast, intense (Tesla scale), spatially isolated, magnetic fields. Three-dimensional particle-in-cell simulations show that a femtosecond azimuthally-polarized infrared vector beam, aimed to a conducting circular aperture, produces an intense axially polarized tip-shaped femtosecond magnetic field, extending over micrometer distances and being isolated from the electric field. Our results are backed-up by an analytic model, demonstrating the underlying physics and guiding for optimal parameters. In particular, we find the conditions under…
Irradiating solids with ultrashort laser pulses is known to initiate femtosecond timescale magnetization dynamics. However, sub-femtosecond spin dynamics have not yet been observed or predicted. Here, we explore ultrafast light-driven spin dynamics in a highly non-resonant strong-field regime. Through state-of-the-art ab-initio calculations, we predict that a non-magnetic material can be transiently transformed into a magnetic one via dynamical extremely nonlinear spin-flipping processes, which occur on attosecond timescales and are mediated by a combination of multi-photon and spin-orbit inte…
We experimentally demonstrate the use of subwavelength optical nanoantennae to assist the gentle ablation of nanostructures directly using ultralow fluence from a Ti: sapphire oscillator through the excitation of surface plasmon waves. We show that this ablation mechanism is the same for metal and dielectric. The analytical solutions of ablation threshold are in excellent agreement with the experiment estimations. Surface plasmon assisted locally enhanced ablation at nanoscale provides a method for nanomachining, manipulation and modification the nanostructures without collateral thermal damag…
We report experiments on the generation of third and fifth harmonics of millijoule-level, tightly focused, femtosecond laser pulses at 2.2 μm wavelength in air. The measured ratio of yields of the third and fifth harmonics in our setup is about 2 \cdot 10-4. This result contradicts the recent suggestion that the Kerr effect in air saturates and changes sign in ultra-intense optical fields.
We propose a feedback-assisted direct laser writing method to perform laser ablation of fiber optics devices in which their light-collection signal is used to optimize their properties. A femtosecond-pulsed laser beam is used to ablate a metal coating deposited around a tapered optical fiber, employed to show the suitability of the approach to pattern devices with small radius of curvature. During processing, the same pulses generate two-photon fluorescence in the surrounding environment and the signal is monitored to identify different patterning regimes over time through spectral analysis. T…
Femtosecond laser ablation has been demonstrated to be a versatile tool to produce micro/nanoscale features with high precision and accuracy. However, the use of high laser fluence to increase the ablation efficiency usually results in unwanted effects, such as redeposition of debris, formation of recast layer and heat-affected zone in or around the ablation craters. Here we circumvent this limitation by exploiting a thin frost layer with a thickness of tens of microns, which can be directly formed by the condensation of water vapor from the air onto the exposed surface whose temperature is be…
Monitoring of nanoplasmonics-assisted deuterium production in a polymer seeded with resonant Au nanorods using in situ femtosecond laser induced breakdown spectroscopy
We report on the generation of broadband, high-energy femtosecond pulses centered at 1.28 um by stimulated Raman scattering in pressurized hydrogen cell. Stimulated Raman scattering is performed by two chirped and delayed pulses originating from a multi-mJ Ti:Sapphire amplifier. The Stokes pulse carries energy of 4.4 mJ and is recompressed down to 66 fs by reflective grating pair. We characterized the short-wavelength mid-infrared source in view of energy stability, beam profile and conversion efficiency at a repetition rate of 100 Hz and 10 Hz. The demonstrated laser will benefit intense THz …
Nonsequential double ionization (NSDI) of helium in an intense few-cycle laser pulse is investigated by applying the three-dimensional semi-classical re-scattering method. It is found that the momentum distribution of He$^{2+}$ shows a single-double-single peak structure as the pulse intensity increases. According to the different mechanisms dominating the NSDI process, the laser intensity can be classified into three regimes where the momentum distribution of He$^{2+}$ exhibits different characteristics. In the relatively high intensity regime, an NSDI mechanism named the "laser-assisted coll…
A dramatic spectral modulation of third-order harmonic (TH) emission generated in a near in- frared femtosecond (fs) pulse filamentation, assisted by a two-dimensional plasma grating formed by two pump femtosecond pulses, is experimentally demonstrated when their spatiotemporal overlap is achieved. It is mainly attributed to strong cross-phase modulation induced by the fundamental wave of the probe pulse and two pump ones. The delay dynamic of TH spectra indicates the influence of two retarded nonlinear responses on the TH generation. The dependences of TH generation on the energies of probe a…
We demonstrate experimentally the full tunability of a coherent femtosecond source in the whole ultraviolet spectral region. The experiment relies on the technique of high-order harmonic generation driven by a near-infrared parametric laser source in krypton gas. By tuning the drive wavelength in the range between 1100 to 1900 nm, we generated intense harmonics from near to extreme ultraviolet. A number of photons per shot of the order of 10^7 has been measured for the first harmonic orders. Many novel scientific prospects are expected to benefit from the use of such a table-top tunable source…
In this paper, the spontaneous bremsstrahlung emission from an electron scattered by two fixed nuclei in an intense laser field is investigated in details based upon the Volkov state and the Dirac-Volkov propagator. It has been found that the fundamental harmonic spectrum from the electron radiation exhibits distinctive fringes, which is dependent not only upon the internucleus distance and orientation, but also upon the initial energy of the electron and the laser intensity. By analyzing the differential cross section, we are able to explain these effects in terms of interference among the el…
Ultrashort light pulse transport and amplification in a 1.3 m long step-index multimode fiber with gain and with weak coupling has been investigated. An adaptive shaping of the input wavefront, only based on the output intensity pattern, has led to an amplified pulse focused both in space (1/32) and in time (1/10) despite a strong modal group delay dispersion. Optimization of the input owing to the two-photon detection of the amplified signal permitted to excite the fastest and more intense principal mode of the fiber and to get an output pulse duration limited by group velocity dispersion.
Ultrashort, intense light pulses permit the study of nanomaterials in the optical non-linear regime, potentially leading to optoelectronics that operate in the petahertz domain. These non-linear regimes are often present just below the damage threshold thus requiring the careful tuning of laser parameters to avoid the melting and disintegration of the materials. Detailed studies of the damage threshold of nanoscale materials are therefore needed. We present results on the damage threshold of Au nanowires when illuminated by intense femtosecond pulses. These nanowires were synthesized with the …
We have demonstrated for the first time that an array of nanoantennas (central nanotips inside sub-micron pits) on an aluminum surface, fabricated using a specific double-pulse femtosecond laser irradiation scheme, results in a 28-fold enhancement of the non-linear (three-photon) electron photoemission yield, driven by a third intense IR femtosecond laser pulse. The supporting numerical electrodynamic modeling indicates that the electron emission is increased not owing to a larger effective aluminum surface, but due to instant local electromagnetic field enhancement near the nanoantenna, contr…
We report the fabrication of large-area phase masks on thin fused-silica substrates that are suitable for shaping multi-terawatt femtosecond laser beams. We apply these phase masks for the generation of intense femtosecond optical vortices. We further quantify distortions of the vortex beam patterns that result from several common types of mask defects.
We report on the observation of backward lasing at 391.4 nm of nitrogen ions pumped by linearly polarized intense femtosecond pulses at 800 nm. The strongly enhanced spectral intensity at 391.4 nm, as well as the amplification of an externally injected backward seeding pulse, confirm that the backward 391.4 nm signal is due to optical amplification in the gas plasma. Compared to the forward emission at 391.4 nm, the optimal backward emission is achieved at a lower gas pressure around 10 mbar, which is due to asymmetry of the backward and forward directions rooted in the traveling excitation ge…
Irradiation of intense ultrafast laser pulses in glasses can lead to formation of nanogratings whose periods are significantly smaller than the incident irradiation wavelength. The mechanism of the exotic phenomenon is still under debate. Here, we access the snapshots of morphologies in the laser affected regions in a porous glass which reveal the evolution of the formation of nanogratings with increasing number of laser pulses. Combined with further theoretical analyses, our observation provides important clues which suggest that excitation of standing plasma waves at the interfaces between a…
The processes of energy gain and redistribution in a dense gas subject to an intense ultrashort laser pulse are investigated theoretically for the case of high-pressure argon. The electrons released via strong-field ionization and driven by oscillating laser field collide with neutral neighbor atoms, thus effecting the energy gain in the emerging electron gas via a short-range inverse Bremsstrahlung interaction. These collisions also cause excitation and impact ionization of the atoms thus reducing the electron-gas energy. A kinetic model of these competing processes is developed which predict…
We show theoretically that an intense femtosecond optical pulse incident normally on a metal surface tends to decay into a pair of counter-propagating surface plasmon-polaritons (SPPs). The interference field heats the medium periodically, which causes a periodic permittivity perturbation and resonantly amplifies the magnitudes of SPPs. The instability growth time is only 10-50 fs for typical metals at damaging laser fluences. This mechanism is promising for the interpretation of laser-induced periodic surface structures formation in a single-pulse pumping regime.
We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrödinger eq…
We demonstrate fabrication of a high quality factor lithium niobate double-disk whispering-gallery microcavity using femtosecond laser assisted ion beam milling. Using this method, two vertically stacked 30-um-diameter disks with a 200-nm-gap are fabricated. With our device, an optical quality factor as high as 1.2*10^5 is demonstrated. Our approach is scalable to fabricate multiple disks on a single chip.
We experimentally studied intense femtosecond pulse filamentation and propagation in water for Gaussian, Laguerre-Gaussian, and Bessel-Gaussian incident beams. These different transverse modes for incident laser pulses were created from an initial Gaussian beam by using a computer generated hologram technique. We found that the length of the filament induced by the Bessel-Gaussian incident beam was longer than that for the other transverse modes under the conditions of the same peak intensity, pulse duration, and the size of the central part of the beam. To better understand the Bessel-Gaussia…
X-ray Free-Electron Lasers (XFELs) deliver X-ray pulses with a coherent flux that is approximately eight orders of magnitude greater than that available from a modern third generation synchrotron source. The power density in an XFEL pulse may be so high that it can modify the electronic properties of a sample on a femtosecond timescale. Exploration of the interaction of intense coherent X-ray pulses and matter is of both intrinsic scientific interest, and of critical importance to the interpretation of experiments that probe the structures of materials using high-brightness femtosecond XFEL pu…
The residual current density in monolayer graphene driven by an intense few-cycle chirped laser pulse is investigated via numerical solution of the time-dependent Schrödinger equation. It is found that the residual current is sensitive to the initial chirp rate, and the defined asymmetry degree for current along the different polarization direction versus chirp rate follows a simple sinusoidal function. The underlying physical mechanism is the chirp-dependent Landau-Zener-Stückelberg interference. The chirp control of currents provides a novel convenient tool in the petaHertz switching of two-…
We investigate dynamics of atomic and molecular systems exposed to intense, shaped chaotic fields and a weak femtosecond laser pulse theoretically. As a prototype example, the photoionization of a hydrogen atom is considered in detail. The net photoionization undergoes an optimal enhancement when a broadband chaotic field is added to the weak laser pulse. The enhanced ionization is analyzed using time-resolved wavepacket evolution and the population dynamics of the atomic levels. We elucidate the enhancement produced by spectrally-shaped chaotic fields of two different classes, one with a tuna…
Single-shot pulse retrieval of femtosecond bright squeezed vacuum
Technion – Israel Institute of Technology（以色列理工学院）；Solid State Institute（固态研究所）；Helen Diller Quantum Center（海伦·迪勒量子中心）；The Russell Berrie Nanotechnology Institute（罗素·贝里纳米技术研究所）；Max Planck Institute for the Science of Light（马克斯·普朗克光科学研究所）；Friedrich–Alexander Universität Erlangen–Nürnberg（埃尔朗根-纽伦堡弗里德里希-亚历山大大学）
Quantum-optical theory of the few femtosecond nonlinear optical response of Drude metals with a non-parabolic conduction band
South China Normal University（华南师范大学）；Shiv Nadar Institution of Eminence Deemed to be University（希夫纳达尔卓越大学）；Ben-Gurion University of the Negev（内盖夫本-古里安大学）
Delayed cavity-free forward lasing at the wavelengths of 391 and 428 nm was observed in recent experiments in air or pure nitrogen pumped with an intense femtosecond laser pulse at wavelength of 800~nm. The mechanism responsible for the lasing is highly controversial. In this article we explain the delayed emission by the presence of long-lived polarizations coupling simultaneously ground state X$^2Σ_g^+$ to states A$^2Π_u$ and B$^2Σ_u^+$ of singly ionized nitrogen molecules N$_2^+$. Ionization of neutral nitrogen molecules in a strong laser field and subsequent ion excitation are described by…
The mechanism of ablation of solids by intense femtosecond laser pulses is described in an explicit analytical form. It is shown that at high intensities when the ionization of the target material is complete before the end of the pulse, the ablation mechanism is the same for both metals and dielectrics. The physics of this new ablation regime involves ion acceleration in the electrostatic field caused by charge separation created by energetic electrons escaping from the target. The formulae for ablation thresholds and ablation rates for metals and dielectrics, combining the laser and target p…
The hybrid Stimulated Raman Scattering - Two Plasmon Decay instability had shown to play the dominant role for plasma waves excitation and energy absorption at interaction of very intense femtosecond obliquely incident $p$-polarized laser pulse (intensity $10^{17}-5\cdot10^{19}$ W/cm$^2$) with a steep gradient ($L\sim λ$) plasma near the quarter critical surface, i.e. within the typical for modern experiments conditions. The plasmons are excited as two wave packets confined near this surface with very wide $\approx ω_0/c$ spatial spectra along its normal. Hence, phase matching conditions for 3…
The dynamical properties of Cu in a regime relevant to femtosecond micro machining are obtained on picosecond time scales using pump-probe reflectivity study for 100fs, 1015 W cm-2 laser pulses. The electrical resistivity is obtained by solving Helmoltz equations. The dissipation mechanisms and scaling laws are obtained in high and low temperature limits. The 'resistivity saturation' effect in an unexplored regime intermediate to hot plasma and cold solid is studied in detail. The temperature evolution and thermal conductivity is obtained in the temporal range 0 to 30ps after the interaction o…
Mie-lithography: void-resonance-assisted femtosecond laser printing for deep-ultraviolet to near-infrared nano dispersion devices
State Key Laboratory of Precision Measurement Technology and Instruments, Department of Precision Instrument, Tsinghua University（精密测试技术与仪器国家重点实验室，精密仪器系，清华大学）；MIIT Key Laboratory of Complex-field Intelligent Exploration, School of Optics and Photonics, Beijing Institute of Technology（工业和信息化部复杂场智能探测重点实验室，光学与光子学院，北京理工大学）
