Femtosecond-scale Synchronisation of Ultra-Intense Focused Laser Beams
D. J. Corvan, W. Schumaker, J. Cole, H. Ahmed, K. Krushelnick, S. P. D. Mangles, Z. Najmudin, D. Symes, A. G. R. Thomas, M. Yeung, M. Zepf, Z. Zhao, G. Sarri
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 beneficial for the next generation of multiple, petawatt class laser systems.
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 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 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…
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 …
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…
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 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 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.
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 …
Frequency downshifting stair for ultra-intense femtosecond lasers through a plasma-photonics structure
Tsinghua University（清华大学）；National Key Laboratory of Plasma Physics, Laser Fusion Research Center, China Academy of Engineering Physics（中国工程物理研究院激光聚变研究中心等离子体物理国家重点实验室）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；Shanghai Institute of Laser Plasma, China Academy of Engineering Physics（中国工程物理研究院上海激光等离子体研究所）；Institute of High Energy Physics, Chinese Academy of Sciences（中国科学院高能物理研究所）
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-…
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…
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 report on experimental realization of impulsive rotational Raman scattering from neutral nitrogen molecules in a femtosecond laser filament using an intense self-induced white-light seeding "air laser" generated during the filamentation of an 800 nm Ti: Sapphire laser in nitrogen gas. The impulsive rotational Raman fingerprint signals are observed with a maximum conversion efficiency of ~0.8%. Our observation provides a promising way of remote identification and location of chemical species in atmosphere by rotational Raman scattering of molecules.
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 measuri…
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 …
We quantify the dependence of the single-shot ablation threshold on the angle of incidence and polarization of a femtosecond laser beam, for three dissimilar solid-state materials: a metal, a dielectric and a semiconductor. Using the constant, linear value of the index of refraction, we calculate the laser fluence transmitted through the air-material interface at the point of ablation threshold. We show that, in spite of the highly nonlinear ionization dynamics involved in the ablation process, the so defined transmitted threshold fluence is universally independent of the angle of incidence an…
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…
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…
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…
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）
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.
We report generation of cascaded rotational Raman scattering up to 58th orders in coherently excited CO_2 molecules. The high-order Raman scattering, which produces a quasiperiodic frequency comb with more than 600 sidebands, is obtained using an intense femtosecond laser to impulsively excite rotational coherence and the femtosecond-laser-induced N_2^+ lasing to generate cascaded Raman signals. The novel configuration allows this experiment to be performed with a single femtosecond laser beam at free-space standoff locations. It is revealed that the efficient spectral extension of Raman signa…
Multiple filamentation in air of high-power ultrashort laser radiation with transverse intensity profile resembling a "corona" composed by incoherent combining of several annularly distributed independent top-hat sub-beams is theoretically studied. Through the numerical solution of time-averaged nonlinear Schrodinger equation, we study the spatio-angular dynamics of synthesized near-infrared "corona-beam" (CB) along the optical path by varying the number and power of the beamlets (corona-spikes). For the first time to our knowledge, the evident advances in the multiple filamentation region man…
The formation of an electron-hole plasma during the interaction of intense femtosecond laser pulses with transparent solids lies at the heart of femtosecond laser processing. Advanced micro- and nanomachining applications require improved control over the excitation characteristics. Here, we relate the emission of low-order harmonics to the strong laser-field-induced plasma formation. Together with a measurement of the total plasma density we identify the contribution of two competing ionization mechanisms - strong-field and electron-impact ionization.
We have demonstrated the fabrication and characterization of 2D liquid-based multimode optical waveguide structures over a Polydimethylsiloxane (PDMS) material-based chip. Fabrication of two separate microstructures, one with a width of 14 microns and a depth of 27 microns while the other with a width as well as depth of 110 microns, was achieved by the femtosecond laser micromachining process. The dye solution is passed through the microstructure from one end to the other; wherein the dye solution acts as the core while PDMS and air act as the cladding medium. The femtosecond laser micromachi…
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…
Laser-induced modification of transparent solids by intense femtosecond laser pulses allows fast integration of nanophotonic and nanofluidic devices with controlled optical properties. So far, the local and dynamic nature of the interactions between plasma and light needed to correctly explain nanograting fabrication on dielectric surfaces has been missing in the theoretical models. With our numerical approach, we show that a self-consistent dynamic treatment of the plasma formation and its interaction with light triggers an ultrafast reconfiguration of the periodic plasma patterns on a field-…
Ultrafast optical excitation with intense mid-infrared and terahertz pulses has emerged as a new tool to control materials dynamically. As most experiments are performed with femtosecond pulse excitation, typical lifetimes of most light-induced phenomena in solids are of only few picoseconds. Yet, many scientific applications require longer drive pulses and lifetimes. Here, we describe a mid-infrared pump - terahertz-probe setup based on a CO$\mathrm{_2}$ laser seeded with 10.6 $\mathrmμ$m wavelength pulses from an optical parametric amplifier, itself pumped by a Ti:Al$\mathrm{_2}$O$\mathrm{_3…
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.
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-…
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）
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…
Femtosecond laser pulses interacting with LiNbO3 has been widely applied in intense terahertz generation, excitation and imaging of phonon polaritons and modulating light. It is of great importance to study the nonlinearities induced by femtosecond laser pulses in LiNbO3. Here, we demonstrate that both Kerr nonlinearity and Kerr-like nonlinearity induced by terahertz wave occur under the interaction between laser pulses and LiNbO3 using optical pump-probe techniques. We show that the contribution of Kerr-like nonlinearity to pump-probe spectra varies with the interaction length because of the …
Nonlinear propagation of intense femtosecond laser pulses in bulk transparent media leads to a specific propagation regime, termed femtosecond filamentation, which in turn produces dramatic spectral broadening, or superbroadening, termed supercontinuum generation. Femtosecond supercontinuum generation in transparent solids represents a compact, efficient and alignment-insensitive technique for generation of coherent broadband radiation at various parts of the optical spectrum, which finds numerous applications in diverse fields of modern ultrafast science. During recent years, this research fi…
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…
Electromagnetic radiation within the terahertz (THz) frequency range is of great interest for applications in remote sensing and time-domain spectroscopy. The laser-induced plasmas are promising mediums for generating THz radiation. It has been recently reported that focusing femtosecond Bessel pulses inside dielectrics induces a high aspect ratio over-critical plasmas. Here we show that the intense resonantly driven electrostatic fields at the so-called critical surface lead to THz radiation emission. Through three-dimensional particle-in-cell simulation and analytical derivation, we have inv…
