Broadband Laser Pulses Research Articles

Anomalous hot electron generation from two-plasmon decay instability driven by broadband laser pulses with intensity modulations

We investigate the hot electrons generated from two-plasmon decay (TPD) instability driven by laser pulses with intensity modulated by a frequency Δω m using theoretical and numerical approaches. Our primary focus lies on scenarios where Δω m is on the same order of the TPD growth rate γ 0 ( Δωm∼γ0 ), corresponding to moderate laser frequency bandwidths for TPD mitigation. With Δω m conveniently modeled by a basic two-color scheme of the laser wave fields in fully-kinetic particle-in-cell simulations, we demonstrate that the energies of TPD modes and hot electrons exhibit intermittent evolution at the frequency Δω m , particularly when Δωm∼γ0 . With the dynamic TPD behavior, the overall ratio of hot electron energy to the incident laser energy, fhot , changes significantly with Δω m . While fhot drops notably with increasing Δω m at large Δω m limit as expected, it goes anomalously beyond the hot electron energy ratio for a single-frequency incident laser pulse with the same average intensity when Δω m falls below a specific threshold frequency Δω c . This anomaly arises from the pronounced sensitivity of fhot to variations in laser intensity. We find this threshold frequency Δω c primarily depends on γ 0 and the collisional damping rate of plasma waves, with relatively lower sensitivity to the density scale length. We develop a scaling model characterizing the relation of Δω c and laser plasma conditions, enabling the potential extention of our findings to more complex and realistic scenarios.

Electron kinetic effects in back-stimulated Raman scattering bursts driven by broadband laser pulses

We examine electron kinetic effects in broadband-laser-driven back-stimulated Raman scattering (BSRS) bursts using particle-in-cell simulations. These bursts occur during the nonlinear stage, causing reflectivity spikes and generating large numbers of hot electrons. Long-duration simulations are performed to observe burst events, and a simplified model is developed to eliminate the interference of the broadband laser’s random intensity fluctuations. Using the simplified model, we isolate and characterize the spectrum of electron plasma waves. The spectrum changes from a sideband structure to a turbulence-like structure during the burst. A significant asymmetry in the spectrum is observed. This asymmetry is amplified and transferred to electron phase space by high-intensity broadband laser pulses, leading to violent vortex-merging and generation of hot electrons. The proportion of hot electrons increases from 6.76% to 14.7% during a single violent burst event. We demonstrate that kinetic effects profoundly influence the BSRS evolution driven by broadband lasers.

Linear and Nonlinear Optics of Broad-Band Laser Pulses: Diffraction.

The typical spectrally limited laser pulse in the near-infrared region is narrow-band up to 40-50 fs. Its spectral width Δk is much smaller than the carrying wavenumber k0 (Δk ≪ k0) . For such kinds of pulses, on distances of a few diffraction lengths, the diffraction is of a Fresnel's type and their evolution can be described correctly in the frame of the well-known paraxial evolution equation. The technology established in 1985 of amplification through chirping of laser pulses triggered remarkable progress in laser optics along with the construction of femtosecond (fs) laser facilities producing high intensity fields of the order of 1015-1021 W/cm2. However, the duration of the pulse was quickly shortened from picoseconds down to 5-6 fs, which have a broad-band nature (Δk ∼ k0). The linear and nonlinear propagation dynamics of broad-band pulses is quite different form their narrow-band counterparts. Here, we review the appropriate theoretical approach to study the evolution of the pulse. Moreover, we shed light on the different diffraction regimes inherent to both narrow-band and broad-band laser pulses and compare them to unveil the main differences. Using this very method, in subsequent papers, we will investigate the influence of the dispersion and nonlinearity on the laser pulse propagation in isotropic media.

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.

Parametric instabilities and hot electron generation in the interactions of broadband lasers with inhomogeneous plasmas

The development of parametric instabilities in the interaction of a large-scale inhomogeneous plasma with either a monochromatic or a broadband laser pulse is investigated theoretically and numerically. For a monochromatic laser at an intensity of W cm−2, the development of Stimulated Brillouin Scattering (SBS) in the relatively low density region will obviously dissipate pump laser and hence inhibit the development of Two-Plasmon Decay (TPD) and absolute Stimulated Raman Scattering (SRS) near the quarter-critical density. By using a laser with a moderate fractional bandwidth (∼1.0%) at the same averged intensity, it is found that the laser reflectivity will be greatly reduced since the SBS can be suppressed effectively due to its low linear growth rate. On the contrary, the TPD and absolute SRS are obviously enhanced since the in situ laser intensity near the quarter-critical density becomes stronger in this case. As a result, the hot electron generation due to the TPD and absolute SRS is dramatically enhanced as well. This indicates that the competition between various parametric instabilities in a large-scale inhomogeneous plasma makes it more challenging to simultaneously suppress all kinds of parametric instabilities by using broadband lasers. Particular attention should be paid to the TPD, which not only has a relatively large linear growth rate but also is efficient in generating harmful hot electrons. Increasing the laser bandwidth further, the hot electron generation will be finally reduced as long as the TPD and SRS are also suppressed with a sufficient bandwidth (3%) at the intensity of W cm−2 that may be encountered in some novel ignition schemes such as shock ignition. However, it is worth noting that the laser bandwidth required to mitigate parametric instabilities and hot electron production strongly depends on laser intensity. A moderate laser bandwidth (∼1%) may be sufficient to mitigate both the laser reflectivity and hot electron production for typical ICF target designs operated with laser intensities lower than 1015 W cm−2.

Three-stage laser wakefield accelerator scheme for sub-Joule few-cycle laser pulses

Laser-driven electron acceleration in underdense plasma is a promising route towards the realization of reliable sources of relativistic electrons in the 0.1–1 GeV energy range. Generation of such electron bunches at high repetition rates is hindered by the limited energy per pulse, which inevitably results in very short pulse duration and tight focusing. Compressing the laser energy in time and space allows scientists to use higher plasma density to drive wakefieds, which in turn results in enhanced diffraction and dispersion of the broadband laser pulse. These features make difficult to control the acceleration in the plasma wave and to improve the beam quality. Here we propose a mm-long three-stage acceleration scheme, which allows for tunable injection and optimal acceleration of high-quality electron bunches. The full interaction length is modeled by 3D particle-in-cell simulations.

Imaging and controlling coherent phonon wave packets in single graphene nanoribbons

The motion of atoms is at the heart of any chemical or structural transformation in molecules and materials. Upon activation of this motion by an external source, several (usually many) vibrational modes can be coherently coupled, thus facilitating the chemical or structural phase transformation. These coherent dynamics occur on the ultrafast timescale, as revealed, e.g., by nonlocal ultrafast vibrational spectroscopic measurements in bulk molecular ensembles and solids. Tracking and controlling vibrational coherences locally at the atomic and molecular scales is, however, much more challenging and in fact has remained elusive so far. Here, we demonstrate that the vibrational coherences induced by broadband laser pulses on a single graphene nanoribbon (GNR) can be probed by femtosecond coherent anti-Stokes Raman spectroscopy (CARS) when performed in a scanning tunnelling microscope (STM). In addition to determining dephasing (~440 fs) and population decay times (~1.8 ps) of the generated phonon wave packets, we are able to track and control the corresponding quantum coherences, which we show to evolve on time scales as short as ~70 fs. We demonstrate that a two-dimensional frequency correlation spectrum unequivocally reveals the quantum couplings between different phonon modes in the GNR.

Rotation of the polarization ellipse for broad-band and narrow-band optical pulses. Analytical solutions

In present days the evolution of broad-band laser pulses, propagating in various types of waveguides, has been of a great interest among the scientists. Currently, it is easy for phase-modulated femtosecond pulses the condition Δω≈ω0 to be obtained. It is known that nowadays it is possible also to reach the attosecond region where the spectral bandwidth of the pulse happens to be of order of the carrier frequency also. Light pulses who fulfil this initial condition are called broad-band. On the other hand, the non-fulfilling pulses are the narrow-band ones.In the present paper it is investigated the parametric interaction of two components of one optical pulse by using the Generalized System of Nonlinear Amplitude Equations (GSNAE). GSNAE was analytically solved. A difference in the period of oscillations of the energy exchange between the two components is found.

Photoelectron circular dichroism in fenchone by short coherent broadband laser pulses

Photoelectron circular dichroism (PECD) of fenchone induced by short coherent broadband laser pulses is studied theoretically using the time-dependent single-center method. In particular, we investigate the chiral response to circularly polarized pulses with a sine-squared energy spectrum between 1 and 3 eV. We consider nonchirped and differently chirped pulses of a moderate peak intensity of $3\ifmmode\times\else\texttimes\fi{}{10}^{12}\phantom{\rule{3.33333pt}{0ex}}\mathrm{W}/{\mathrm{cm}}^{2}$ and a nonchirped pulse of a higher peak intensity of $1\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{3.33333pt}{0ex}}\mathrm{W}/{\mathrm{cm}}^{2}$ leading to a strong-field ionization. Thereby, effects of the frequency ordering and pulse intensity are investigated in some detail. The present theoretical study predicts a substantial multiphoton PECD of fenchone, which can be manipulated by tailoring a spectral phase and intensity profile of a single coherent broadband laser pulse.

Ultra-broadband all-optical sampling of optical waveforms.

Optical-field sampling techniques provide direct access to the electric field of visible and near-infrared light. The existing methods achieve the necessary bandwidth using highly nonlinear light-matter interaction that involves ionization of atoms or generation of charge carriers in solids. We demonstrate an alternative, all-optical approach for measuring electric fields of broadband laser pulses, which offers an advantage in terms of sensitivity and signal-to-noise ratio and extends the detection bandwidth of optical methods to the petahertzdomain.

Features of noncollinear second harmonic generation by infrared laser pulses with opposite frequency chirps

The features of noncollinear second harmonic generation during the interaction of broadband laser pulses with opposite frequency chirps are considered. The impact of spectral phase mismatch of the interacting pulses on spectrum width and the efficiency of conversion to the noncollinear second harmonic is analyzed on an example of lithium triborate and beta-barium borate crystals.

Stochastic exciton-scattering theory of optical line shapes: Renormalized many-body contributions.

Spectral line shapes provide a window into the local environment coupled to a quantum transition in the condensed phase. In this paper, we build upon a stochastic model to account for non-stationary background processes produced by broad-band pulsed laser stimulation, as distinguished from those for stationary phonon bath. In particular, we consider the contribution of pair-fluctuations arising from the full bosonic many-body Hamiltonian within a mean-field approximation, treating the coupling to the system as a stochastic noise term. Using the Itô transformation, we consider two limiting cases for our model, which lead to a connection between the observed spectral fluctuations and the spectral density of the environment. In the first case, we consider a Brownian environment and show that this produces spectral dynamics that relax to form dressed excitonic states and recover an Anderson-Kubo-like form for the spectral correlations. In the second case, we assume that the spectrum is Anderson-Kubo like and invert to determine the corresponding background. Using the Jensen inequality, we obtain an upper limit for the spectral density for the background. The results presented here provide the technical tools for applying the stochastic model to a broad range of problems.

Temporal characterization of broadband femtosecond laser pulses by surface third-harmonic dispersion scan with ptychographic retrieval.

We present a new, to the best of our knowledge, variant of dispersion scan (d-scan) based on surface third-harmonic generation (STHG) and a ptychographic algorithm tailored for full retrieval (amplitude and phase) of broadband laser pulses. We demonstrate the technique by temporally measuring and compressing few-cycle pulses with 7 fs and 2.5 nJ from a Ti:sapphire oscillator, using a sapphire window as the nonlinear medium. The results are in very good agreement with standard second-harmonic d-scan measurements based on a nonlinear crystal. The intrinsically broadband and phase-matching-independent nature of STHG make this technique very suitable for the characterization of ultrashort laser pulses over a broad wavelength range extending into the mid-infrared.

Time-resolved vibrational-pump visible-probe spectroscopy for thermal conductivity measurement of metal-halide perovskites.

Understanding thermal transport at the microscale to the nanoscale is crucially important for a wide range of technologies ranging from device thermal management and protection systems to thermal-energy regulation and harvesting. In the past decades, non-contact optical methods, such as time-domain and frequency-domain thermoreflectance, have emerged as extremely powerful and versatile thermal metrological techniques for the measurement of material thermal conductivities. Here, we report the measurement of thermal conductivity of thin films of CH3NH3PbI3 (MAPbI3), a prototypical metal-halide perovskite, by developing a time-resolved optical technique called vibrational-pump visible-probe (VPVP) spectroscopy. The VPVP technique relies on the direct thermal excitation of MAPbI3 by femtosecond mid-infrared optical pump pulses that are wavelength-tuned to a vibrational mode of the material, after which the time dependent optical transmittance across the visible range is probed in the ns to the μs time window using a broadband pulsed laser. Using the VPVP method, we determine the thermal conductivities of MAPbI3 thin films deposited on different substrates. The transducer-free VPVP method reported here is expected to permit spectrally resolving and spatiotemporally imaging of the dynamic lattice temperature variations in organic, polymeric, and hybrid organic-inorganic semiconductors.

Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules

Fixing molecules in space is a crucial step for the imaging of molecular structure and dynamics. Here, we demonstrate three-dimensional (3D) field-free alignment of the prototypical asymmetric top molecule indole using elliptically polarized, shaped, off-resonant laser pulses. A truncated laser pulse is produced using a combination of extreme linear chirping and controlled phase and amplitude shaping using a spatial-light-modulator (SLM) based pulse shaper of a broadband laser pulse. The angular confinement is detected through velocity-map imaging of H+ and C2+ fragments resulting from strong-field ionization and Coulomb explosion of the aligned molecules by intense femtosecond laser pulses. The achieved three-dimensional alignment is characterized by comparing the result of ion-velocity-map measurements for different alignment directions and for different times during and after the alignment laser pulse to accurate computational results. The achieved strong three-dimensional field-free alignment of < {cos }^{2}delta > =0.89 demonstrates the feasibility of both, strong three-dimensional alignment of generic complex molecules and its quantitative characterization.

Spectral phase-front diagnostics for ultrashort laser pulses via quasi-self-referenced interferometry

We present a novel, to the best of our knowledge, design for the spectrally resolved wavefront diagnostics of ultrashort laser pulses. The design uses quasi-self-referenced interferometry (qSRI), is completely achromatic, and avoids dispersion. The qSRI utilizes a perfect reference beam enabling an absolute measurement of the near-field spatial phase distributions for the different spectral components of ultrashort laser pulses. For this, a Mach–Zehnder geometry is coupled with a spatial filter. Combining the qSRI with a reflective grating allows for the measurement of phase fronts in the whole spectrum of a broadband laser pulse without any calibration.

Potential continuous zooming scheme based on high-power broadband laser

Continuous zooming is efficient in mitigating the cross-beam energy transfer effect and improving implosion hydrodynamic efficiency in the application of inertial confinement fusion. In this paper, a novel continuous zooming scheme is proposed, based on the chromatic aberration effect of the lens groups to gradually reduce the size of the focal spot at the target position by focusing the broadband laser pulse. This scheme is simulated theoretically on the Shenguang-II upgrade (SG-II UP) facility, and the results show that the focal spot size is positive and linear for the beam wavelength. When the fundamental wave bandwidth was 5 nm, the focal spot radius was reduced by 15.21% without changing the geometric parameters of the SG-II upgrade, and the focal spot radius was reduced by 27.73% after optimization. In addition, the conversion efficiency is compensated for in the harmonic converter. This paper supports a new perspective for the realization of high-power laser zooming.

Suppression of the non-linear background in a multimode fibre CARS endoscope.

Multimode fibres show great potential for use as miniature endoscopes for imaging deep in tissue with minimal damage. When used for coherent anti-Stokes Raman scattering (CARS) microscopy with femtosecond excitation sources, a high band-width probe is required to efficiently focus the broadband laser pulses at the sample plane. Although graded-index (GRIN) fibres have a large bandwidth, it is accompanied by a strong background signal from four-wave mixing and other non-linear processes occurring inside the fibre. We demonstrate that using a composite probe consisting of a GRIN fibre with a spliced on step-index fibre reduces the intensity of the non-linear background by more than one order of magnitude without significantly decreasing the focusing performance of the probe. Using this composite probe we acquire CARS images of biologically relevant tissue such as myelinated axons in the brain with good contrast.

Superluminal-subluminal orbital angular momentum femtosecond laser focus.

The interplay between the frequency chirping of a broadband laser pulse and the longitudinal chromatic aberration of a focusing optic introduces the superluminal or subluminal behavior to a laser focus. In this paper, we present an analytic expression for an electric field describing a superluminal or subluminal femtosecond laser focus with orbital angular momentum. The analytic expression for a superluminal or subluminal laser focus is obtained through a diffraction integral, in which the focal length is replaced by a time-dependent focal length under the paraxial approximation, and the Fourier transformation. The speed and pulse duration of a laser focus are determined by the total group delay dispersion and a chromaticity parameter defined by the longitudinal chromatic aberration of a dispersive focusing optic. It is shown that it is possible to generate a several femtosecond superluminal orbital angular momentum laser focus in the focal region.

Broadband visible two-dimensional spectroscopy of molecular dyes.

Two-dimensional Fourier transform spectroscopy is a promising technique to study ultrafast molecular dynamics. Similar to transient absorption spectroscopy, a more complete picture of the dynamics requires broadband laser pulses to observe transient changes over a large enough bandwidth, exceeding the inhomogeneous width of electronic transitions, as well as the separation between the electronic or vibronic transitions of interest. Here, we present visible broadband 2D spectra of a series of dye molecules and report vibrational coherences with frequencies up to ∼1400cm-1 that were obtained after improvements to our existing two-dimensional Fourier transform setup [Al Haddad et al., Opt. Lett. 40, 312-315 (2015)]. The experiment uses white light from a hollow core fiber, allowing us to acquire 2D spectra with a bandwidth of 200nm, in a range between 500 and 800nm, and with a temporal resolution of 10-15fs. 2D spectra of nile blue, rhodamine 800, terylene diimide, and pinacyanol iodide show vibronic spectral features with at least one vibrational mode and reveal information about structural motion via coherent oscillations of the 2D signals during the population time. For the case of pinacyanol iodide, these observations are complemented by its Raman spectrum, as well as the calculated Raman activity at the ground- and excited-state geometry.