Interaction Of Femtosecond Pulses Research Articles

Ionization dynamics and damage conditions in fused silica irradiated with mid-infrared femtosecond pulses

The employment of ultrashort laser sources at the mid-infrared (mid-IR) spectral region for dielectrics is expected to open innovative routes for laser patterning and a wealth of exciting applications in optics and photonics. To elucidate the material response to irradiation with mid-IR laser sources, a consistent analysis of the interaction of long wavelength femtosecond pulses with dielectric materials is presented. The influence of the pulse duration is particularly emphasized in specifying the laser parameters for which photoionization and impact ionization are important. Simulation results using pulses at 2.2, 3.2, and 5 μm are conducted to illustrate optimum conditions for the onset of damage on the solid that is related to the occurrence of the optical breakdown. The results predict that the damage threshold scales as ∼τpa (0.31≤a≤0.37) at all laser wavelengths. Given the significant effect of the induced excitation level on excitation of surface plasmons (SPs), which account for the formation of laser-induced periodic structures oriented perpendicular to the laser polarization, a correlation of the produced electron densities with SPs and the threshold of SP excitation (∼τpβ, 0.33≤β≤0.39) are also discussed in this as yet unexplored spectral region. The results are expected to guide development of an innovative approach to surface patterning using strong mid-IR pulses for advanced applications.

Frequency Down-Conversion of Optical Pulse to the Far Infrared and THz Frequency Ranges Due to the Cascading Process in a Medium with a Quadratic Nonlinear Response

Difference-frequency generation is a well-known method of obtaining IR and THz radiation. It has many practical applications, such as sensing, optical metrology, diagnostics, detection and identification of substances, etc. One of the generation methods is based on the three-wave interaction in a medium with second-order nonlinear susceptibility. In this study, we investigated a special case of the frequency down-conversion into IR and THz ranges of the frequencies: the frequencies of interacting waves were multiple. We analyzed theoretically two cases of three-wave interactions: amplification of the infrared (or THz) radiation (incident weak intensity of a wave at this frequency) and a wave generation with the difference-frequency (incident zero-value intensity at this frequency). The amplification efficiency could achieve 75% and the maximal frequency conversion efficiency is about 25%. The computer simulation results made for the femtosecond pulse interaction in a crystal with the wavelength 4, 10, and 24 μm demonstrates applicability of such a scheme for the frequency down-conversion. This scheme of the THz radiation generation is a perspective tool for its application in the screening system for the detection and identification of substances.

Effect of Electron–Ion Collisions on the Generation of Terahertz Radiation at the Interaction of Femtosecond Pulse with Plasma in Magnetic Field

Effect of Electron–Ion Collisions on the Generation of Terahertz Radiation at the Interaction of Femtosecond Pulse with Plasma in Magnetic Field

Pulse Energy and Pulse Duration Effects in the Ionization and Fragmentation of Iodomethane by Ultraintense Hard X Rays

The interaction of intense femtosecond x-ray pulses with molecules sensitively depends on the interplay between multiple photoabsorptions, Auger decay, charge rearrangement, and nuclear motion. Here, we report on a combined experimental and theoretical study of the ionization and fragmentation of iodomethane (CH_{3}I) by ultraintense (∼10^{19} W/cm^{2}) x-ray pulses at 8.3keV, demonstrating how these dynamics depend on the x-ray pulse energy and duration. We show that the timing of multiple ionization steps leading to a particular reaction product and, thus, the product's final kinetic energy, is determined by the pulse duration rather than the pulse energy or intensity. While the overall degree of ionization is mainly defined by the pulse energy, our measurement reveals that the yield of the fragments with the highest charge states is enhanced for short pulse durations, in contrast to earlier observations for atoms and small molecules in the soft x-ray domain. We attribute this effect to a decreased charge transfer efficiency at larger internuclear separations, which are reached during longer pulses.

Comparative study on epsilon-near-zero transparent conducting oxides: High-order chromatic dispersions and modeling of ultrashort pulse interactions

A comparative study on the chromatic dispersions and the interactions with ultrashort pulses in epsilon-near-zero (ENZ) transparent conducting oxides (TCOs) is theoretically presented. The ENZ TCOs exhibit rapidly varying and unprecedentedly large $N\mathrm{th}$-order dispersions in the ENZ region, which is exclusive to ENZ plasmonic materials. However, it is found that in both physical and mathematical senses, the concepts of high $N\mathrm{th}$-order chromatic dispersions are inapplicable for ENZ TCOs with Drude-like permittivity. Subsequently, the impacts of the complex permittivity dispersion profiles on ultrashort pulse interactions are discussed. Comparisons are made between propagation patterns in an ENZ AZO waveguide obtained from the nonlinear Schr\"odinger equation (NLSE) and Maxwell's equations, as well as between interactions of femtosecond pulses with different temporal widths in a subwavelength ENZ AZO slab. Results show that the well-received NLSE is not suitable for modeling ENZ TCOs in either case, and subwavelength interaction patterns with different pulse widths are quite different, where the shorter pulse can excite stronger localized resonance.

Ultrabroadband nonlinear optics in nanophotonic periodically poled lithium niobate waveguides

Quasi-phase-matched interactions in waveguides with quadratic nonlinearities enable highly efficient nonlinear frequency conversion. In this paper, we demonstrate the first generation of devices that combine the dispersion engineering available in nanophotonic waveguides with quasi-phase-matched nonlinear interactions available in periodically poled lithium niobate (PPLN). This combination enables quasi-static interactions of femtosecond pulses, reducing the pulse energy requirements by several orders of magnitude compared to conventional devices, from picojoules to femtojoules. We experimentally demonstrate two effects associated with second harmonic generation (SHG). First, we observe efficient quasi-phase-matched SHG with < 100 f J of pulse energy. Second, in the limit of strong phase-mismatch, we observe spectral broadening of both harmonics with as little as 2 pJ of pulse energy. These results lay a foundation for a new class of nonlinear devices, in which coengineering of dispersion with quasi-phase-matching enables efficient nonlinear optics at the femtojoule level.

A Model Describing the Propagation of a Femtosecond Pulse in a Kerr Nonlinear Medium

We consider a model of nonlinear interaction of femtosecond pulses with a Kerr nonlinear medium, allowing for first and second order dispersion, nonlinear response dispersion, and mixed time and space derivatives. The invariants are constructed by a transformation of the generalized nonlinear Schrodinger equation that involves changing to new functions and reduces the original equation to a form without the nonlinear response derivatives and the mixed derivatives. Appropriate conservation laws are established for the transformed equation. The invariants derived in this article lead to conservative difference schemes and allow control of computer simulation results.

Scattering of a short electromagnetic pulse from a Lorentz–Duffing film: Theoretical and numerical analysis

We combine scattering theory, Fourier, traveling wave and asymptotic analyses together with numerical simulations to present interesting and practically useful properties of femtosecond pulse interaction with thin films. The dispersive material is described by a single resonance Lorentz model and its nonlinear extension with a cubic Duffing-type nonlinearity. A key feature of the Lorentz dielectric function is that its real part becomes negative between its zero and its pole, generating a forbidden region. We illustrate numerically the linear interaction of the pulse with the film using both scattering theory and Fourier analysis. Outside this region we show the generation of a sequence of pulses separated by round trips in the Fabry–Perot cavity due to multiple reflections. When the pulse spectrum is inside the forbidden region, we observe total reflection. Near the pole of the dielectric function, we demonstrate the slowing down of the pulse (group velocity tending to zero) in the medium that behaves as a high-Q cavity. We use the combination of analysis and simulations in the linear regime to validate the delta function approximation of the thin layer; this collapses the forbidden region to a single resonant point of the spectrum. We also study the single cycle pulse interaction with a thin film and show three distinct types of reflection: half-pulse, sinusoidal wave train and cosine wavelet. Finally we analyze the influence of a strong nonlinearity and observe that the film switches from reflecting to transparent.

Interaction of Phase-Modulated Femtosecond Pulses with an Optically Dense Quasi-Resonant Medium of Rubidium Vapors

For the first time, it is demonstrated that the magnitude and sign of the effect of “spectral condensation” of a laser pulse at the resonant-transition frequency of a dense medium can be controlled by changing the driving-pulse parameters (chirp, pulse width, and pulse amplitude). In the process of this, importantly, the driving-pulse energy and spectrum remain unchanged. Direct time-resolved measurements revealed an oscillatory character of the induced superradiance of rubidium vapors representing a long train of decaying short pulses. The width and repetition rate of the pulses in the train are determined by atomic density N0 of the medium, while the width of an entire superradiance pulse (10 ps) is considerably larger than that of the driving laser pulse (50 fs).

Growth mechanisms of multiscale, mound-like surface structures on titanium by femtosecond laser processing.

Femtosecond laser surface processing (FLSP) can be used to functionalize many surfaces, imparting specialized properties such as increased broadband optical absorption or super-hydrophobicity/-hydrophilicity. In this study, the subsurface microstructure of a series of mound-like FLSP structures formed on commercially pure titanium using five combinations of laser fluence and cumulative pulse counts was studied. Using a dual beam Scanning Electron Microscope with a Focused Ion Beam, the subsurface microstructure for each FLSP structure type was revealed by cross-sectioning. The microstructure of the mounds formed using the lowest fluence value consists of the original Ti grains. This is evidence that preferential laser ablation is the primary formation mechanism. However, the underlying microstructure of mounds produced using higher fluence values was composed of a distinct smaller-grained α-Ti region adjacent to the original larger Ti grains remaining deeper beneath the surface. This layer was attributed to resolidification of molten Ti from the hydrodynamic Marangoni effect driven fluid flow of molten Ti, which is the result of the femtosecond pulse interaction with the material.

Pulse reshaping in nearly resonant interaction of femtosecond pulses with dense rubidium vapor

Propagation of intense femtosecond pulses resonant with the atomic rubidium vapor results in phenomenon known as conical emission. The origin of this phenomenon is connected with self-phase modulation in time domain accompanied with spatial self-focusing for blue-detuned pulses. When the laser central wavelength is red-detuned the self-defocusing occurs. Using frequency-resolved optical gating measurements and simple modeling of pulse propagation within the linear dispersion theory it is shown that the retrieved phase of the propagated pulse, and the associated instantaneous frequency, shows evidence of both linear dispersion and self-phase modulation. These results are consistent with the theory of the intensity dependent nonlinear refraction index in medium where linear dispersion contributes significantly to pulse reshaping.

Interactions of femtosecond pulses with Λ-type atoms

The dynamics ofatomic populations in the field of a single femtosecond pulse is numerically investigated in the frameworks of the resonant approximation and beyond it. It is shown that for the pulses with the extremely short duration the violation of resonant approximation leads not only to the quantitative but also to the qualitative changes in the behavior of the three-level atom.

Ultrafast structural dynamics studied by kilohertz time-resolved x-ray diffraction**Project supported by the National Natural Science Foundation of China (Grant Nos. 61222509 and 11421064) and the W. M. Keck Foundation.

Ultrashort multi-keV x-ray pulses are generated by electron plasma produced by the irradiation of femtosecond pulses on metals. These sub-picosecond x-ray pulses have extended the field of x-ray spectroscopy into the femtosecond time domain. However, pulse-to-pulse instability and long data acquisition time restrict the application of ultrashort x-ray systems operating at low repetition rates. Here we report on the performance of a femtosecond laser plasma-induced hard x-ray source that operates at 1-kHz repetition rate, and provides a flux of 2.0 × 1010 photons/s of Cu Kα radiation. Using this system for time-resolved x-ray diffraction experiments, we record in real time, the transient processes and structural changes induced by the interaction of 400-nm femtosecond pulse with the surface of a 200-nm thick Au (111) single crystal.

Theoretical analysis of hard x-ray generation by nonperturbative interaction of ultrashort light pulses with a metal.

The interaction of intense femtosecond pulses with metals allows for generating ultrashort hard x-rays. In contrast to plasma theories, tunneling from the target into vacuum is introduced as electron generation step, followed by vacuum acceleration in the laser field and re-entrance into the target to generate characteristic x-rays and Bremsstrahlung. For negligible space charge in vacuum, the Kα flux is proportional to the incident intensity and the wavelength squared, suggesting a strong enhancement of the x-ray flux by mid-infrared driving pulses. This prediction is in quantitative agreement with experiments on femtosecond Cu Kα generation.

Programming cell fate on bio-functionalized silicon

Controlling the growth of cells on the surface of silicon without an additive layer or topographical modification is unexplored. This research article delineates the discovery of unique properties of a bio-functionalized silicon substrate, programmed to repel or control cells, generated by ultrafast femtosecond pulse interaction with silicon. Remarkably, bio-functionalization in any shape or size without change in topology or morphology is observed indicating only sub-surface phase transformations. Material characterization reveals the presence of a unique mixture of phases of SiO2 and Si. Consequently, these variations in phase alter the physicochemical characteristics on the surface of silicon resulting in its bio-functionalization. The culture of mouse embryonic fibroblasts shows unique adhesion characteristics on these bio-functionalized silicon surfaces that include cell controlling, cell trapping, and cell shaping. Furthermore, the directionality of fibroblasts is restrained parallel to bio-functionalized zones as evidenced by changes in cytoskeleton. The controlling of proliferation, migration and adhesion of cells is attributed to unique phase bio-functionalization. This method presents considerable promise in a myriad of applications such as tissue engineering, MEMS, and lab-on-a-chip devices.

Diffraction before destruction.

X-ray free-electron lasers have opened up the possibility of structure determination of protein crystals at room temperature, free of radiation damage. The femtosecond-duration pulses of these sources enable diffraction signals to be collected from samples at doses of 1000 MGy or higher. The sample is vaporized by the intense pulse, but not before the scattering that gives rise to the diffraction pattern takes place. Consequently, only a single flash diffraction pattern can be recorded from a crystal, giving rise to the method of serial crystallography where tens of thousands of patterns are collected from individual crystals that flow across the beam and the patterns are indexed and aggregated into a set of structure factors. The high-dose tolerance and the many-crystal averaging approach allow data to be collected from much smaller crystals than have been examined at synchrotron radiation facilities, even from radiation-sensitive samples. Here, we review the interaction of intense femtosecond X-ray pulses with materials and discuss the implications for structure determination. We identify various dose regimes and conclude that the strongest achievable signals for a given sample are attained at the highest possible dose rates, from highest possible pulse intensities.

Interaction of femtosecond pulses of a two-harmonic Ti:Sapphire laser with liquid media

The interaction of ultrashort laser pulses having wavelengths of 400 and 800 nm with liquid media, including organic solutions, has been experimentally studied. It is shown that transparent drops evaporate and boil (with partial mass ejection in the form of vapor and liquid fragments) in the field of ultrashort light pulse. A large-scale change in the spectrum of laser pulse during its interaction with a water particle is revealed. This change is caused by self-modulation of the light phase due to the Kerr optical nonlinearity of liquid and the formation of plasma. Filamentation in continuous liquid media is analyzed; specifically, the dependences of the number of filaments, the lasing spectrum width, the nonlinear-focusing distance, and the filamentation region diameter on the laser pulse power are measured. It is noted that there is a range of relative powers where the number of filaments very rapidly increases. It is shown that the spectral broadening at filamentation, observed for fixed pulse energy with a change in pulse width, overlaps the entire visible spectral range. This circumstance makes it possible to obtain width-tunable pulses and use them, e.g., in optoacoustic diagnostics of media.

Direct laser writing of buried waveguide in As_2S_3 glass using a helical sample translation

We report the fabrication and the characterization of buried waveguide in As(2)S(3) glass. It is well known that the interaction of femtosecond pulses with this material at high laser repetition rates results in a mainly negative refractive index variation, due to heat accumulation effect. However, we show here that a helical translation of the sample parallel to the laser beam, allows the inscription of a core of positive refractive variation, with full control over its magnitude and diameter. An example demonstrating the high symmetry of the guided mode is given.

Transformation of terahertz spectra emitted from dual-frequency femtosecond pulse interaction in gases

We demonstrate that the two basic physical mechanisms of terahertz (THz) generation in a femtosecond filament, namely, the free electron photocurrent and the nonlinear polarization of neutrals, can be identified through the spectral analysis of THz radiation. The contribution from the photocurrent peaks at the units of THz, while the neutrals yield the peak at the tens of THz. We suggest the practical implementation of such spectral analysis by varying the initial transform-limited laser pulse duration.

Interaction of femtosecond pulses of p-polarised radiation with a rapidly heated metal

The effects of rapid nonuniform heating of electrons on reflection of a p-polarised pulse from the metal are quantitatively described. Under conditions of normal and high-frequency skin effects, the absorption coefficient and phase shift of the reflected wave are calculated numerically upon irradiation of a gold target.