Frequency down-conversion based on optical cascading process-New effective way for generation of far infrared or THz radiation.

Infrared and THz optics has many promising practical applications such as in spectroscopy, diagnostic, optical metrology, sensing, and many others. Due to limited number of IR radiation sources, the frequency down-conversion processes are widely used for obtaining infrared radiation. Among them, the most applicable method is a generation of wave with difference frequency under the three-waves interaction in a medium with quadratic nonlinear response. Below we propose a new effective tool for three times decreasing frequency of the incident pulse based on three-waves interaction in a medium with the quadratic susceptibility. At such interaction, a medium's response inherent cubic non-linearity appears due to so-called cascading SHG. The frequency down-conversion process possesses two stable modes. This is shown using multi-scale method. For each of the modes, the analytical solution is developed in the framework of the long pulse duration approximation without using the pump energy non-depletion approximation. The computer simulation results confirm those of analytical analysis. We show that the conversion efficiency of the incidentpump pulse energy achieves about 70%, if the low frequency wave incident intensity equals zero, or almost 100%, if the incident intensity of the low frequency wave is non-zero. The developed theoretical approach may be applied to other processes of the frequency down-conversion.

Spurious Absorption Frequency Appearance Due to Frequency Conversion Processes in Pulsed THz TDS Problems.

The appearance of the spurious absorption frequencies caused by the frequency conversion process at the broadband THz pulse propagation in a medium is theoretically and experimentally discussed. The spurious absorption frequencies appear due to both the frequency doubling and generation of waves with sum or difference frequency. Such generation might occur because of the nonlinear response of a medium or its non-instantaneous response. This phenomenon is confirmed by the results of a few physical experiments provided with the THz CW signals and broadband THz pulses that are transmitted through the ordinary or dangerous substances. A high correlation between the time-dependent spectral intensities for the basic frequency and generated frequencies is demonstrated while using the computer simulation results. This feature of the frequency conversion might be used for the detection and identification of a substance.

Generalized nonlinear Schrödinger equations describing the Second Harmonic Generation of femtosecond pulse, containing a few cycles, and their integrals of motion.

An interaction of laser pulse, containing a few cycles, with substance is a modern problem, attracting attention of many researches. The frequency conversion is a key problem for a generation of such pulses in various ranges of frequencies. Adequate description of such pulse interaction with a medium is based on a slowly evolving wave approximation (SEWA), which has been proposed earlier for a description of propagation of the laser pulse, containing a few cycles, in a medium with cubic nonlinear response. Despite widely applicability of the frequency conversion for various nonlinear optics problems solutions, SEWA has not been applied and developed for a theoretical investigation of the frequency doubling process until present time. In this study the set of generalized nonlinear Schrödinger equations describing a second harmonic generation of the super-short femtosecond pulse is derived. The equations set contains terms, describing the pulses self-steepening, and the second order dispersion (SOD) of the pulse, a diffraction of the beam as well as mixed derivatives. We propose the transform of the equations set to a type, which does not contain both the mixed derivatives and time derivatives of the nonlinear terms. This transform allows us to derive the integrals of motion of the problem: energy, spectral invariants and Hamiltonian. We show the existence of two specific frequencies (singularities in the Fourier space) inherent to the problem. They may cause an appearance of non-physical absolute instability of the problem solution if the spectral invariants are not taken into account. Moreover, we claim that the energy preservation at the laser pulses propagation may not occur if these invariants do not preserve. Developed conservation laws, in particular, have to be used for developing of the conservative finite-difference schemes, preserving the conservation laws difference analogues, and for developing of adequate theory of the modulation instability of the laser pulses, containing a few cycles.

A Possible Way for the Detection and Identification of Dangerous Substances in Ternary Mixtures Using THz Pulsed Spectroscopy.

We discuss an effective tool for the detection and identification of substances in ternary mixtures with similar spectral properties using a broadband reflected THz signal. Nowadays, this is an urgent problem; its effective solution is still far off. Two ternary mixtures of the explosives (RDX+TNT+HMX and RDX+TNT+PETN) were used as the examples for demonstration of the efficiency of the method proposed. The identification is based on the pulsed THz spectroscopy. We follow the spectral intensities together with the use of integral correlation criteria. They use the spectral line dynamics of the THz pulse reflected from the substance under investigation and that of the standard THz signal from database. In order to increase the accuracy and reliability of the identification, we analyze the partial non-overlapping time intervals, containing the main pulse of the reflected THz signal and the sequential sub-pulses. The main pulse is shown to contain information about high absorption frequencies (ν > 2.6 THz) of the mixture components. In the sub-pulses, the absorption frequencies of the components are detected in the range of low (ν < 2.6 THz) and high (ν > 2.6 THz) frequencies. The opportunity of distinguishing the mixtures with similar spectral properties is also shown.

Implicit finite-difference schemes, based on the Rosenbrock method, for nonlinear Schrödinger equation with artificial boundary conditions.

We investigate the effectiveness of using the Rosenbrock method for numerical solution of 1D nonlinear Schrödinger equation (or the set of equations) with artificial boundary conditions (ABCs). We compare the computer simulation results obtained during long time interval at using the finite-difference scheme based on the Rosenbrock method and at using the conservative finite-difference scheme. We show, that the finite-difference scheme based on the Rosenbrock method is conditionally conservative one. To combine the advantages of both numerical methods, we propose new implicit and conditionally conservative combined method based on using both the conservative finite-difference scheme and conditionally conservative Rosenbrock method and investigate its effectiveness. The combined method allows decreasing the computer simulation time in comparison with the corresponding computer simulation time at using the Rosenbrock method. In practice, the combined method is effective at computation during short time interval, which does not require an asymptotic stability property for the finite-difference scheme. We generalize also the combined method with ABCs for 2D case.

Conservative finite-difference scheme for the problem of THz pulse interaction with multilevel layer covered by disordered structure based on the density matrix formalism and 1D Maxwell's equation.

On the basis of the Crank-Nicolson method, we develop a conservative finite-difference scheme for investigation of the THz pulse interaction with a multilevel medium, covered by a disordered layered structure, in the framework of the Maxwell-Bloch equations, describing the substance evolution and the electromagnetic field evolution. For this set of the partial differential equations, the conservation laws are derived and proved. We generalize the Bloch invariant with respect to the multilevel medium. The approximation order of the developed finite-difference scheme is investigated and its conservatism property is also proved. To solve the difference equations, which are nonlinear with respect to the electric field strength, we propose an iteration method and its convergence is proved. To increase the computer simulation efficiency, we use the well-known solution of Maxwell's equations in 1D case as artificial boundary condition. It is approximated using Cabaret scheme with the second order of an accuracy. On the basis of developed finite-difference scheme, we investigate the broadband THz pulse interaction with a medium covered by a disordered structure. This problem is of interest for the substance detection and identification. We show that the disordered structure dramatically induces an appearance of the substance false absorption frequencies. We demonstrate also that the spectrum for the transmitted and reflected pulses becomes broader due to the cascade mechanism of the high energy levels excitation of molecules. It leads to the substance emission at the frequencies, which are far from the frequency range for the incident pulse spectrum. Time-dependent spectral intensities at these frequencies are weakly disturbed by the disordered cover and, hence, they can be used for the substance identification.

High effective time-dependent THz spectroscopy method for the detection and identification of substances with inhomogeneous surface.

We discuss an effective time-dependent THz spectroscopy method for the detection and identification of a substance with an inhomogeneous surface using a broadband THz signal reflected from the substance. We show that a successful and reliable identification can be made using the single long-duration THz signal, which contains not only the main reflected pulse, but also several sub-pulses. The method does not use averaging of the measured THz signals over the viewing angles and scanning over the surface area, which significantly increases the signal processing speed. The identification is based on the method of spectral dynamics analysis together with the integral correlation criteria (ICC). We compare the absorption spectral dynamics of a substance under analysis with the corresponding dynamics for a standard substance from database. For reliable and effective substance detection, we propose to use several ICC simultaneously in different time intervals, which contain not only the main pulse of the reflected THz signal, but also the sub-pulses. This way, one can detect and identify the substance in the sample with high probability. As examples of identification, we used the THz signals reflected from the plastic explosive PWM C4 with both rough and concave surface. We show that the main pulse, reflected from the inhomogeneous surface of the sample, contains information about its absorption frequencies.

Aberrated surface soliton formation in a nonlinear 1D and 2D photonic crystal.

We discuss a novel type of surface soliton-aberrated surface soliton-appearance in a nonlinear one dimensional photonic crystal and a possibility of this surface soliton formation in two dimensional photonic crystal. An aberrated surface soliton possesses a nonlinear distribution of the wavefront. We show that, in one dimensional photonic crystal, the surface soliton is formed at the photonic crystal boundary with the ambient medium. Essentially, that it occupies several layers at the photonic crystal boundary and penetrates into the ambient medium at a distance also equal to several layers, so that one can infer about light energy localization at the lateral surface of the photonic crystal. In the one dimensional case, the surface soliton is formed from an earlier formed soliton that falls along the photonic crystal layers at an angle which differs slightly from the normal to the photonic crystal face. In the two dimensional case, the soliton can appear if an incident Gaussian beam falls on the photonic crystal face. The influence of laser radiation parameters, optical properties of photonic crystal layers and ambient medium on the one dimensional surface soliton formation is investigated. We also discuss the influence of two dimensional photonic crystal configuration on light energy localization near the photonic crystal surface. It is important that aberrated surface solitons can be created at relatively low laser pulse intensity and for close values of alternating layers dielectric permittivity which allows their experimental observation.

The Anomalous Influence of Spectral Resolution on Pulsed THz Time Domain Spectroscopy under Real Conditions.

We have studied the spectral resolution influence on the accuracy of the substance detection and identification at using a broadband THz pulse measured under real conditions (at a distance of more than 3 m from a THz emitter in ambient air with a relative humidity of about 50%). We show that increasing spectral resolution leads to manifestation of small-scale perturbations (random fluctuations) in the signal spectrum caused by the influence of the environment or the sample structure. Decreasing the spectral resolution allows us to exclude from consideration this small-scale modulation of the signal as well as to detect the water vapor absorption frequencies. This fact is important in practice because it allows us to increase the signal processing rate. In order to increase the detection reliability, it is advisable to decrease the spectral resolution up to values of not more than 40% of the corresponding spectral line bandwidth. The method of spectral dynamics analysis together with the integral correlation criteria is used for the substance detection and identification. Neutral substances such as chocolate and cookies are used as the samples in the physical experiment.

New Possibilities of Substance Identification Based on THz Time Domain Spectroscopy Using a Cascade Mechanism of High Energy Level Excitation.

Using an experiment with thin paper layers and computer simulation, we demonstrate the principal limitations of standard Time Domain Spectroscopy (TDS) based on using a broadband THz pulse for the detection and identification of a substance placed inside a disordered structure. We demonstrate the spectrum broadening of both transmitted and reflected pulses due to the cascade mechanism of the high energy level excitation considering, for example, a three-energy level medium. The pulse spectrum in the range of high frequencies remains undisturbed in the presence of a disordered structure. To avoid false absorption frequencies detection, we apply the spectral dynamics analysis method (SDA-method) together with certain integral correlation criteria (ICC).

Detection and identification of drugs under real conditions by using noisy terahertz broadband pulse.

We discuss an effective method for detecting and identifying drugs using a high-noise terahertz (THz) signal. We add a noisy THz signal obtained in real conditions to the THz signal transmitted through a sample with the illicit drug methamphetamine. The insufficiency of the standard THz time-domain spectroscopy method is demonstrated, showing that this method detects the spectral features of neutral substances and explosives in a noisy THz signal. The method discussed is based upon time-dependent integral correlation criteria calculated using spectral dynamics of the medium response. We propose a modification of the integral correlation criterion that is less dependent on the spectral characteristics of a noisy signal under investigation.

Essential Limitations of the Standard THz TDS Method for Substance Detection and Identification and a Way of Overcoming Them.

Low efficiency of the standard THz TDS method of the detection and identification of substances based on a comparison of the spectrum for the signal under investigation with a standard signal spectrum is demonstrated using the physical experiments conducted under real conditions with a thick paper bag as well as with Si-based semiconductors under laboratory conditions. In fact, standard THz spectroscopy leads to false detection of hazardous substances in neutral samples, which do not contain them. This disadvantage of the THz TDS method can be overcome by using time-dependent THz pulse spectrum analysis. For a quality assessment of the standard substance spectral features presence in the signal under analysis, one may use time-dependent integral correlation criteria.

An effective method for substance detection using the broad spectrum THz signal with a "terahertz nose".

We propose an effective method for the detection and identification of dangerous substances by using the broadband THz pulse. This pulse excites, for example, many vibrational or rotational energy levels of molecules simultaneously. By analyzing the time-dependent spectrum of the THz pulse transmitted through or reflected from a substance, we follow the average response spectrum dynamics. Comparing the absorption and emission spectrum dynamics of a substance under analysis with the corresponding data for a standard substance, one can detect and identify the substance under real conditions taking into account the influence of packing material, water vapor and substance surface. For quality assessment of the standard substance detection in the signal under analysis, we propose time-dependent integral correlation criteria. Restrictions of usually used detection and identification methods, based on a comparison between the absorption frequencies of a substance under analysis and a standard substance, are demonstrated using a physical experiment with paper napkins.

Asymmetric femtosecond laser ablation of silicon surface governed by the evolution of surface nanostructures.

The femtosecond laser ablation of silicon surface near the ablation threshold was investigated and the preferential ablation along different directions was observed in different stages. It was found that the ripples formed in the initial stage facilitate the ablation along the direction perpendicular to the ripples, leading to the formation of an elliptical ablation area. With increasing length and depth of the ripples, however, nanohole arrays formed in the ripples will modify the distribution of electric field which benefits the ablation along the direction parallel to the ripples. Consequently, the ablation area is gradually changed to a circular one after irradiating sufficient number of pulses.

Size dependent competition between second harmonic generation and two-photon luminescence observed in gold nanoparticles.

We investigate systematically the competition between the second harmonic generation (SHG) and two-photon-induced luminescence (TPL) that are simultaneously present in Au nanoparticles excited by using a femtosecond (fs) laser. For a large-sized (length ~ 800 nm, diameter ~ 200 nm) Au nanorod, the SHG appears to be much stronger than the TPL. However, the situation is completely reversed when the Au nanorod is fragmented into many Au nanoparticles by the fs laser. In sharp contrast, only the TPL is observed in small-sized (length ~ 40 nm, diameter ~ 10 nm) Au nanorods. When a number of the small-sized Au nanorods are optically trapped and fused into a large-sized Au cluster by focused fs laser light, the strong TPL is reduced while the weak SHG increases significantly. In both cases, the morphology change is characterized by scanning electron microscope. In addition, the modification of the scattering and absorption cross sections due to the morphology change is calculated by using the discrete dipole approximation method. It is revealed that SHG is dominant in the case when the scattering is much larger than the absorption. When the absorption becomes comparable to or larger than the scattering, the TPL increases dramatically and will eventually become dominant. Since the relative strengths of scattering and absorption depend strongly on the size of the Au nanoparticles, the competition between SHG and TPL is found to be size dependent.

Role of interfering optical fields in the trapping and melting of gold nanorods and related clusters.

We investigate the simultaneous trapping and melting of a large number of gold (Au) nanorods by using a single focused laser beam at 800 nm which is in resonance with the longitudinal surface plasmon resonance of Au nanorods. The trapping and melting processes were monitored by the two-photon luminescence of Au nanorods. A multi-ring-shaped pattern was observed in the steady state of the trapping process. In addition, optical trapping of clusters of Au nanorods in the orbits circling the focus was observed. The morphology of the structure after trapping and melting of Au nanorods was characterized by scanning electron microscope. It was revealed that Au nanorods were selectively melted in the trapping region. While Au nanorods distributed in the dark rings were completely melted, those located in the bright rings remain unmelted. The multi-ring-shaped pattern formed by the interference between the incident light and the scattered light plays an important role in the trapping and melting of Au nanorods.

Assembling of three-dimensional crystals by optical depletion force induced by a single focused laser beam.

We proposed a method to assemble microspheres into a three-dimensional crystal by utilizing the giant nonequilibrium depletion force produced by nanoparticles. Such assembling was demonstrated in a colloid formed by suitably mixing silica microspheres and magnetic nanoparticles. The giant nonequilibrium depletion force was generated by quickly driving magnetic nanoparticles out of the focusing region of a laser light through both optical force and thermophoresis. The thermophoretic binding of silica beads is so tight that a colloidal photonic crystal can be achieved after complete evaporation of solvent. This technique could be employed for fabrication of colloidal photonic crystals and molecular sieves.

Colorizing silicon surface with regular nanohole arrays induced by femtosecond laser pulses.

We report on the formation of one- and two-dimensional (1D and 2D) nanohole arrays on the surface of a silicon wafer by scanning with a femtosecond laser with appropriate power and speed. The underlying physical mechanism is revealed by numerical simulation based on the finite-difference time-domain technique. It is found that the length and depth of the initially formed gratings (or ripples) plays a crucial role in the generation of 1D or 2D nanohole arrays. The silicon surface decorated with such nanohole arrays can exhibit vivid structural colors through efficiently diffracting white light.

High spatial frequency periodic structures induced on metal surface by femtosecond laser pulses.

The high spatial frequency periodic structures induced on metal surface by femtosecond laser pulses was investigated experimentally and numerically. It is suggested that the redistribution of the electric field on metal surface caused by the initially formed low spatial frequency periodic structures plays a crucial role in the creation of high spatial frequency periodic structures. The field intensity which is initially localized in the grooves becomes concentrated on the ridges in between the grooves when the depth of the grooves exceeds a critical value, leading to the ablation of the ridges in between the grooves and the formation of high spatial frequency periodic structures. The proposed formation process is supported by both the numerical simulations based on the finite-difference time-domain technique and the experimental results obtained on some metals such as stainless steel and nickel.

Dynamics of optical matter creation and annihilation in colloidal liquids controlled by laser trapping power.

We investigate the dynamics of optical matter creation and annihilation in a colloidal liquid that was employed to construct an all-optical switch. It is revealed that the switching-on process can be characterized by the Fermi-Dirac distribution function, while the switching-off process can be described by a steady state followed by a single exponential decay. The phase transition times exhibit a strong dependence on trapping power. With an increasing trapping power, while the switching-on time decreases rapidly, the switch-off time increases significantly, indicating the effects of optical binding and van der Waals force on the lifetime of the optical matter.