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Showing papers on "High harmonic generation published in 2005"


Journal ArticleDOI
26 May 2005-Nature
TL;DR: Evidence for quantum interference of electron de Broglie waves in the recombination process of HHG from aligned CO2 molecules is reported and it is proposed that simultaneous observations of both ion yields and harmonic signals can serve as a new route to probe the instantaneous structure of molecular systems.
Abstract: High-order harmonic generation (HHG) from atoms and molecules offers potential application as a coherent ultrashort radiation source in the extreme ultraviolet and soft X-ray regions1,2,3. In the three-step model4,5,6 of HHG, an electron tunnels out from the atom and may recombine with the parent ion (emitting a high-energy photon) after undergoing laser-driven motion in the continuum. Aligned molecules7,8,9,10,11 can be used to study quantum phenomena in HHG associated with molecular symmetries; in particular, simultaneous observations of both ion yields and harmonic signals under the same conditions serve to disentangle the contributions from the ionization and recombination processes. Here we report evidence for quantum interference of electron de Broglie waves12,13,14 in the recombination process of HHG from aligned CO2 molecules. The interference takes place within a single molecule and within one optical cycle. Characteristic modulation patterns of the harmonic signals measured as a function of the pump–probe delay are explained with simple formulae determined by the valence orbital of the molecules. We propose that simultaneous observations of both ion yields and harmonic signals can serve as a new route to probe the instantaneous structure of molecular systems.

540 citations


Journal ArticleDOI
14 Jul 2005-Nature
TL;DR: In this paper, the authors demonstrate intra-cavity high harmonic generation in the extreme ultraviolet, which promises to lead to another joint frontier of precision spectroscopy and ultrafast science.
Abstract: Since 1998, the interaction of precision spectroscopy and ultrafast laser science has led to several notable accomplishments. Femtosecond laser optical frequency 'combs' (evenly spaced spectral lines) have revolutionized the measurement of optical frequencies and enabled optical atomic clocks. The same comb techniques have been used to control the waveform of ultrafast laser pulses, which permitted the generation of single attosecond pulses, and have been used in a recently demonstrated 'oscilloscope' for light waves. Here we demonstrate intra-cavity high harmonic generation in the extreme ultraviolet, which promises to lead to another joint frontier of precision spectroscopy and ultrafast science. We have generated coherent extreme ultraviolet radiation at a repetition frequency of more than 100 MHz, a 1,000-fold improvement over previous experiments. At such a repetition rate, the mode spacing of the frequency comb, which is expected to survive the high harmonic generation process, is large enough for high resolution spectroscopy. Additionally, there may be many other applications of such a quasi-continuous compact and coherent extreme ultraviolet source, including extreme ultraviolet holography, microscopy, nanolithography and X-ray atomic clocks.

511 citations


Journal ArticleDOI
TL;DR: Optical-heterodyne-based measurements reveal that the coherent frequency comb structure of the original laser is fully preserved in the high-harmonic generation process and permits the efficient generation of phase-coherent high-order harmonics using only a standard laser oscillator without active amplification of single pulses.
Abstract: We demonstrate the generation of phase-coherent frequency combs in the vacuum utraviolet spectral region. The output from a mode-locked laser is stabilized to a femtosecond enhancement cavity with a gas jet at the intracavity focus. The resulting high-peak power of the intracavity pulse enables efficient high-harmonic generation by utilizing the full repetition rate of the laser. Optical-heterodyne-based measurements reveal that the coherent frequency comb structure of the original laser is fully preserved in the high-harmonic generation process. These results open the door for precision frequency metrology at extreme ultraviolet wavelengths and permit the efficient generation of phase-coherent high-order harmonics using only a standard laser oscillator without active amplification of single pulses.

437 citations


Journal ArticleDOI
TL;DR: In this article, a femtosecond Ti:sapphire laser was used for high-harmonic generation in helium using a two-color laser field that consisted of the fundamental and second harmonic fields of a femto-cond Ti-sappire laser.
Abstract: Highly efficient high-harmonic generation was achieved in helium using a two-color laser field that consisted of the fundamental and the second harmonic fields of a femtosecond Ti:sapphire laser. By applying a high intensity second harmonic, the harmonics generated in the orthogonally polarized two-color field were stronger than those obtained in the fundamental field by more than 2 orders of magnitude, and even stronger than those of the parallel polarization case. A conversion efficiency as high as $5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}5}$ was obtained for the 38th harmonic at 21.6 nm. The physical origin of this enhancement was deduced by analyzing the electron behavior in the two-color field.

332 citations


Journal ArticleDOI
TL;DR: It is demonstrated that interference effects in high-order harmonic generation in impulsively aligned CO2 molecules can be effectively controlled by changing the ellipticity of the driving laser field.
Abstract: We experimentally investigate the process of intramolecular quantum interference in high-order harmonic generation in impulsively aligned CO2 molecules. The recombination interference effect is clearly seen through the order dependence of the harmonic yield in an aligned sample. The experimental results can be well modeled assuming that the effective de Broglie wavelength of the returning electron wave is not significantly altered by the Coulomb field of the molecular ion. We demonstrate that such interference effects can be effectively controlled by changing the ellipticity of the driving laser field.

279 citations


Journal ArticleDOI
TL;DR: In this paper, the authors present a consistent S-matrix formulation of the quantum amplitude for high harmonic generation (HHG) and point out some of the most general properties of HHG radiation emitted by a single atom as well as its relation to coherent emission from many atoms.
Abstract: Intense-field many-body S-matrix theory (IMST) provides a systematic ab initio approach to investigate the dynamics of atoms and molecules interacting with intense laser radiation. We review the derivation of IMST as well as its diagrammatic representation and point out its advantage over the conventional 'prior' and 'post' expansions which are shown to be special cases of IMST. The practicality and usefulness of the theory is illustrated by its application to a number of current problems of atomic and molecular ionization in intense fields. We also present a consistent S-matrix formulation of the quantum amplitude for high harmonic generation (HHG) and point out some of the most general properties of HHG radiation emitted by a single atom as well as its relation to coherent emission from many atoms. Experimental results for single and double (multiple) ionization of atoms and the observed distributions of coincidence measurements are analysed and the dominant mechanisms behind them are discussed. Ionization of more complex systems such as diatomic and polyatomic molecules in intense laser fields is analysed as well using IMST and the results are discussed with special attention to the role of molecular orbital symmetry and molecular orientation in space. The review ends with a summary and a brief outlook.

265 citations


Journal ArticleDOI
Manfred Lein1
TL;DR: The numerical solution of the time-dependent Schrodinger equation for vibrating hydrogen molecules in few-cycle laser pulses shows that high-harmonic generation is sensitive to the laser-induced vibrational motion.
Abstract: The numerical solution of the time-dependent Schrodinger equation for vibrating hydrogen molecules in few-cycle laser pulses shows that high-harmonic generation is sensitive to the laser-induced vibrational motion. More intense harmonics are generated in heavier isotopes, the difference increasing with the harmonic frequency. Analytical theory reveals a dependence of the harmonics on the vibrational autocorrelation function. With the help of a genetic algorithm, the nuclear motion can be reconstructed from the harmonic spectra with sub-fs time resolution.

252 citations


Journal ArticleDOI
TL;DR: It is shown that, by controlling the alignment of molecules, it is possible to influence the high harmonic generation process by observing strong intensity modulation and spectral shaping of high harmonics produced with a rotational wave packet in a low-density gas.
Abstract: We show that, by controlling the alignment of molecules, we can influence the high harmonic generation process. We observed strong intensity modulation and spectral shaping of high harmonics produced with a rotational wave packet in a low-density gas of N2 or O2. In N2, where the highest occupied molecular orbital (HOMO) has sigma(g) symmetry, the maximum signal occurs when the molecules are aligned along the laser polarization while the minimum occurs when it is perpendicular. In O2, where the HOMO has pi(g) symmetry, the harmonics are enhanced when the molecules are aligned around 45 degrees to the laser polarization. The symmetry of the molecular orbital can be read by harmonics. Molecular wave packets offer a means of shaping attosecond pulses.

202 citations


Journal ArticleDOI
TL;DR: In this article, the authors report the short-pulse operation of a 460 GHz gyrotron oscillator both at the fundamental (near 230 GHz) and second harmonic (near 460 GHz) of electron cyclotron resonance.
Abstract: We report the short-pulse operation of a 460 GHz gyrotron oscillator both at the fundamental (near 230 GHz) and second harmonic (near 460 GHz) of electron cyclotron resonance. During operation in a microsecond pulse length regime with 13-kV beam voltage and 110-mA beam current, the instrument generates several watts of power in two second harmonic modes, the TE/sub 2,6,1/ at 456.15 GHz and the TE/sub 0,6,1/ at 458.56 GHz. Operation in the fundamental modes, including the TE/sub 0,3,1/ mode at 237.91 GHz and the TE/sub 2,3,1/ at 233.15 GHz, is observed at output powers up to 70 W. Further, we demonstrate broadband continuous frequency tuning of the fundamental modes of the oscillator over a range of more than 2 GHz through variation of the magnetic field alone. We interpret these results in terms of smooth transitions between higher order axial modes of the resonator. The 460 GHz gyrotron is currently being processed for continuous duty operation, where it will serve as a microwave source for sensitivity-enhanced nuclear magnetic resonance (dynamic nuclear polarization) studies at 16 T (700 MHz /sup 1/H), a field strength which is two-fold higher than has been accessible with previous technology.

201 citations


Journal ArticleDOI
TL;DR: In this paper, the phase of the atomic polarization in the process of high-order harmonic generation is studied and its dependence on the laser intensity and the harmonic order induce a frequency variation in time (chirp) respectively of the harmonic pulses and attosecond pulses.
Abstract: We study the phase of the atomic polarization in the process of high-order harmonic generation. Its dependence on the laser intensity and the harmonic order induce a frequency variation in time (chirp) respectively of the harmonic pulses and attosecond pulses. We review the recent experimental results on the temporal characterization of the harmonic emission and show that measurements performed using very different techniques (like XFROG and RABITT), probing the phase in different parameter spaces, can be connected through the mixed phase derivatives, demonstrating the common underlying physics.

146 citations


Journal ArticleDOI
TL;DR: In this article, the authors used the Prolate Spheroidal coordinate system (PSCG) and expanded the time-dependent wave function in a complex basis of Laguerre polynomials and Legendre functions.
Abstract: We describe a numerical method used previously [Phys. Rev. A 70, 011404(R) (2004)] for solving the three-dimensional time-dependent Schr\"odinger equation for ${\mathrm{H}}_{2}^{+}$ (with fixed nuclei) in interaction with an intense, arbitrary oriented laser pulse. In this approach, we use the prolate spheroidal coordinate system, and expand the time-dependent wave function in a complex basis of Laguerre polynomials and Legendre functions. Our results indicate that ionization, excitation, and harmonic generation are strongly influenced by the orientation of the molecular axis with respect to the laser polarization axis. We evaluate the contribution of each nucleus to harmonic generation, as this permits a quantitative and nonambiguous assessment of interference effects as a function of molecular orientation. A time-profile analysis, using a Gabor transform of the harmonic spectrum around certain harmonics, shows that every half-cycle high-order harmonics are emitted by each nucleus when the electron wave packet returns for a recollision with the molecular core, thus confirming the strong field recollision model in molecules. In general, each nucleus emits both odd and even harmonics, but even harmonics are destroyed by interferences between contributions of each nucleus. These interferences are shown to be maximum at certain harmonic orders as a function of molecular orientation. A comparison of acceleration and dipole formulations of the harmonic emission process is made in order to assess the use of high-order harmonic generation for electron wave-function imaging.

Journal ArticleDOI
TL;DR: In this article, a fast ion-beam irradiation procedure based on electronic (not nuclear) excitation was used to generate a large index jump step-like optical waveguide (Δn0≈0.2,Δne≈ 0.1) in LiNbO3.
Abstract: We demonstrate a swift ion-beam irradiation procedure based on electronic (not nuclear) excitation to generate a large index jump step-like optical waveguide (Δn0≈0.2,Δne≈0.1) in LiNbO3. The method uses medium-mass ions with a kinetic energy high enough to assure that their electronic stopping power Se(z) reaches a maximum value close to the amorphous (latent) track threshold inside the crystal. Fluorine ions of 20 and 22MeV and fluences in the range (1–30)×1014 are used for this work. A buried amorphous layer having a low refractive index (2.10 at a wavelength of 633nm) is then generated at a controlled depth in LiNbO3, whose thickness is also tuned by irradiation fluence. The layer left at the surface remains crystalline and constitutes the core of the optical waveguide which, moreover, is several microns far from the end of the ion range. The waveguides show, after annealing at 300°C, low propagation losses (≈1dB∕cm) and a high second-harmonic generation coefficient (50%–80% of that for bulk unirradiat...

Journal ArticleDOI
TL;DR: A rigorous theory of third-harmonic generation in optical waveguides is introduced and applied to design a micro-fiber waveguide for efficient generation of third -harmonic radiation from infrared lasers.
Abstract: We introduce a rigorous theory of third-harmonic generation in optical waveguides and apply it to design a micro-fiber waveguide for efficient generation of third-harmonic radiation from infrared lasers. Phase-matching with efficient mode overlap is achieved in micro-fibers having a diameter roughly equal to half of the fundamental wavelength. Using a typical solid-state or fiber laser for pumping, high conversion efficiency is possible in only a few centimeters of a micro-fiber.

Journal ArticleDOI
TL;DR: In this paper, the authors studied the generation of up to the 57th harmonic (λ = 13.96 nm) of a Ti:sapphire laser radiation from the prepulse produced silver plasma.

Journal ArticleDOI
TL;DR: This work proposes a chirp excitation method for contrast agents using the second harmonic component of the response based on a compression filter that selectively compresses and extracts thesecond harmonic component from the received echo signal.
Abstract: Coded excitation is currently used in medical ultrasound to increase signal-to-noise ratio (SNR) and penetration depth. We propose a chirp excitation method for contrast agents using the second harmonic component of the response. This method is based on a compression filter that selectively compresses and extracts the second harmonic component from the received echo signal. Simulations have shown a clear increase in response for chirp excitation over pulse excitation with the same peak amplitude. This was confirmed by two-dimensional (2-D) optical observations of bubble response with a fast framing camera. To evaluate the harmonic compression method, we applied it to simulated bubble echoes, to measured propagation harmonics, and to B-mode scans of a flow phantom and compared it to regular pulse excitation imaging. An increase of approximately 10 dB in SNR was found for chirp excitation. The compression method was found to perform well in terms of resolution. Axial resolution was in all cases within 10% of the axial resolution from pulse excitation. Range side-lobe levels were 30 dB below the main lobe for the simulated bubble echoes and measured propagation harmonics. However, side-lobes were visible in the B-mode contrast images.

Journal ArticleDOI
TL;DR: In this article, the cross sections of the two-photon double ionization and above-threshold ionization in the soft-x-ray region were estimated based on the measured time-of-flight spectra for both ions and electrons obtained using intense soft x-ray pulses produced by high-order harmonics.
Abstract: We report on the multiphoton ionization processes in the soft-x-ray region $(\ensuremath{\lambda}\ensuremath{\leqslant}30\phantom{\rule{0.3em}{0ex}}\mathrm{nm})$. On the basis of the measured time-of-flight spectra for both ions and electrons obtained using intense soft-x-ray pulses produced by high-order harmonics, the cross sections of the two-photon double ionization and above-threshold ionization of $\mathrm{He}$ are estimated. The high-intensity soft-x-ray radiation achieved by phase-matched high-order harmonics enables the investigation of these nonlinear optical processes, which were beyond the reach of conventional light sources.

Journal ArticleDOI
TL;DR: In this paper, the authors investigated high-order harmonic generation in argon driven by 25-fs-light pulses from the gaseous to the cluster regime, showing the existence of an optimal cluster dimension, which maximizes the harmonic photon yield.
Abstract: High-order harmonic generation in argon driven by 25-fs-light pulses is investigated from the gaseous to the cluster regime. The harmonic cutoff observed in presence of clusters shows a considerable extension with respect to the gaseous phase. Harmonic spectra are investigated as a function of cluster size, showing the existence of an optimal cluster dimension, which maximizes the harmonic photon yield.

Journal ArticleDOI
TL;DR: Harmonic generation appeared to be efficient for the plasma that comprised neutral atoms and singly ionized boron as the nonlinear medium.
Abstract: We demonstrate the generation of up to the 63rd harmonic (?=12.6?nm) of a Ti:sapphire laser pulse (150?fs,10?mJ), using a prepulse- (210-ps,24-mJ) produced boron plasma as the nonlinear medium. The influence of various parameters on the harmonic conversion efficiency was analyzed. The steep decrease in intensity for low-order harmonics (up to 19th order) was followed by a plateau. Typical conversion efficiencies were evaluated to be 10?4 (for a 3rd harmonic) to 10?7 (within the plateau region). Harmonic generation appeared to be efficient for the plasma that comprised neutral atoms and singly ionized boron.

Journal ArticleDOI
TL;DR: The long-range propagation of two-colored femtosecond filaments produced by an infrared (IR) ultrashort pulse exciting third harmonics (TH) in the atmosphere is investigated, both theoretically and experimentally, and it is shown that the coupling between the pump and TH components is responsible for a wide spectral broadening.
Abstract: The long-range propagation of two-colored femtosecond filaments produced by an infrared (IR) ultrashort pulse exciting third harmonics (TH) in the atmosphere is investigated, both theoretically and experimentally. First, it is shown that the coupling between the pump and TH components is responsible for a wide spectral broadening, extending from ultraviolet (UV) wavelengths (220 nm) to the mid-IR (4.5 microm). Supercontinuum generation takes place continuously as the laser beam propagates, while TH emission occurs with a conversion efficiency as high as 0.5%. Second, the TH pulse is proven to stabilize the IR filament like a saturable quintic nonlinearity through four-wave mixing and cross-phase modulation. Third, the filamentation is accompanied by a conical emission of the beam, which becomes enlarged at UV wavelengths. These properties are revealed by numerical simulations and direct experimental observations performed from the Teramobile laser facility.

Journal ArticleDOI
TL;DR: This work demonstrates the first experimental complete temporal characterization of high-harmonic XUV pulses by spectral phase interferometry, with an all-optical setup, revealing a remarkable shot-to-shot stability.
Abstract: We demonstrate the first experimental complete temporal characterization of high-harmonic XUV pulses by spectral phase interferometry, with an all-optical setup. This method allows us to perform single-shot measurements of the harmonic temporal profile and phase, revealing a remarkable shot-to-shot stability. We characterize harmonics generated in argon by a 50 fs 800 nm laser pulse. The 11th harmonic is found to be 22 fs long with a negative chirp rate of $\ensuremath{-}4.8\ifmmode\times\else\texttimes\fi{}{10}^{27}\text{ }\text{ }{\mathrm{s}}^{\ensuremath{-}2}$. This duration can be reduced to 13 fs by modulating the polarization of the generating laser. The technique is easy to implement and could be routinely used in femtosecond XUV pump-probe experiments with harmonics.

Journal ArticleDOI
Kenzo Miyazaki1, M. Kaku, Godai Miyaji, A. Abdurrouf, Farhard Faisal 
TL;DR: High-order harmonic generation is demonstrated to provide a sensitive way for an extensive study of dynamic processes in the field-free alignment of strong-field-induced molecular rotational wave packets.
Abstract: High-order harmonic generation is demonstrated to provide a sensitive way for an extensive study of dynamic processes in the field-free alignment of strong-field-induced molecular rotational wave packets. The time-dependent harmonic signal observed from field-free-aligned N2, O2, and CO2 has been found to include two sets of beat frequency for pairs of coherently populated rotational states. One of them is the well-known frequency component characterizing the field-free alignment of molecules, and the other is ascribed to the beat that arises from coherence embedded in the wave packet. We discuss the effect of each frequency component on the revival signal observed with the harmonic generation.

Journal ArticleDOI
17 Jan 2005
TL;DR: In this article, the authors introduce nonlinear transmission lines based on left-handed (LH) media and simulates harmonic generation and parametric generation in a material that, in two dimensions, could also focus microwaves.
Abstract: This paper introduces nonlinear transmission lines based on left-handed (LH) media and simulates harmonic generation and parametric generation in a material that, in two dimensions, could also focus microwaves. This paper discusses physical phenomena that lead to and affect self-supporting harmonic generation and parametric generation in LH nonlinear transmission-line media and outline advantages of these media for developing new types of compact and efficient frequency multipliers and "active lens" devices.

Journal ArticleDOI
TL;DR: It is demonstrated that multilayer extreme-ultraviolet chirped mirrors can be numerically optimized and designed to compensate for the intrinsic harmonic chirp that was recently discovered and that is responsible for temporal broadening of pulses.
Abstract: In the race toward attosecond pulses, for which high-order harmonics generated in rare gases are the best candidates, both the harmonic spectral range and the spectral phase have to be controlled. We demonstrate that multilayer extreme-ultraviolet chirped mirrors can be numerically optimized and designed to compensate for the intrinsic harmonic chirp that was recently discovered and that is responsible for temporal broadening of pulses. A simulation shows that an optimized mirror is capable of compressing the duration from ?260to90?as. This new technique is an interesting solution because of its ability to cover a wider spectral range than other technical devices that have already been proposed to overcome the chirp of high harmonics.

Journal ArticleDOI
TL;DR: In this article, the first demonstration of extreme ultraviolet (XUV) supercontinuum generation in the plateau region of the high-order harmonic spectrum indicative of a single attosecond pulse was reported.
Abstract: We report the first demonstration of extreme ultraviolet (XUV) supercontinuum generation in the plateau region of the high-order harmonic spectrum indicative of a single attosecond pulse. It was accomplished by combining the generation of sub-10 fs laser pulses with the polarization gating of high harmonic generation. When an 8 fs pulse centred at 750 nm was split and delayed with a quartz plate and then recombined with a quarter waveplate, a laser pulse was created whose polarization varied rapidly from circular to linear and back to circular. The near-linearly polarized portion of the resultant pulse was only 1.3 fs long, which was much shorter than the laser pulse duration. Since the high-order harmonic generation process is susceptible to the ellipticity of the driving field, the pulse with a time-dependent ellipticity behaved like a half-cycle linearly polarized pulse for generating XUV radiation. By exciting argon gas with the pulse, a supercontinuum that covered 25–45 nm was produced, which corresp...

Journal ArticleDOI
TL;DR: In this article, the linear and nonlinear-optical lineshapes of metal nanoparticles and metallic photonic crystal slabs were analyzed analytically and numerically for femtosecond second-or third-harmonic-generation (THG) experiments together with linear extinction measurements.
Abstract: We study the linear- and nonlinear-optical lineshapes of metal nanoparticles (theory) and metallic photonic crystal slabs (experiment and theory). For metal nanoparticle ensembles, we show analytically and numerically that femtosecond second- or third-harmonic-generation (THG) experiments together with linear extinction measurements generally do not allow to determine the homogeneous linewidth. This is in contrast to claims of previous work in which we identify a technical mistake. For metallic photonic crystal slabs, we introduce a simple classical model of two coupled Lorentz oscillators, corresponding to the plasmon and waveguide modes. This model describes very well the key experimental features of linear optics, particularly the Fano-like lineshapes. The derived nonlinear-optical THG spectra are shown to depend on the underlying source of the optical nonlinearity. We present corresponding THG experiments with metallic photonic crystal slabs. In contrast to previous work, we spectrally resolve the interferometric THG signal, and we additionally obtain a higher temporal resolution by using 5 fs laser pulses. In the THG spectra, the distinct spectral components exhibit strongly different behaviors versus time delay. The measured spectra agree well with the model calculations.

Journal ArticleDOI
TL;DR: In this paper, the authors demonstrate the generation of arbitrarily shaped spectra of coherent soft X-ray radiation by adaptive control of the driving laser pulse by selecting both narrow and wide spectral ranges as well as suppression of high-harmonic emission in a selected wavelength region.
Abstract: We demonstrate the generation of arbitrarily shaped spectra of coherent soft X-ray radiation by adaptive control of the driving laser pulse. The selection of both narrow and wide spectral ranges as well as suppression of high-harmonic emission in a selected wavelength region is achieved. Feedback-controlled spectral engineering of coherent soft X-rays paves the way to shaping of soft X-ray pulses and coherent control of electron dynamics in the sub-femtosecond regime.

Journal ArticleDOI
TL;DR: In this article, the angular dependence of the yields of high-order harmonic generation from aligned molecules is investigated, which can be attributed to the orbital symmetry of the outmost electrons.
Abstract: The strong field approximation is used to investigate the harmonic generation of aligned ${\mathrm{N}}_{2}$ and ${\mathrm{O}}_{2}$ molecules. It is shown that the angular dependence of the yields of high-order harmonic generation from ${\mathrm{N}}_{2}$ and ${\mathrm{O}}_{2}$ molecules are different, which can be attributed to the orbital symmetry of the outmost electrons. The theory is applied to study the angular dependence of harmonic generation from recent pump-probe experiments where the pump pulse was used to produce the time-dependent partial alignment of molecules and the probe pulse was used to generate high-order harmonics. Good agreement with the experiments was found.

Journal ArticleDOI
TL;DR: In this article, the derivation of semianalytical expressions providing the most significant aspects of the high-gain free-electron laser dynamics is considered, and new expressions for the growth of the laser power, of the e-beam-induced energy spread, and of the higher-order nonlinearly generated harmonics are derived.
Abstract: We reconsider the derivation of semianalytical expressions providing the most significant aspects of the high-gain free-electron laser dynamics. We obtain new expressions for the growth of the laser power, of the e-beam-induced energy spread, and of the higher-order nonlinearly generated harmonics. The procedure we employ, based on theoretical ansatz and fitting methods, allows the determination of crucial quantities like the expected harmonic output power and its dependences on the e-beam parameters.

Journal ArticleDOI
TL;DR: First virtual biopsy based on backward propagating optical higher harmonics, combining second harmonic and third harmonic, is demonstrated in the fixed human skin specimens and can provide morphologic information including the distribution of basal cells while second harmonic generation can provide distribution of collagen fibers in dermis.
Abstract: Harmonics-based optical microscopy has been widely applied in biomedical researches due to its noninvasiveness to the studied biomaterials. Due to momentum conservation consideration, most previous studies collect harmonics generation signals in a forward geometry, especially for third harmonic generation signals. However, the adopted forward transmission type geometry is not feasible for future clinical diagnosis. In this paper, first virtual biopsy based on backward propagating optical higher harmonics, combining second harmonic and third harmonic, is demonstrated in the fixed human skin specimens. In our study, third harmonic generation can provide morphologic information including the distribution of basal cells while second harmonic generation can provide distribution of collagen fibers in dermis. Therefore, this technique is ideal for future noninvasive in vivo skin disease examination without dye.

Book ChapterDOI
TL;DR: Together with its nonlinearity, higher harmonic generation microscopy provides sub-micron three-dimensional sectioning capability and millimeter penetration in live samples without using fluorescence and exogenous markers, offering morphological, structural, functional, and cellular information of biomedical specimens without modifying their natural biological and optical environments.
Abstract: Higher harmonic-generation, including second harmonic generation and third harmonic generation, leaves no energy deposition to the interacted matters due to its virtual-level transition characteristic, providing a truly non-invasive modality and is ideal for in vivo imaging of live specimens without any preparation Second harmonic generation microscopy provides images on stacked membranes and arranged proteins with organized nano-structures due to the bio-photonic crystalline effect Third harmonic generation microscopy provides general cellular or subcellular interface imaging due to optical inhomogeneity Due to their virtual-transition nature, no saturation or bleaching in the generated signal is expected With no energy release, continuous viewing without compromising sample viability can thus be achieved Combined with its nonlinearity, higher harmonic generation microscopy provides sub-micron three-dimensional sectioning capability and millimeter penetration in live samples without using fluorescence and exogenous markers, offering morphological, structural, functional, and cellular information of biomedical specimens without modifying their natural biological and optical environments