Turnable Second Harmonic Generation from an Organic Dye Laser

Abstract

Ultraviolet light has been generated from a Rhodamine 60 organic dye laser by frequency doubling with a KDP crystal. The second harmonic was tuned from 2900Å to 3000Å with peak powers of 40 watts.

Organic dye lasers have now been reported with output wave-lengths extending throughout the visible and near infrared^1-12. The tunability^4,6,13 and output energies now available in the visible protion of the spectrum suggest frequency doubling as a means of obtaining a tunable source of ultraviolet light. We wish to report the observation of tunable second harmonic radiation centered at 2950Å generated from the laser output of a 10^?4 molar solution of Rhodamine 6G dissolved in ethyl alcohol.     

Controlling the divergence of high harmonics from solid targets: a route toward coherent harmonic focusing

Harmonic generation from relativistically oscillating plasma surfaces formed during the interaction of high contrast lasers with solid-density targets has been shown to be an efficient source of extreme ultraviolet (XUV) and X-ray radiation. Recent work has demonstrated that the exceptional coherence properties of the driving laser can be mirrored in the emitted radiation, permitting diffraction limited performance and attosecond phase locking of the harmonic radiation. These unique properties may allow the coherent harmonic focusing (CHF) of high harmonics generated from solid density targets to intensities on the order of the Schwinger limit of 10²⁹ W cm^-2 with laser systems available in the near future [Phys. Rev. Lett. 93, 115002 (2004)] and thus pave the way for unique experiments exploring the nonlinear properties of vacuum on ultra-fast timescales. In this paper we investigate experimentally as well as numerically the prospect of focusing high harmonics under realistic experimental conditions and demonstrate, using particle in cell (PIC) simulations, that precise control of the wavefronts and thus the focusability of the generated harmonics is possible with pre-shaped targets.     

Beam properties of fully optimized,table-top,coherent source at 30 nm

We present results on development and experimental implementation of a 1-kHz, coherent extreme ultraviolet (XUV) radia- tion source based on high-order harmonic generation of the femtosecond, near-infrared laser pulses produced by the titanium-doped sapphire laser system (35 fs, 1.2 mJ, 810 nm) at the Institute of Physics AS CR / PALS Centre. The source comprises a low-density static gas cell filled with a conversion medium, typically argon. The comprehensive optimization of the XUV harmonic source has been performed with respect to major parameters such as gas pressure in the cell, cell length, position of the focus of the driving laser field with respect to the gas cell position, size of the driving near-infrared laser beam, chirp of the femtosecond pulse, and the focal length of the lens deployed in the experimental setup. Harmonic spectra were recorded using an XUV transmission grating spectrometer developed specifically for this purpose. Detailed characterization of the XUV source has been performed including measurement of the XUV beam profile, M² parameter of the beam, absolute energy, and spatial coherence.     

Ultraviolet quasi-phase-matched second harmonic generation in surface periodically poled lithium niobate optical waveguides

The compatibility of low concentration (α-phase) proton exchange channel waveguides with electric field surface periodic poling of congruent lithium niobate (SPPLN) crystals has been experimentally demonstrated. With such waveguides, we obtained ultraviolet second harmonic generation (SHG) by first order quasi-phase-matching (QPM), a result made possible by the fabrication, on Z-cut LN crystals, of periodic structures with a pitch down to 750 nm. Nonlinear copropagating QPM-SHG measurements have been carried out on such structures. The pump source was a Ti:sapphire laser with a tunability range of 700–980 nm and a 40 GHz linewidth. We have measured UV continuous wave light at 390 nm by means of a lock-in amplifier and a photodiode with an enhanced response in the UV. The measured conversion efficiency was about 1% W^?1 cm^?2.     

Molecular gases as a source of coherent,tunable XUV radiation

Coherent and broadly tunable over 3500 cm^-1 extreme ultraviolet (XUV) radiation from 935 to 967 Å has been generated by frequency tripling the second harmonic output of a rhodamine 590 pulsed dye laser in molecular nitrogen and carbon monoxide. The scheme exploits high lying Rydberg and valence states of these gases and leads to the production of about 5 × 10⁹ XUV photons per pulse corresponding to a conversion efficiency of 5 × 10^-6.     

Optimization of the focused flux of high harmonics

Following the theoretical predictions [1], the observation of two-photon processes by interaction of vacuum ultraviolet (VUV) radiation with inner-shell levels of atoms requires focused intensities in the 10¹³-10¹⁴ W/cm² range. Our aim is to reach this regime in order to study non-linear optics at these wavelengths. We first optimized the high harmonic conversion efficiency in argon by studying the best experimental conditions for phase-matching, concentrating on focus geometry related to laser energy, cell length and position relative to the focus. We then studied the resulting harmonic beam focusability by a toroidal mirror (f=10 cm) and made an image of the harmonic focus. We conclude with an evaluation of the focused intensity that we are able to reach experimentally.Received: 28 January 2003, Published online: 24 April 2003PACS: 32.80.Rm Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 42.65.Ky Frequency conversion; harmonic generation, including higher-order harmonic generation     

Controlling continuum harmonic generation with attosecond pulses

Photo-ionization and high-order harmonic generation (HOHG) in molecular systems under the combined action of infrared femtosecond (fs) and UV attosecond (as) intense laser pulses are investigated numerically for a one-dimensional non-Born–Oppenheimer H⁺ ₂ ion. It is shown that such a coherent control scheme of fs–as ionization leads to significant enhancement of HOHG, with efficiencies exceeding the one obtained from a single fs pulse by several orders of magnitude. The basic mechanism for this enhancement is established as enhanced ionization and control of the recollision of a high-energy non-zero-velocity ionized electron, as compared to tunneling ionization models where the ionized electron has initial zero velocity. The combined superposition of fs–as pulses results in broad HOHG spectra with a large continuum near the cutoff, thus providing a new source for synthesizing new X-ray (vacuum ultraviolet) as pulses. PACS 33.60.-q; 33.80.-b     

Generation of high-order harmonic continuum with two-hump-structure infrared laser pulse

We experimentally investigate the high-order harmonic generation in argon gas cell driven by a multi-cycle broadband infrared laser pulse from a tunable optical-parametric-amplifier （OPA） source. The generation of high-order harmonic continuum with the cut-off photon energy up to 110 eV is observed by tuning the chirp of the 800-nm laser pulse which pumps OPA source. The generation of harmonic continuum is understood in terms of the two-hump structure of the OPA output spectrum and the optimal relative phase of the two humps. The demonstrated scheme is of importance for the generation of extreme ultraviolet （XUV） continuum at higher photon energy region.     

Attosecond manipulation of ionization and efficient broadband supercontinuum generation in stretched molecules

<正>We theoretically investigate the high-order harmonic generation from stretched molecules in a linearly polarized intense field.By adopting an infrared pulse combined with an ultraviolet(UV) attosecond pulse,the ionization process can be controlled effectively.In this excitation scheme,the harmonic spectrum beyond I_p+3.17U_P is significantly enhanced by two orders,where I_p and U_p=e~2E_0~2/(4m_eω~2) are the ionization and ponderomotive potential,then smooth broadband supercontinuum with the bandwidth of about 120 eV is obtained,which leads to an isolated sub-60- as attosecond pulse with a high signal-noise ratio.Moreover,the bandwidth of the supercontinuum is weakly dependent on the location and pulse duration of the UV pulse.     

Sixth Harmonic of A Nd：YVO4 Laser Generation In KBBF for ARPES

We report that a deep ultraviolet （DUV） laser from the sixth harmonic of a 1064nm laser has been firstly used as light source in an ultrahigh energy-resolution angle-resolved photoemission spectroscopy （ARPES）. The wavelength is 177.3nm obtained by using the second harmonic KBe2BO3F2 crystal with a frequency tripled 1064nm Nd：YVO4 laser. The large flux （10^14 - 10^15 photons/s） and narrow line width （0.26 meV） are suitable for the ultrahigh-energy resolution ARPES. The laser-ARPES can be a powerful tool to study the electronic structure at and near the Fermi level of the superconductor and correlated materials. The laser-ARPES has worked more than 500 h already.     

A nanohole in a thin metal film as an efficient nonlinear optical element

The nonlinear optical properties of single nanoholes and nanoslits fabricated in gold and aluminum nanofilms are studied by third harmonic generation (THG). It is shown that the extremely high third-order optical susceptibility of aluminum and the presence of strong plasmon resonance of a single nanohole in an aluminum film make possible an efficient nanolocalized radiation source at the third harmonic frequency. The THG efficiency for a single nanohole in a thin metal film can be close to unity for an exciting laser radiation intensity on the order of 10¹³ W/cm².     

Multi-photon-pumped stimulated emission from ZnO nanowires: A time-resolved study

In this work, we study temporal evolution of multi-photon-pumped stimulated emission from ZnO nanowires. In addition to second harmonic generation, ultraviolet stimulated emission is observed in ZnO nanowires under femtosecond pulse excitation at 800 nm. Sharp emission peaks appear when excitation flux reaches a threshold of 80 mJ/cm², which can be interpreted as lasing action in self-formed nanowire microcavities. Temporal evolution of the emission captured by Kerr shutter technique shows strong excitation-power dependence. The dynamic trace of stimulated emission exhibits a fast decay with a lifetime about 4.5 ps at intermediate excitation (∼100 mJ/cm²) and a lifetime about 2 ps at high excitation (>160 mJ/cm²). The difference in the lifetime can be attributed to different gain mechanisms related to excitonic interaction and electron-hole plasma, respectively.     

Possibility of lasing in the visible band by molecule photodissociation

The lower excited states of certain diatomic radicals and atoms, transitions from which to the ground state lie in the visible and in the near ultraviolet regions of the spectrum, are analyzed. Possible mechanisms of inversion via photodissociation of the molecules by radiation from a source with a continuous spectrum, having a brightness temperature T ? 3·10⁴ °K, are considered.     

Plasma dynamically induced frequency shifts in high-order harmonic generation in nitrogen

Experiments and theoretical calculations on high-harmonic generation in nitrogen are presented in the regime of laser pulses of a 300-ps duration, where the plasma dynamics following the ionization of the medium plays a decisive role. The experiments are performed with ～4-GW Ti:sapphire laser pulses, giving rise to fully saturated ionization. The shifts between the exact harmonic frequency in the extreme ultraviolet and the integer multiple of the fundamental frequency are caused by the self-phase modulation of the laser pulse due to the time-dependent free-electron density in the plasma generated in the focal zone. Well-calibrated atomic resonances in the extreme ultraviolet measured through absorption in a secondary gas jet are used as frequency markers in the extreme ultraviolet for the accurate determination of the sign and magnitude of the frequency shifts. A theoretical model including both plasma dynamics and harmonic generation from atoms and ions has previously been developed, and successfully applied to explain the frequency red shift observed in xenon [Phys. Rev. Lett. 96, 123904 (2006)]. The plasma-dynamical model is extended and applied to the results of the harmonic generation in nitrogen, fully explaining the observed harmonic frequency shifts in the 9th and 13th harmonic.     

Development of scattering near-field optical microspectroscopy apparatus using an infrared synchrotron radiation source

We report the status of a scattering near-field microspectroscopy apparatus developed at SPring-8 using an infrared synchrotron radiation (IR-SR) source. It consists of a scattering type scanning near-field optical microscope and a Fourier transform infrared spectrometer. The IR-SR is used as a highly brilliant and broad-band IR source. This apparatus has potential for application in near-field spectroscopy with high spatial resolution beyond the diffraction limit. In order to eliminate background scatterings from the probe shaft and/or sample surface, we used higher harmonic demodulation method. The near-field spectra were observed by 2nd harmonic components using the lock-in detection. The spatial resolution of about 300 nm was achieved at around 1000 cm^? 1 (10 μm wavelength).     

An extremely narrow UV pulse generation using a micro- and nano-ring system for pico-lithographic resolution

We propose a new technique of an extremely narrow ultraviolet (UV) pulse width generation for pico-lithography technology using a nonlinear ring resonator system. A system consists of three micro- and a nano-optical ring resonators, which can be used to generate the 50 pm (10⁻¹² m) optical spectral width at the ultraviolet wavelength. By using a soliton pulse with a pulse width of 50 ns, 1 W peak power, center wavelength at 1550 nm, after the soliton pulse is launched into a first ring device, the chaotic pulses are generated within the first ring. The chaotic filtering behaviors are performed by using the second and third ring devices, whereas the extremely short pulse, i.e. narrow spectral width, can be generated by using the extended nano-ring device. The broad spectrum of the harmonic waves is generated and filtered, especially the generation of third harmonic wave, which is known as the ultraviolet wavelength, is achieved, which is capable of forming pico-lithographic resolution. Results obtained have shown that the generation of the spectral width of 50 pm at a wavelength of 511.125 nm, with peak power at 35 mW is achieved.     

Generation of picosecond UV pulses by stimulated anti-Stokes Raman scattering

Picosecond stimulated anti-Stokes Raman scattering of hydrogen gas in the ultraviolet region has been studied, using the second harmonic of a modelocked Nd³⁺: YAG laser as an incident pulse (25 ps, 532 nm, 10 mJ). Good conversion efficiency for higher-order anti-Stokes lines has been realized, yielding 2 μJ (200 kW, 10 ps) output for the 8th one at 192 nm. Some features of transient stimulated Raman scattering have been examined and discussed.     

Vacuum ultraviolet frequency combs generated by a femtosecond enhancement cavity in the visible

We present the first (to our best knowledge) femtosecond enhancement cavity in the visible wavelength range for ultraviolet frequency comb generation. The cavity is seeded at 518 nm by a frequency-doubled Yb fiber laser and operates at a peak intensity of 1.2×10(13) W/cm(2). High harmonics of up to the ninth order (~57 nm) are generated in an intracavity xenon gas jet. Intracavity high harmonic powers of several milliwatts for the third harmonic order and microwatts for the fifth harmonic order prove the potential of the "green cavity" as an efficient ultraviolet frequency comb source for future spectroscopic experiments. A limiting degradation effect of the cavity mirrors is avoided by operating at a constant oxygen background pressure.     

Photoluminescence degradation mechanism of BaMgAl10O17：Eu2＋ phosphor by vacuum ultraviolet irradiation

<正>A real high power vacuum ultraviolet light source is applied to the investigation on the vacuum ultraviolet irradiation degradation of BaMgA₁₀O₁₇:Eu²⁺ phosphor.The degradations of emission intensity and color quality of the sample are clearly observed after irradiation.It reveals that the oxidation of Eu²⁺ during irradiation is partly responsible for the degradations.The excitation and absorption spectra show that some traps generated during irradiation have negative influence on the luminescence of sample and these traps have been identified as positively charged oxygen vacancies by positron annihilation.The investigations on host emission and decay curve further confirm that these oxygen vacancies are involved in the perturbation of energy transfer from the host to Eu²⁺ and finally result in the degradation.     

Generation of ultrashort coherent vacuum ultraviolet pulses using electron storage rings: a new bright light source for experiments

We demonstrate for the first time that seeded harmonic generation on electron storage rings can produce coherent optical pulses in the vacuum ultraviolet spectral range. The experiment is performed at Elettra, where coherent pulses are generated at 132 nm, with a duration of about 100 fs. The light source has a repetition rate of 1 kHz and adjustable polarization; it is very bright, with a peak power several orders of magnitude above that of spontaneous synchrotron radiation. Owing to high stability, the source is used in a test photoemission electron microscopy experiment. We anticipate that seeded harmonic generation on storage rings can lead to unprecedented developments in time-resolved femtosecond spectroscopy and microscopy.