Teruto Kanai

Nonlinear optics in the extreme ultraviolet

Nonlinear responses to an optical field are universal in nature but have been difficult to observe in the extreme ultraviolet (XUV) and soft X-ray regions owing to a lack of coherent intense light sources. High harmonic generation is a well-known nonlinear optical phenomenon and is now drawing much attention in attosecond pulse generation. For the application of high harmonics to nonlinear optics in the XUV and soft X-ray regime, optical pulses should have both large pulse energy and short pulse duration to achieve a high optical electric field. Here we show the generation of intense isolated pulses from a single harmonic (photon energy 27.9 eV) by using a sub-10-femtosecond blue laser pulse, producing a large dipole moment at the relatively low (ninth) harmonic order nonadiabatically. The XUV pulses with pulse durations of 950 attoseconds and 1.3 femtoseconds were characterized by an autocorrelation technique, based on two-photon above-threshold ionization of helium atoms. Because of the small cross-section for above-threshold ionization, such an autocorrelation measurement of XUV pulses with photon energy larger than the ionization energy of helium has not hitherto been demonstrated. The technique can be extended to the characterization of higher harmonics at shorter wavelengths.

A versatile system for ultrahigh resolution, low temperature, and polarization dependent Laser-angle-resolved photoemission spectroscopy

We have developed a low temperature ultrahigh resolution system for polarization dependent angle-resolved photoemission spectroscopy (ARPES) using a vacuum ultraviolet (vuv) laser (hnu=6.994 eV) as a photon source. With the aim of addressing low energy physics, we show the system performance with angle-integrated PES at the highest energy resolution of 360 mueV and the lowest temperature of 2.9 K. We describe the importance of a multiple-thermal-shield design for achieving the low temperature, which allows a clear measurement of the superconducting gap of tantalum metal with a T(c)=4.5 K. The unique specifications and quality of the laser source (narrow linewidth of 260 mueV, high photon flux), combined with a half-wave plate, facilitates ultrahigh energy and momentum resolution polarization dependent ARPES. We demonstrate the use of s- and p-polarized laser-ARPESs in studying the superconducting gap on bilayer-split bands of a high T(c) cuprate. The unique features of the quasi-continuous-wave vuv laser and low temperature enables ultrahigh-energy and -momentum resolution studies of the spectral function of a solid with large escape depth. We hope the present work helps in defining polarization dependent laser excited angle-resolved photoemission spectroscopy as a frontier tool for the study of electronic structure and properties of materials at the sub-meV energy scale.

Generation of vacuum-ultraviolet light by an optically contacted, prism-coupled KBe2BO3F2 crystal

We have demonstrated the second harmonic of a frequency-tripled Nd:YVO4 laser with 2.5-mW quasi-cw output by using an optically contacted, prism-coupled KBe2BO3F2 crystal. We also achieved the second harmonic with a frequency-doubled single-mode Ti:sapphire laser at 172.5 nm and sum-frequency mixing with a dual-wavelength Ti:sapphire laser at 163.3 nm. These wavelengths are to our knowledge the shortest obtained by use of nonlinear crystals for second-harmonic generation and sum-frequency mixing, respectively.

Generation of vacuum-ultraviolet light below 160 nm in a KBBF crystal by the fifth harmonic of a single-mode Ti:sapphire laser

We have generated a vacuum-ultraviolet light below 160 nm by sum-frequency mixing in an optically contacted, prism-coupled KBe2BO3F2 crystal. The vacuum-ultraviolet light was generated as the fifth harmonic of a tunable, single-mode, 1-kHz Ti:sapphire laser system. The wavelength of 156 nm, to our knowledge, is the shortest ever obtained by use of nonlinear crystals in a phase-matched process. In addition, we demonstrated a 157.6-nm light source as an inspection tool for F2 laser lithography with an average power of 0.8 μW.

Carrier-envelope phase-dependent high harmonic generation in the water window using few-cycle infrared pulses

High harmonic generation (HHG) using waveform-controlled, few-cycle pulses from Ti:sapphire lasers has opened emerging researches in strong-field and attosecond physics. However, the maximum photon energy of attosecond pulses via HHG remains limited to the extreme ultraviolet region. Long-wavelength light sources with carrier-envelope phase stabilization are promising to extend the photon energy of attosecond pulses into the soft X-ray region. Here we demonstrate carrier-envelope phase-dependent HHG in the water window using sub-two-cycle optical pulses at 1,600 nm. Experimental and simulated results indicate the confinement of soft X-ray emission in a single recombination event with a bandwidth of 75 eV around the carbon K edge. Control of high harmonics by the waveform of few-cycle infrared pulses is a key milestone to generate soft X-ray attosecond pulses. We measure a dependence of half-cycle bursts on the gas pressure, which indicates subcycle deformation of the waveform of the infrared drive pulses in the HHG process.

Watt-level tunable deep ultraviolet light source by a KBBF prism-coupled device.

We have obtained an average output power as much as 1.2 W at 200 nm by using a 2.71-mm thick KBe2BO3F2 crystal optically contacted by CaF2 and SiO2 prisms on the both sides. Watt-level average-power was generated tunably in the deep ultraviolet region from 185 nm to 200 nm. The average power is the highest, to our knowledge, ever obtained by nonlinear crystals in the wavelength region below 200 nm.

Improved Sellmeier Equations and Phase-Matching Characteristics in Deep-Ultraviolet Region of

A 3.0-mm-thick KBe 2BO3F2 (KBBF) crystal has been successfully grown and used to fabricate a right angle prism. Its refractive indices were accurately measured with a prism technique at seven wavelengths from 0.4047 to 0.6562 mum . Its phase-matching characteristics in deep-ultraviolet (UV) region were investigated. Using the measured indices and phase-matching angles from deep-UV to near infrared, improved Sellmeier equations for KBBF have been derived.

{\hbox {KBe}}_{2}{\hbox {BO}}_{3}{\hbox {F}}_{2}

Time-resolved photoelectron spectroscopy (trPES) can directly detect transient electronic structure, thus bringing out its promising potential to clarify nonequilibrium processes arising in condensed matters. Here we report the result of core-level (CL) trPES on 1T-TaS2, realized by developing a high-intensity 60 eV laser obtained by high-order harmonic (HH) generation. Ta4f CL-trPES offers the transient amplitude of the charge-density-wave (CDW), via the site-selective and real-time observation of Ta electrons. The present result indicates an ultrafast photoinduced melting and recovery of CDW amplitude, followed by a peculiar long-life oscillation (i.e. collective amplitudon excitation) accompanying the transfer of 0.01 electrons among adjacent Ta atoms. CL-trPES offers a broad range of opportunities for investigating the ultrafast atom-specific electron dynamics in photo-related phenomena of interest.

Crystal

Blue pulses with durations of 8.5 fs are generated by broadband frequency doubling of subterawatt Ti:sapphire laser systems at 1-5-kHz repetition rates. The average powers are 1.6 W at 5 kHz and 1.9 W at 1 kHz. The peak power is 0.16 TW with a duration of 12 fs at 1 kHz.

Femtosecond core-level photoemision spectroscopy on 1T-TaS2 using a 60-eV laser source

Pulse-front distortion as a result of broadband frequency doubling (BFD) has been compensated for over a 3-cm beam diameter by use of a telescope image relay system. As a result, distortion-free blue pulses with a peak power of 1.4 TW and a pulse width of 10 fs have been generated with a 10-Hz Ti:sapphire laser by use of this modified BFD configuration.