RESUMEN

We describe a setup for time- and angle-resolved photoemission spectroscopy with wavelength-tunable excitation and an extreme ultraviolet probe. It is enabled by using the 10 kHz twin Ti:sapphire amplifiers seeded by the common Ti:sapphire oscillator. The typical probe energy is 21.7 eV, and the wavelength of the pump excitation is tuned between 2400 and 1200 nm by using the optical parametric amplifier. The spectral width of the extreme ultraviolet probe is 53 meV, and the time resolution is dependent on the wavelength for the pump, better than 60 fs for the pump energy >0.7 eV. This system enables the pump energy to be matched with a specific interband transition and to probe a wider energy-momentum space. We present the results for the prototypical materials of highly oriented pyrolytic graphite and Bi2Se3 to show the performance of our system.

RESUMEN

We develop a BiB3O6 (BiBO)-based optical parametric amplifier in the spectral region around 2 µm using a Yb:KGW amplifier operating at 100 kHz. The two-stage degenerate optical parametric amplification results in a typical output energy of 30 µJ after compression, spectrum covering 1.7-2.5 µm range, and a pulse duration fully compressible down to 16.4 fs, corresponding to 2.3 cycles. Due to the inline difference frequency generation of the seed pulses, the carrier envelope phase (CEP) is passively stabilized without feedback over 11 hours at the level below 100 mrad including a long-term drift. Short-term statistical analysis in the spectral domain further shows a behavior qualitatively different from that of parametric fluorescence, indicating high degree of suppression of optical parametric fluorescence. The high phase stability together with the few-cycle pulse duration is promising for the investigation of high-field phenomena such as subcycle spectroscopy in solids or high harmonics generation.

RESUMEN

The stereochemistry of pericyclic reactions is explained by orbital symmetry conservation, referred to as the Woodward-Hoffmann (WH) rule. Although this rule has been verified using the structures of reactants and products, the temporal evolution of the orbital symmetry during the reaction has not been clarified. Herein, we used femtosecond soft X-ray transient absorption spectroscopy to elucidate the thermal pericyclic reaction of 1,3-cyclohexadiene (CHD) molecules, i.e., their isomerization to 1,3,5-hexatriene. In the present experimental scheme, the ring-opening reaction is driven by the thermal vibrational energy induced by photoexcitation to the Rydberg states at 6.2 eV and subsequent femtosecond relaxation to the ground state of CHD molecules. The direction of the ring opening, which can be conrotatory or disrotatory, was the primary focus, and the WH rule predicts the disrotatory pathway in the thermal process. We observed the shifts in K-edge absorption of the carbon atom from the 1s orbital to vacant molecular orbitals around 285 eV at a delay between 340 and 600 fs. Furthermore, a theoretical investigation predicts that the shifts depend on the molecular structures along the reaction pathways and the observed shifts in induced absorption are attributed to the structural change in the disrotatory pathway. This confirms that the orbital symmetry is dynamically conserved in the ring-opening reaction of CHD molecules as predicted using the WH rule.

RESUMEN

Ultrafast carrier dynamics in a graphene system are very important in terms of optoelectronic devices. Recently, a twisted bilayer graphene has been discovered that possesses interesting electronic properties owing to strong modifications in interlayer couplings. Thus, a better understanding of ultrafast carrier dynamics in a twisted bilayer graphene is highly desired. Here, we reveal the unbalanced electron distributions in a quasicrystalline 30° twisted bilayer graphene (QCTBG), using time- and angle-resolved photoemission spectroscopy on the femtosecond time scale. We distinguish time-dependent electronic behavior between the upper- and lower-layer Dirac cones and gain insight into the dynamical properties of replica bands, which show characteristic signatures due to Umklapp scatterings. The experimental results are reproduced by solving a set of rate equations among the graphene layers and substrate. We find that the substrate buffer layer plays a key role in initial carrier injections to the upper and lower layers. Our results demonstrate that QCTBG can be a promising element for future devices.

RESUMEN

We report on a wavelength-tunable optical parametric amplifier (OPA) from 2.7 to 3.8 µm seeded with carrier-envelope phase (CEP) stabilized pulses generated by intra-pulse difference frequency generation (DFG) using a commercial Yb:KGW chirped-pulse amplifier. The Yb:KGW laser's output pulses are spectrally broadened in two-stage multi-plate pulse compression from 0.8 to 1.25 µm, which are compressed down to a sub-two-cycle duration of 6.5 fs using chirp mirrors. CEP-stabilized mid-infrared pulses are produced in intra-pulse DFG of the spectrally broaden pulses around 1.03 µm and parametrically amplified in KTiOAsO 4 crystals. The output energy and temporal duration of the OPA output pulses range from 31 to 56 µJ and from 102 to 203 fs, respectively. The root mean square value of their CEP errors is measured to be 101 mrad.

RESUMEN

The characterization of the temporal waveform of few-cycle laser pulses is an indispensable part in strong-field physics and attosecond science. Recently, a simple waveform-characterization technique called TIPTOE (tunneling ionization with a perturbation for the time-domain observation of an electric field) has been demonstrated for measuring linearly polarized few-cycle pulses. We theoretically and experimentally show that TIPTOE can be extended to resolve more characteristics of an optical waveform: the two-dimensional polarization and the Gouy phase. Based on the plasma fluorescence of a gaseous medium, we achieve all-optical and spatially resolved measurements of the waveform of an infrared pulse. This detection method enables the remote characterization of a waveform without the need to place an apparatus near the focal point of the laser beam. The proposed approach represents a simple and powerful method for conducting waveform diagnostics on few-cycle laser sources.

RESUMEN

High harmonic spectroscopy in solids is emerging as a new tool to investigate ultrafast electron dynamics in the presence of strong optical fields. However, the observed high harmonic spectra do not usually reflect the microscopic origin of high harmonic generation (HHG) because of nonlinear and/or linear propagation effects. Here, we systematically investigate the HHG in reflection and transmission from gallium arsenide exposed to intense mid-infrared optical pulses. In transmission geometry, we find that the properties of high harmonics are drastically changed by nonlinear effects during the propagation of even tens of micrometers. Especially, the nonlinear absorption and/or nonlinearly induced ellipticity of the drive pulses as well as a cascade nonlinear mixing significantly alter the high harmonic signals in the case of the transmission geometry, making an extraction of the microscopic electron dynamics of gallium arsenide difficult. On the contrary, in reflection geometry, we obtain HHG spectra that are free from propagation effects, opening a general approach for high harmonic spectroscopy.

RESUMEN

Using light to manipulate materials into desired states is one of the goals in condensed matter physics, since light control can provide ultrafast and environmentally friendly photonics devices. However, it is generally difficult to realise a photo-induced phase which is not merely a higher entropy phase corresponding to a high-temperature phase at equilibrium. Here, we report realisation of photo-induced insulator-to-metal transitions in Ta2Ni(Se1-xSx)5 including the excitonic insulator phase using time- and angle-resolved photoemission spectroscopy. From the dynamic properties of the system, we determine that screening of excitonic correlations plays a key role in the timescale of the transition to the metallic phase, which supports the existence of an excitonic insulator phase at equilibrium. The non-equilibrium metallic state observed unexpectedly in the direct-gap excitonic insulator opens up a new avenue to optical band engineering in electron-hole coupled systems.

RESUMEN

We demonstrate the generation of 21 fs (1.8 optical cycle), 45-µJ, carrier-envelope phase (CEP)-stable optical pulses with an octave-spanning spectrum from 2.2 to 4.9 µm. Multi-cycle output pulses (120 fs, 149 µJ, 3.5 µm, and 300 Hz) from a KTA-based optical parametric amplifier are compressed down to the sub-two-cycle regime using YAG and Si plates. The single-shot CEP stability of the compressed pulses is measured to be 283 mrad for 500 s. This robust and compact scheme realizes a field strength of 282 MV/cm with f/11 focusing, opening a new regime of attosecond strong-field physics in solids.

RESUMEN

Long-wavelength lasers have great potential to become a new-generation drive laser for tabletop coherent light sources in the soft X-ray region. Because of the significantly low conversion efficiency from a long-wavelength light field to high-order harmonics, their pulse characterization has been carried out by measuring the carrier-envelope phase and/or spatial dependences of high harmonic spectra. However, these photon detection schemes, in general, have difficulty in obtaining information on the spectral phases, which is crucial to determine the temporal structures of high-order harmonics. Here, we report the first attosecond streaking measurement of high harmonics generated by few-cycle optical pulses at 1.7 µm from a BiB3O6-based optical parametric chirped-pulse amplifier. This is also the first demonstration of time-resolved photoelectron spectroscopy using high harmonics from a long-wavelength drive laser other than Ti:sapphire lasers, which paves the way towards ultrafast soft X-ray photoelectron spectroscopy.

RESUMEN

Large-scale (180 × 60 × 1 mm(3)) transmission gratings with groove densities of 1250 and 1740 lines/mm have been developed, resulting in diffraction efficiencies above 95%. The throughput of a folded pulse compressor with two large-scale transmission gratings was approximately 80% in a 20-fs Ti:sapphire chirped-pulse amplification (CPA) laser. The parabolic bending of the transmission grating due to anti-reflection (AR) coating was minimized to 2.9 λ at 633 nm by improving the evaporation process. By a simple analysis, we explain why this level of bending does not induce a wavefront distortion through the transmission grating near the Littrow condition while the wavefront from a reflection grating is distorted to nearly twice the bending of the grating. The calculation based on the measured bending shows that both the group delay difference relative to the ideally flat grating from 750 to 850 nm and the spatial pulse front distortion over a 60-mm-diameter input beam are negligible, even when the dispersive beam covers ~140 mm on the grating. The spatial pulse front distortion measured after the compressor was less than the measurement limit (1.5 fs) for a 20-mm-diameter beam, where the beam size in the dispersive direction on the grating was 85 mm.

RESUMEN

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.

RESUMEN

Ultrashort pulses with a 25-µJ output energy were generated at 200 nm by dual broadband frequency doubling with a thin KBe(2)BO(3)F(2) (KBBF) crystal at 1 kHz as the fourth harmonic of a high power Ti:sapphire laser. The spectrum was broadened to a spectral width of 2.25 nm. The pulse duration of 56 fs was measured by single-shot autocorrelation with two-photon fluorescence from self-trapped excitons in a CaF(2) crystal.

Asunto(s)

RESUMEN

Multimillijoule, few-cycle, carrier-envelope-phase (CEP)-locked, near-IR pulses at 750 nm from an optical parametric chirped-pulse amplifier are applied to the generation of CEP-dependent, soft x-ray high harmonics around the boron K-edge at 188 eV. The dependence on the CEP manifests the phase coherence of high harmonics preserved in the highest-photon energy ever reported. Multimillijoule optical pulses also allow the extension of the cutoff energy up to 325 eV, exceeding the carbon K-edge of the water window. However, in this spectral range, the CEP dependence of harmonic spectra is not observed, suggesting the degradation of temporal coherence due to the heavy ionization of helium atoms.

RESUMEN

We report the generation of quasi-continuous-wave vacuum-ultraviolet (VUV) coherent light based on a Ti:sapphire laser with two successive frequency doubling stages. In the first stage, UV light at 399 nm with power of 1.1 W was obtained by exploiting an enhanced cavity. With a KBBF crystal as nonlinear material, quasi-continuous-wave VUV coherent light with power of about 25 mW at 199.5 nm and 4.7 mW at 193.5 nm were achieved through a single-pass SHG configuration, respectively, in the second stage.

RESUMEN

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.

RESUMEN

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.

RESUMEN

We have successfully observed two-photon above-threshold ionization in rare gas atoms (Ar, Xe, and He) by the fifth harmonic (25 eV photon energy) of a KrF laser. Use of the energy-resolved photoelectron counting system together with our laser, providing strong 25 eV radiation at 40-100 Hz, enabled us to detect the very weak single-color two-photon above-threshold ionization signals. Experimental data are in good agreement with our theoretical calculations newly developed along the line of multichannel quantum defect theory.

RESUMEN

A hybrid tabletop (2 m x 3 m) terawatt chirped-pulse amplification Ti:sapphire-Nd:glass laser (1054 nm, 475 fs, 500 mJ, 9 x 10(17) W cm(-2)) has been developed for laser-matter experiments. An overall gain factor of 10(10) was achieved for the laser. The results of laser applications in the studies of soft-x-ray Ni-like Mo 18.9-nm lasing and of harmonic generation from solid surfaces are presented.

RESUMEN

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.