Carrier-envelope phase control of synthesized waveforms with two acousto-optic programmable dispersive filters.

We demonstrate the scanning and control of the carrier-envelope phases (CEPs) of two adjacent spectral components totally spanning more than one-octave in the short-wave infrared (SWIR) wavelength region by operating two individual acousto-optic programmable dispersive filters (AOPDFs) applied to each of the two spectral components. The total CEP shift of the synthesized sub-cycle pulse composed of the two spectral components is controlled with simultaneous scans of the two CEPs. The resultant error of the controlled CEP was 642 mrad, so that this technique is useful for searching zero CEP of the synthesized pulse with the maximum field amplitude. In addition, we conduct a closed feedback loop to compensate for the CEP fluctuation by using the two AOPDFs together. As a result, we succeed to reduce the rms error of the CEP from 399 mrad to 237 mrad.

100-mJ class, sub-two-cycle, carrier-envelope phase-stable dual-chirped optical parametric amplification.

Based on dual-chirped optical parametric amplification (DC-OPA) and type-I BiB3O6 (BiBO) crystals, the generation of >100 mJ, 10.4 fs, 10 Hz, carrier-envelope phase (CEP)-stable laser pulses, which are centered at 1.7 µm, was demonstrated producing a peak power of 10 TW. CEP-dependent high harmonic generation (HHG) was implemented to confirm the sub-two-cycle pulse duration and CEP stabilization of infrared (IR) laser pulses. As far as we know, the obtained pulse energy and peak power represented the highest values for sub-two-cycle CEP-stable IR optical parametric amplification. Additionally, the prospects of achieving high-energy water window isolated attosecond pulses (IAPs) via our developed laser source were discussed.

Adaptive optics with spatio-temporal lock-in detection for temporal focusing microscopy.

Wavefront distortion in temporal focusing microscopy (TFM) results in a distorted temporal profile of the excitation pulses owing to spatio-temporal coupling. Since the pulse duration is dramatically changed in the excitation volume, it is difficult to correct the temporal profile for a thick sample. Here, we demonstrate adaptive optics (AO) correction in a thick sample. We apply structured illumination microscopy (SIM) to an AO correction in wide-field TFM to decrease the change in the pulse duration in the signal detection volume. The AO correction with SIM was very successful in a thick sample for which AO correction with TFM failed.

Optimization of a multi-TW few-cycle 1.7-µm source based on Type-I BBO dual-chirped optical parametric amplification.

This paper presents the optimization of a dual-chirped optical parametric amplification (DC-OPA) scheme for producing an ultrafast intense infrared (IR) pulse. By employing a total energy of 0.77 J Ti:sapphire pump laser and type-I BBO crystals, an IR pulse energy at the center wavelength of 1.7 µm exceeded 0.1 J using the optimized DC-OPA. By adjusting the injected seed spectrum and prism pair compressor with a gross throughput of over 70%, the 1.7-µm pulse was compressed to 31 fs, which resulted in a peak power of up to 2.3 TW. Based on the demonstration of the BBO type-I DC-OPA, we propose a novel OPA scheme called the "dual pump DC-OPA" for producing a high-energy IR pulse with a two-cycle duration.

Indirect high-bandwidth stabilization of carrier-envelope phase of a high-energy, low-repetition-rate laser.

We demonstrate a method of stabilizing the carrier-envelope phase (CEP) of low-repetition-rate, high-energy femtosecond laser systems such as TW-PW class lasers. A relatively weak high-repetition-rate (~1 kHz) reference pulse copropagates with a low-repetition-rate (10 Hz) high-energy pulse, which are s- and p-polarized, respectively. Using a Brewster angle window, the reference pulse is separated after the power amplifier and used for feedback to stabilize its CEP. The single-shot CEP of the high-energy pulse is indirectly stabilized to 550 mrad RMS, which is the highest CEP stability ever reported for a low-repetition-rate (10-Hz) high-energy laser system. In this novel method, the feedback frequency of the reference pulse from the front-end preamplifier can be almost preserved. Thus, higher CEP stability can be realized than for lower frequencies. Of course, a reference pulse with an even higher repetition rate (e.g., 10 kHz) can be easily employed to sample and feed back CEP jitter over a broader frequency bandwidth.

Conical third-harmonic generation of optical vortex through ultrashort laser filamentation in air.

We experimentally generate third-harmonic (TH) vortex beams in air by the filamentation of femtosecond pulses produced in a lab-built Ti:sapphire chirped pulse amplifier. The generated TH beam profile is shown to evolve with increasing pump energy. At a sufficiently high pump energy, we observe a conical TH emission of the fundamental vortex and confirm that the conical radiation follows the conservation law for orbital angular momentum. We further investigate the far-field angularly resolved spectra of the TH wave to analyze the conical emission angle. We theoretically verify that the formation of the conical TH vortex results from the phase-matching between the fundamental and TH waves during the filamentation process.

Wide-range narrowband multilayer mirror for selecting a single-order harmonic in the photon energy range of 40-70 eV.

An experimental demonstration of a wide-range narrowband multilayer mirror for selecting a single-order high-harmonic (HH) beam from multiple-order harmonics in the photon energy range between 40 eV and 70 eV was carried out. This extreme ultraviolet (XUV) mirror, based on a pair of Zr and Al0.7Si0.3 multilayers, has a reflectivity of 20-35% and contrast of more than 7 with respect to neighboring HHs at angles of incidence from 10 to 56.9 degrees, assuming HHs pumped at 1.55 eV. Thus, specific single-order harmonic beams can be arbitrarily selected from multiple-order harmonics in this photo energy range. In addition, the dispersion for input pulses of the order of 1 fs is negligible. This simple-to-align optical component is useful for the many various applications in physics, chemistry and biology that use ultrafast monochromatic HH beams.

Carrier-envelope phase stabilization of a 16 TW, 10 Hz Ti:sapphire laser.

We propose and demonstrate a simple and promising method for stabilizing the carrier-envelope phase (CEP) of a high-energy ultrashort pulse laser operating at a low repetition rate. The method was successfully applied to a Ti:sapphire laser operating at 10 Hz with 400 mJ pulse energy and 25 fs pulse duration (16 TW). The laser system consists of a 1 kHz front-end preamplifier and a 10 Hz back-end power amplifier. By sampling a 500 Hz reference pulse from a 1 kHz seed pulse, the measured single-shot CEP noise of a 10 Hz amplified pulse is stabilized to 670 mrad rms. Our proposed CEP stabilization concept can be applied to single-shot ultrahigh-power lasers, such as a petawatt laser system.

High-energy infrared femtosecond pulses generated by dual-chirped optical parametric amplification.

We demonstrate high-energy infrared femtosecond pulse generation by a dual-chirped optical parametric amplification (DC-OPA) scheme [Opt. Express19, 7190 (2011)]. By employing a 100 mJ pump laser, a signal pulse energy exceeding 20 mJ at a wavelength of 1.4 µm was achieved before dispersion compensation. A total output energy of 33 mJ was recorded. Under a further energy scaling condition, the signal pulse was compressed to an almost transform-limited duration of 27 fs using a fused silica prism compressor. Since the DC-OPA scheme is efficient and energy scalable, design parameters for obtaining 100 mJ level infrared pulses are presented, which are suitable as driver lasers for the energy scaling of high-order harmonic generation with sub-keV photon energy.

Nuclear reaction induced by carrier-envelope-phase controlled proton recollision in a laser-driven molecule.

Nuclear reactions induced by proton recollision with a nearby nucleus are studied in a setup where a neutral molecule is exposed to an extremely intense, few-cycle laser pulse. At the rising edge of the laser pulse, all electrons in the molecule are first ejected by field ionization, resulting in a molecule consisting of the bare nuclei only. A proton in the bare molecule is subsequently accelerated by the laser field in such a way that it recollides with a nearby, heavier nucleus, with a kinetic energy high enough to induce a nuclear reaction. As a specific example, the probability of triggering the (15)N(p,α)(12)C reaction by exposing either a (15)NH molecule or a (15)NH3 molecule to an intense laser pulse is calculated using the classical trajectory Monte Carlo method. We show that the proton recollision process can be controlled both by varying the carrier-envelope phase of the laser field and by the degree of molecular orientation. We also find that the magnetic field of the laser pulse plays a crucial role in the recollision dynamics.

Absorption mechanism of the second pulse in double-pulse femtosecond laser glass microwelding.

The absorption mechanism of the second pulse is experimentally and theoretically investigated for high-efficiency microwelding of photosensitive glass by double-pulse irradiation using a femtosecond laser. The transient absorption change during the second pulse irradiation for various energies induced by the first pulse is measured at different delay times. The resulting effects depend on whether the delay time is 0-30 ps (time domain I) or 30- several ns (domain II). By solving rate equations for the proposed electronic processes, the excitation and relaxation times of free electrons in time domain I are estimated to be 0.98 and 20.4 ps, respectively, whereas the relaxation times from the conduction band to a localized state and from the localized state to the valence band in domain II are 104.2 and 714.3 ps, respectively. Single-photon absorption of the second pulse by free electrons dominates in domain I, resulting in high bonding strength. In time domain II, about 46% of the second pulse is absorbed by a single photon due to the localized state, which is responsible for higher bonding strength compared with that prepared by single-pulse irradiation.

Femtosecond laser nanostructuring in porous glass with sub-50 nm feature sizes.

We report on controllable production of nanostructures embedded in a porous glass by femtosecond laser direct writing. We show that a hollow nanovoid with a lateral size of ~40 nm and an axial size of ~1500 nm can be achieved by manipulating the peak intensity and polarization of the writing laser beam. Our finding enables applications ranging from direct construction of 3D nanofluidics in glass to clean stealth dicing of transparent plates.

Wavefront control of subcycle vortex pulses via carrier-envelope-phase tailoring.

The carrier-envelope phase (CEP) of an ultrashort laser pulse is becoming more crucial to specify the temporal characteristic of the pulse's electric field when the pulse duration becomes shorter and attains the subcycle regime; here, the pulse duration of the intensity envelope is shorter than one cycle period of the carrier field oscillation. When this subcycle pulse involves a structured wavefront as is contained in an optical vortex (OV) pulse, the CEP has an impact on not only the temporal but also the spatial characteristics owing to the spatiotemporal coupling in the structured optical pulse. However, the direct observation of the spatial effect of the CEP control has not yet been demonstrated. In this study, we report on the measurement and control of the spatial wavefront of a subcycle OV pulse by adjusting the CEP. To generate subcycle OV pulses, an optical parametric amplifier delivering subcycle Gaussian pulses and a Sagnac interferometer as a mode converter were integrated and provided an adequate spectral adaptability. The pulse duration of the generated OV pulse was 4.7 fs at a carrier wavelength of 1.54 µm. To confirm the wavefront control with the alteration of the CEP, we developed a novel [Formula: see text]-2[Formula: see text] interferometer that exhibited spiral fringes originating from the spatial interference between the subcycle OV pulse and the second harmonic of the subcycle Gaussian pulse producing a parabolic wavefront as a reference; this resulted in the successful observation of the rotation of spiral interference fringes during CEP manipulation.

Rotation-free holographic imaging with extended arc reference.

We proposed and experimentally demonstrated a rotation-free approach of holographic imaging by using an extended arc reference. From the diffraction intensity, the objects were retrieved using a two-step algorithm without a prior knowledge of the information of the sample and reference. This scheme alleviates the convergence problem of coherent diffractive imaging and also promises to achieve a high resolution.

Plasmonically enhanced Faraday effect in metal and ferrite nanoparticles composite precipitated inside glass.

Using femtosecond laser irradiation and subsequent annealing, nanocomposite structures composed of spinel-type ferrimagnetic nanoparticles (NPs) and plasmonic metallic NPs have been formed space-selectively within glass doped with both α-Fe(2)O(3) and Al. The Faraday rotation spectra exhibit a distinct negative peak at around 400 nm, suggesting that the ferrimagnetic Faraday response is enhanced by the localized surface plasmon resonance (LSPR) due to metallic Al NPs. At the interfaces in the nanocomposites, the ferrimagnetism of magnetite NPs is directly coupled with the plasmon in the Al NPs. The control of the resonance wavelength of the magneto-optical peaks, namely, the size of plasmonic NPs has been demonstrated by changing the irradiation or annealing conditions.

Fabrication of three-dimensional microfluidic channels inside glass using nanosecond laser direct writing.

We show that fabrication of three-dimensional microfluidic channels embedded in glass can be achieved by using a Q-switched, frequency-doubled Nd:YAG laser. The processing mainly consists of two steps: (1) formation of hollow microfluidic channels in porous glass immersed in Rhodamine 6G dissolved in water by nanosecond laser ablation; and (2) postannealing of the fabricated porous glass sample at 1120 °C for consolidation of the sample. In particular, a bilayer microfluidic structure is created in glass substrate using this technique for showcasing its capability of three-dimensional structuring.

Characterization and mechanism of glass microwelding by double-pulse ultrafast laser irradiation.

We investigated the physical mechanism of high-efficiency glass microwelding by double-pulse ultrafast laser irradiation by measuring the dependences of the size of the heat-affected zone and the bonding strength on the delay time between the two pulses for delay time up to 80 ns. The size of the heat-affected zone increases rapidly when the delay time is increased from 0 to 12.5 ps. It then decreases dramatically when the delay time is further increased to 30 ps. It has a small peak around 100 ps. For delay time up to 40 ns, the size of the heat-affected zone exceeds that for a delay time of 0 ps, whereas for delay time over 60 ps, it becomes smaller than that for a delay time of 0 ps. The bonding strength exhibits the same tendency. The underlying physical mechanism is discussed in terms of initial electron excitation by the first pulse and subsequent excitation by the second pulse: specifically, the first pulse induces multiphoton ionization or tunneling ionization, while the second pulse induces electron heating or avalanche ionization or the second pulse is absorbed by the localized state. Transient absorption of glass induced by the ultrafast laser pulse was analyzed by an ultrafast pump-probe technique. We found that the optimum pulse energy ratio is unity. These results provide new insights into high-efficiency ultrafast laser microwelding of glass and suggest new possibilities for further development of other ultrafast laser processing techniques.

Resolving vibrational wave-packet dynamics of D2(+) using multicolor probe pulses.

We demonstrate the generation and real-time observation of the vibrational wave packet of D(2)(+) by using a sub-10-fs extreme UV high-harmonic pump pulse and a three-color probe laser pulse whose wavelength ranges from near-IR to vacuum UV. This multicolor pump-probe scheme can provide us with a powerful experimental tool for investigating a variety of wave packets evolving with a time scale of ~20 fs.

Dual-chirped optical parametric amplification for generating few hundred mJ infrared pulses.

An ultrafast high-power infrared pulse source employing a dual-chirped optical parametric amplification (DC-OPA) scheme based on a Ti:sapphire pump laser system is theoretically investigated. By chirping both pump and seed pulses in an optimized way, high-energy pump pulses can be utilized for a DC-OPA process without exceeding the damage threshold of BBO crystals, and broadband signal and idler pulses at 1.4 µm and 1.87 µm can be generated with a total conversion efficiency approaching 40%. Furthermore, few-cycle idler pulses with a passively stabilized carrier-envelope phase (CEP) can be generated by the difference frequency generation process in a collinear configuration. DC-OPA, a BBO-OPA scheme pumped by a Ti:sapphire laser, is efficient and scalable in output energy of the infrared pulses, which provides us with the design parameters of an ultrafast infrared laser system with an energy up to a few hundred mJ.

Temporal control of local plasmon distribution on Au nanocrosses by ultra-broadband femtosecond laser pulses and its application for selective two-photon excitation of multiple fluorophores.

We theoretically demonstrate spatiotemporal control of local plasmon distribution on Au nanocrosses, which have different aspect ratios, by chirped ultra-broadband femtosecond laser pulses. We also demonstrate selective excitation of fluorescence proteins using this spatiotemporal local plasmon control technique for applications to two-photon excited fluorescence microscopy.