Single-shot, high-repetition rate carrier-envelope-phase detection of ultrashort laser pulses.

We propose a single-shot, high-repetition rate measurement scheme of the carrier-envelope phase offset of ultrashort laser pulses. The spectral fringes resulting from f-2f nonlinear interferometry, encoding the carrier-envelope-phase, are evaluated completely optically via an optical Fourier transform. For demonstration, the carrier-envelope-phase of a 200 kHz, few-cycle optical parametric chirped-pulse amplification (OPCPA) laser system was measured employing an interferometer as a periodic optical filter. The proposed method shows excellent agreement with simultaneous measurement of the spectral fringes by a fast line-scan camera.

Few-cycle all-fiber supercontinuum laser for ultrabroadband multimodal nonlinear microscopy.

Temporally coherent supercontinuum sources constitute an attractive alternative to bulk crystal-based sources of few-cycle light pulses. We present a monolithic fiber-optic configuration for generating transform-limited temporally coherent supercontinuum pulses with central wavelength at 1.06 µm and duration as short as 13.0 fs (3.7 optical cycles). The supercontinuum is generated by the action of self-phase modulation and optical wave breaking when pumping an all-normal dispersion photonic crystal fiber with pulses of hundreds of fs duration produced by all-fiber chirped pulsed amplification. Avoidance of free-space propagation between stages confers unequalled robustness, efficiency and cost-effectiveness to this novel configuration. Collectively, the features of all-fiber few-cycle pulsed sources make them powerful tools for applications benefitting from the ultrabroadband spectra and ultrashort pulse durations. Here we exploit these features and the deep penetration of light in biological tissues at the spectral region of 1 µm, to demonstrate their successful performance in ultrabroadband multispectral and multimodal nonlinear microscopy.

Sub-10-fs observation of bound exciton formation in organic optoelectronic devices.

Fundamental mechanisms underlying exciton formation in organic semiconductors are complex and elusive as it occurs on ultrashort sub-100-fs timescales. Some fundamental aspects of this process, such as the evolution of exciton binding energy, have not been resolved in time experimentally. Here, we apply a combination of sub-10-fs Pump-Push-Photocurrent, Pump-Push-Photoluminescence, and Pump-Probe spectroscopies to polyfluorene devices to track the ultrafast formation of excitons. While Pump-Probe is sensitive to the total concentration of excited states, Pump-Push-Photocurrent and Pump-Push-Photoluminescence are sensitive to bound states only, providing access to exciton binding dynamics. We find that excitons created by near-absorption-edge photons are intrinsically bound states, or become such within 10 fs after excitation. Meanwhile, excitons with a modest >0.3 eV excess energy can dissociate spontaneously within 50 fs before acquiring bound character. These conclusions are supported by excited-state molecular dynamics simulations and a global kinetic model which quantitatively reproduce experimental data.

Temporal characterization of broadband femtosecond laser pulses by surface third-harmonic dispersion scan with ptychographic retrieval.

We present a new, to the best of our knowledge, variant of dispersion scan (d-scan) based on surface third-harmonic generation (STHG) and a ptychographic algorithm tailored for full retrieval (amplitude and phase) of broadband laser pulses. We demonstrate the technique by temporally measuring and compressing few-cycle pulses with 7 fs and 2.5 nJ from a Ti:sapphire oscillator, using a sapphire window as the nonlinear medium. The results are in very good agreement with standard second-harmonic d-scan measurements based on a nonlinear crystal. The intrinsically broadband and phase-matching-independent nature of STHG make this technique very suitable for the characterization of ultrashort laser pulses over a broad wavelength range extending into the mid-infrared.

Dynamical behaviour of ultrathin [CoFeB (tCoFeB)/Pd] films with perpendicular magnetic anisotropy.

CoFeB-based ultrathin films with perpendicular magnetic anisotropy are promising for different emerging technological applications such as nonvolatile memories with low power consumption and high-speed performance. In this work, the dynamical properties of [CoFeB (tCoFeB)/Pd (10 Å)]5 multilayered ultrathin films (1 Å ≤ tCoFeB ≤ 5 Å) are studied by using two complementary methods: time-resolved magneto-optical Kerr effect and broadband ferromagnetic resonance. The perpendicular magnetization is confirmed for multilayers with tCoFeB ≤ 4 Å. The effective perpendicular magnetic anisotropy reaches a clear maximum at tCoFeB = 3 Å. Further increase of CoFeB layer thickness reduces the perpendicular magnetic anisotropy and the magnetization became in-plane oriented for tCoFeB ≥ 5 Å. This behaviour is explained by considering competing contributions from surface and magnetoelastic anisotropies. It was also found that the effective damping parameter αeff decreases with CoFeB layer thickness and for tCoFeB = 4 Å reaches a value of ~ 0.019 that is suitable for microwave applications.

Detection and elimination of pulse train instabilities in broadband fibre lasers using dispersion scan.

We use self-calibrating dispersion scan to experimentally detect and quantify the presence of pulse train instabilities in ultrashort laser pulse trains. We numerically test our approach against two different types of pulse instability, namely second-order phase fluctuations and random phase instability, where the introduction of an adequate metric enables univocally quantifying the amount of instability. The approach is experimentally demonstrated with a supercontinuum fibre laser, where we observe and identify pulse train instabilities due to nonlinear propagation effects under anomalous dispersion conditions in the photonic crystal fibre used for spectral broadening. By replacing the latter with an all-normal dispersion fibre, we effectively correct the pulse train instability and increase the bandwidth of the generated coherent spectrum. This is further confirmed by temporal compression and measurement of the output pulses down to 15 fs using dispersion scan.

SyncRGB-FLIM: synchronous fluorescence imaging of red, green and blue dyes enabled by ultra-broadband few-cycle laser excitation and fluorescence lifetime detection.

We demonstrate for the first time that an ultra-broadband 7 femtosecond (fs) few-cycle laser can be used for multicolor nonlinear imaging in a single channel detection geometry, when employing a time-resolved fluorescence detection scheme. On a multi-chromophore-labelled cell sample we show that the few-cycle laser can efficiently excite the multiple chromophores over a >400 nm two-photon absorption range. By combining the few-cycle laser excitation with time-correlated single-photon counting (TCSPC) detection to record two-photon fluorescence lifetime imaging microscopy (FLIM) images, the localization of different chromophores in the cell can be identified based on their fluorescence decay properties. The novel SyncRGB-FLIM multi-color bioimaging technique opens the possibility of real-time protein-protein interaction studies, where its single-scan operation translates into reduced laser exposure of the sample, resulting in more photoprotective conditions for biological specimens.

Simultaneous measurement of two ultrashort near-ultraviolet pulses produced by a multiplate continuum using dual self-diffraction dispersion-scan.

We present a new method based on self-diffraction dispersion-scan (SD d-scan) that enables the simultaneous measurement of two distinct ultrashort laser pulses in a region where they spatially and temporally overlap. This situation can arise when sampling and focusing two different spatial portions of a single inhomogeneous beam onto a medium. We demonstrate this new dual SD d-scan method by simultaneously characterizing two intense broadband ultraviolet pulses at 400 nm, with durations in the 10 fs range, originating from two different spatial portions of a beam produced by a multiplate continuum (MPC).

All-optical measurement of the complete waveform of octave-spanning ultrashort light pulses.

We demonstrate the complete temporal characterization of the optical waveform of visible near-infrared octave-spanning ultrashort laser pulses, using an all-optical, all-solid-state, and fully inline dispersion-scan device based only on second-harmonic generation.

Self-calibrating d-scan: measuring ultrashort laser pulses on-target using an arbitrary pulse compressor.

In most applications of ultrashort pulse lasers, temporal compressors are used to achieve a desired pulse duration in a target or sample, and precise temporal characterization is important. The dispersion-scan (d-scan) pulse characterization technique usually involves using glass wedges to impart variable, well-defined amounts of dispersion to the pulses, while measuring the spectrum of a nonlinear signal produced by those pulses. This works very well for broadband few-cycle pulses, but longer, narrower bandwidth pulses are much more difficult to measure this way. Here we demonstrate the concept of self-calibrating d-scan, which extends the applicability of the d-scan technique to pulses of arbitrary duration, enabling their complete measurement without prior knowledge of the introduced dispersion. In particular, we show that the pulse compressors already employed in chirped pulse amplification (CPA) systems can be used to simultaneously compress and measure the temporal profile of the output pulses on-target in a simple way, without the need of additional diagnostics or calibrations, while at the same time calibrating the often-unknown differential dispersion of the compressor itself. We demonstrate the technique through simulations and experiments under known conditions. Finally, we apply it to the measurement and compression of 27.5 fs pulses from a CPA laser.

Strategies for achieving intense single-cycle pulses with in-line post-compression setups.

Intense few- and single-cycle pulses are powerful tools in different fields of science Today, third- and higher-order terms in the remnant spectral phase of the pulses remain a major obstacle for obtaining high-quality few- and single-cycle pulses from in-line post-compression setups. In this Letter, we show how input pulse shaping can successfully be applied to standard post-compression setups to minimize the occurrence of high-order phase components during nonlinear propagation and to directly obtain pulses with durations down to 3 fs. Furthermore, by combining this pulse shaping of the input pulse with new-generation broadband chirped mirrors and material addition for remnant third-order phase correction, pulses down to 2.2 fs duration have been measured.

Inline self-diffraction dispersion-scan of over octave-spanning pulses in the single-cycle regime.

We present an implementation of dispersion-scan based on self-diffraction (SD d-scan) and apply it to the measurement of over octave-spanning sub-4-fs pulses. The results are compared with second-harmonic generation (SHG) d-scan. The efficiency of the SD process is derived theoretically and compared with the spectral response retrieved by the d-scan algorithm. The new SD d-scan has a robust inline setup and enables measuring pulses with over-octave spectra, single-cycle durations, and wavelength ranges beyond those of SHG crystals, such as the ultraviolet and the deep-ultraviolet.

Simultaneous compression, characterization and phase stabilization of GW-level 1.4 cycle VIS-NIR femtosecond pulses using a single dispersion-scan setup.

We have temporally characterized, dispersion compensated and carrier-envelope phase stabilized 1.4-cycle pulses (3.2 fs) with 160 µJ of energy at 722 nm using a minimal and convenient dispersion-scan setup. The setup is all inline, does not require interferometric beamsplitting, and uses components available in most laser laboratories. Broadband minimization of third-order dispersion using propagation in water enabled reducing the compressed pulse duration from 3.8 to 3.2 fs with the same set of chirped mirrors. Carrier-envelope phase stabilization of the octave-spanning pulses was also performed by the dispersion-scan setup. This unprecedentedly simple and reliable approach provides reproducible CEP-stabilized pulses in the single-cycle regime for applications such as CEP-sensitive spectroscopy and isolated attosecond pulse generation.

Spatiotemporal characterization of few-cycle laser pulses.

In this paper we apply a broadband fiber optic coupler interferometer to the measurement of few-cycle laser pulses. Sub-8-fs pulses delivered by an ultrafast oscillator were characterized spatiotemporally using STARFISH, which is based on spatially resolved spectral interferometry. The reference pulse was measured with the d-scan technique. The pulses were focused by an off-axis parabolic mirror and were characterized at different transverse planes along the focusing region. The evolution of the retrieved pulses is analyzed, exhibiting small variations in the temporal (and spectral) amplitude and phase during propagation. Finally, the peak irradiance evolution is estimated from the integration of the spatiotemporal intensity.

Characterization of broadband few-cycle laser pulses with the d-scan technique.

We present an analysis and demonstration of few-cycle ultrashort laser pulse characterization using second-harmonic dispersion scans and numerical phase retrieval algorithms. The sensitivity and robustness of this technique with respect to noise, measurement bandwidth and complexity of the measured pulses is discussed through numerical examples and experimental results. Using this technique, we successfully demonstrate the characterization of few-cycle pulses with complex and structured spectra generated from a broadband ultrafast laser oscillator and a high-energy hollow fiber compressor.

Simultaneous compression and characterization of ultrashort laser pulses using chirped mirrors and glass wedges.

We present a simple and robust technique to retrieve the phase of ultrashort laser pulses, based on a chirped mirror and glass wedges compressor. It uses the compression system itself as a diagnostic tool, thereby making unnecessary the use of complementary diagnostic tools. We used this technique to compress and characterize 7.1 fs laser pulses from an ultrafast laser oscillator.

Generation of high-energy vacuum UV femtosecond pulses by multiple-beam cascaded four-wave mixing in a transparent solid.

The generation of ultrashort vacuum UV (VUV) pulses by nondegenerate cascaded four-wave mixing of femtosecond pulses in a thin slide of a large band-gap transparent solid is numerically demonstrated. Using a novel noncollinear multiple-beam configuration, cascaded four-wave mixing of amplified 30 fs Ti:sapphire laser pulses at 800 nm, and their second harmonic in lithium fluoride results in the generation of VUV radiation down to 134 nm with energies in the µJ range and durations comparable to those of the pump pulses. The proposed geometry is advantageous in large dispersion scenarios, namely for generating radiation close to absorption bands. Hence these results set this technique as a promising way to efficiently generate ultrashort VUV radiation in solids for several applications in science and technology.

Octave-spanning spectra and pulse synthesis by nondegenerate cascaded four-wave mixing.

We present a theoretical model and 2D numerical simulation of cascaded four-wave mixing of femtosecond pulses in bulk chi((3)) media, evidencing the importance of 2D interaction geometries in the efficient generation of frequency-converted pulses. Octave-spanning spectra and pulse synthesis down to the sub-two-cycle regime is demonstrated without the need for complex amplitude or phase control, in agreement with experimental measurements.