Noncollinear Optical Parametric Amplifier Research Articles

Fluorescence-Encoded Time-Domain Coherent Raman Spectroscopy in the Visible Range.

Fluorescence-encoded vibrational spectroscopy has attracted increasing attention by virtue of its high sensitivity and high chemical specificity. We recently demonstrated fluorescence-encoded time-domain coherent Raman spectroscopy (FLETCHERS), which enables low-frequency vibrational spectroscopy of low-concentration fluorophores using near-infrared (800-900 nm) light excitation. However, the feasibility of this study was constrained by the scarcity of excitable molecules in the near-infrared range. Consequently, the broader applicability of FLETCHERS has not been investigated. Here we extend the capabilities of FLETCHERS into the visible range by employing a noncollinear optical parametric amplifier as a light source, significantly enhancing its versatility. Specifically, we use the method, which we refer to as visible FLETCHERS (vFLETCHERS), to individually acquire Raman spectra from five visible fluorophores that have absorption peaks in the 600-700 nm region. These results not only confirm the versatility of vFLETCHERS for a wide range of molecules but also allude to its widespread applicability in biological research through highly sensitive supermultiplexed imaging.

Vortex plate retarder-based approach for the generation of sub-20 fs light pulses carrying orbital angular momentum

We use a vortex retarder-based approach to generate few optical cycles light pulses carrying orbital angular momentum (OAM) (known also as twisted light or optical vortex) from a Yb:KGW oscillator pumping a noncollinear optical parametric amplifier generating sub-10 fs linearly polarized light pulses in the near infrared spectral range (central wavelength 850 nm). We characterize such vortices both spatially and temporally by using astigmatic imaging technique and second harmonic generation-based frequency resolved optical gating, respectively. The generation of optical vortices is analyzed, and its structure reconstructed by estimating the spatio-spectral field and Fourier transforming it into the temporal domain. As a proof of concept, we show that we can also generate sub-20 fs light pulses carrying OAM and with arbitrary polarization on the first-order Poincaré sphere.

Spatiotemporal dispersion compensation for a 200-THz noncollinear optical parametric amplifier.

A noncollinear optical parametric amplifier (NOPA) can produce few-cycle femtosecond laser pulses that are ideally suited for time-resolved optical spectroscopy measurements. However, the nonlinear-optical process giving rise to ultrabroadband pulses is susceptible to spatiotemporal dispersion problems. Here, we detail refinements, including chirped-pulse amplification (CPA) and pulse-front matching (PFM), that minimize spatiotemporal dispersion and thereby improve the properties of ultrabroadband pulses produced by a NOPA. The description includes a rationale behind the choices of optical and optomechanical components, as well as assessment protocols. We demonstrate these techniques using a 1kHz, second-harmonic Ti:sapphire pump configuration, which produces ∼5-fs duration pulses that span from about 500 to 800nm with a bandwidth of about 200THz. To demonstrate the utility of the CPA-PFM-NOPA, we measure vibrational quantum beats in the transient-absorption spectrum of methylene blue, a dye molecule that serves as a reference standard.

Femtosecond fluorescence conical optical parametric amplification spectroscopy.

Parametric superfluorescence (PSF), which originated from the optical amplification of vacuum quantum noise, is the primary noise source of femtosecond fluorescence non-collinear optical parametric amplification spectroscopy (FNOPAS). It severely affects the detection limit of FNOPAS to collect the femtosecond time-resolved spectra of extremely weak fluorescence. Here, we report the development of femtosecond fluorescence conical optical parametric amplification spectroscopy (FCOPAS), aimed at effectively suppressing the noise fluctuation from the PSF background. In contrast to traditional FNOPAS configurations utilizing lateral fluorescence collection and dot-like parametric amplification, FCOPAS employs an innovative conical fluorescence collection and ring-like amplification setup. This design enables effective cancellation of noise fluctuation across the entire PSF ring, resulting in an approximate order of magnitude reduction in PSF noise compared to prior FNOPAS outcomes. This advancement enables the resolution of transient fluorescence spectra of 4-dicyanomethylene-2-methyl-6-p-dimethylaminostyryl-4H-pyran (DCM) dye molecules in ethanol, even at an optically dilute concentration of 10-6 mol/l, with significantly enhanced signal-to-noise ratios. This improvement will be significant for extremely weak fluorescence detection on the femtosecond time scale.

Noncollinear Optical Parametric Amplification of Broadband Infrared Sum Frequency Generation Vibrational Spectroscopy.

Sum-frequency generation (SFG) vibrational spectroscopy is an invaluable tool in surface science, known for its specificity to surfaces and interfaces. Despite its wide application, it is often hampered by weak signal detection. Here, we present an innovative enhancement technique of postsample amplification, using a picosecond noncollinear optical parametric amplifier (NOPA). We conducted a systematical investigation into the impact of different intensities of pump and SFG seed light, as the input signal in NOPA, and demonstrated this method on the octadecanethiol (ODT) molecules on gold films. The amplified SFG by NOPA reproduced the SFG vibrational spectra, enhanced by about 4 orders of magnitude but with broader spectral resolution due to the short pulse width of the pump light in NOPA. This study makes it possible to realize highly sensitive SFG measurements, marking a significant advancement in spectroscopic analysis techniques.

Measurement of three-photon excitation cross-sections of fluorescein from 1154 nm to 1500 nm.

Measurements of three-photon action cross-sections for fluorescein (dissolved in water, pH ∼11.5) are presented in the excitation wavelength range from 1154 to 1500 nm in ∼50 nm steps. The excitation source is a femtosecond wavelength tunable non-collinear optical parametric amplifier, which has been spectrally filtered with 50 nm full width at half maximum band pass filters. Cube-law power dependance is confirmed at the measurement wavelengths. The three-photon excitation spectrum is found to differ from both the one- and two-photon excitation spectra. The three-photon action cross-section at 1154 nm is more than an order of magnitude larger than those at 1450 and 1500 nm (approximately three times the wavelength of the one-photon excitation peak), which possibly indicates the presence of resonance enhancement.

Spatio-spectral couplings in optical parametric amplifiers.

Optical parametric amplification (OPA) is a powerful tool for the generation of ultrashort light pulses. However, under certain circumstances, it develops spatio-spectral couplings, color dependent aberrations that degrade the pulse properties. In this work, we present a spatio-spectral coupling generated by a non-collimated pump beam and resulting in the change of direction of the amplified signal with respect to the input seed. We experimentally characterize the effect, introduce a theoretical model to explain it as well as reproduce it through numerical simulations. It affects high-gain non-collinear OPA configurations and becomes especially relevant in sequential optical parametric synthesizers. In collinear configuration, however, beyond the direction change, also angular and spatial chirp is produced. We obtain with a synthesizer about 40% decrease in peak intensity in the experiments and local elongation of the pulse duration by more than 25% within the spatial full width at half maximum at the focus. Finally, we present strategies to correct or mitigate the coupling and demonstrate them in two different systems. Our work is important for the development of OPA-based systems as well as few-cycle sequential synthesizers.

Generation of 2 μm few-cycle laser pulse with dual laser filaments nonlinear processes

For the first time, we propose a new scheme for generating few-cycle 2 μm seed laser pulse in an optical parametric chirped pulse amplifier (OPCPA) front-end. The 2 μm ultrafast seed laser pulse is generated via a difference frequency generation (DFG) process between the visible and near-IR supercontinuum from two different filamentation processes inside the transparent YAG crystals. The generated DFG pulse spectrum has a broad spectrum range of 1200 nm from 1500 nm to 2700 nm. By further scaling up the pulse energy of the seed laser pulse via a non-collinear optical parametric amplification (OPA) stage, the single pulse energy is boosted to 15.6 μJ. After dispersion compensation, the pulse duration is compressed to 14.3 fs with its spectrum covering from 1600 nm to 2600 nm.

Demonstration of a petawatt-scale optical parametric chirped pulse amplifier based on yttrium calcium oxyborate

Abstract As optical parametric chirped pulse amplification has been widely adopted for the generation of extreme intensity laser sources, nonlinear crystals of large aperture are demanded for high-energy amplifiers. Yttrium calcium oxyborate (YCa4O(BO3)3, YCOB) is capable of being grown with apertures exceeding 100 mm, which makes it possible for application in systems of petawatt scale. In this paper, we experimentally demonstrated for the first time to our knowledge, an ultra-broadband non-collinear optical parametric amplifier with YCOB for petawatt-scale compressed pulse generation at 800 nm. Based on the SG-II 5 PW facility, amplified signal energy of approximately 40 J was achieved and pump-to-signal conversion efficiency was up to 42.3%. A gain bandwidth of 87 nm was realized and supported a compressed pulse duration of 22.3 fs. The near-field and wavefront aberration represented excellent characteristics, which were comparable with those achieved in lithium triborate-based amplifiers. These results verified the great potential for YCOB utilization in the future.

Angular dispersion compensation for ultra-broadband pulses by using a cascaded prism and hollow-core fiber configuration.

In this paper, we report that the angular dispersion of the output pulses in a nonlinear process can be efficiently compensated by using a cascaded prism(s) and short hollow-core fiber (HCF) configuration. Here, the prism(s) is used to suppress the angular dispersion and transform it into spatial chirp, while the HCF is used for removing this spatial chirp and the residual angular dispersion, which can also significantly improve the beam quality. The feasibility of this novel method is numerically and experimentally investigated with the ultra-broadband idler pulses centered at 1250 nm wavelength and generated by an LBO crystal based non-collinear optical parametric amplifier. The proof-of-principle experiment shows that the angular dispersion can be effectively removed and ultra-broadband idler pulses with good spectral quality and spatial profile can be obtained. The total transmission efficiency in the experiment is around 67% and the measured M x2 and M y2 can reach 1.12 and 1.04, respectively. To the best of our knowledge, this is the first reported ultra-broadband angular dispersion compensation scheme combining prism(s) and HCF, which can remarkably eliminate the angular dispersion while simultaneously possesses high efficiency, good spectral and beam spatial quality.

Transient absorption microscopy setup with multi-ten-kilohertz shot-to-shot subtraction and discrete Fourier analysis.

Recording of transient absorption microscopy images requires fast detection of minute optical density changes, which is typically achieved with high-repetition-rate laser sources and lock-in detection. Here, we present a highly flexible and cost-efficient detection scheme based on a conventional photodiode and an USB oscilloscope with MHz bandwidth, that deviates from the commonly used lock-in setup and achieves benchmark sensitivity. Our scheme combines shot-to-shot evaluation of pump-probe and probe-only measurements, a home-built photodetector circuit optimized for low pulse energies applying low-pass amplification, and a custom evaluation algorithm based on Fourier transformation. Advantages of this approach include abilities to simultaneously monitor multiple pulse modulation frequencies, implement the detection of additional pulse sequences (e.g., pump-only), and expand to multiple parallel detection channels for wavelength-dispersive probing. With a 40 kHz repetition-rate laser system powering two non-collinear optical parametric amplifiers for wide tuneability, we find that laser pulse fluctuations limit the sensitivity of the setup, while the detection scheme has negligible contribution. We demonstrate the 2-D imaging performance of our transient absorption microscope with studies on micro-crystalline molecular thin films.

Ultrashort near-infrared pulse generation by non-collinear optical parametric amplification in LiInS2

We demonstrate non-collinear optical parametric amplification (NOPA) in LiInS2 to generate ultrashort near-infrared pulses. White light pulses around 1400 nm generated in yttrium aluminum garnet are amplified by five orders of magnitude up to 1.0 µJ by three-stage NOPA in LiInS2. The dispersion of the amplified pulses is compensated by an acousto-optic programmable dispersive filter, resulting in the pulse compression down to 40 fs, which is 1.1 times the pulse width of the Fourier-transform limited pulse. The successful demonstration of NOPA in LiInS2 indicates the possibility as a new light source to obtain high peak intensity which enables us to access the regime of non-perturbative physics.

Modulated Noncollinear Optical Parametric Amplifier Output Induced by Stimulated Raman Scattering

We studied spectra of the amplified signal from a noncollinear optical parametric amplifier (NOPA) based on a Ti:sapphire laser and BBO crystal gain medium. The signal shows characteristic structures with periodic intensity variations in the signal during the parametric amplification processes in a BBO crystal. This phenomenon is attributed to the stimulated Raman process excited by the pump pulse affected by the phase-matching condition of four-wave mixing. The effect of this stimulated Raman process on optical parametric amplification and on final pulse compression of the signal was analyzed. The results demonstrate that caution must be taken when constructing a NOPA. Specifically, great care must be taken not to use mirrors with non-uniform spectral reflectivity for obtaining a stable pulse in terms of both temporal and spectral shapes.

Single 3.3 fs multiple plate compression light source in ultrafast transient absorption spectroscopy

Ultrafast transient absorption spectroscopy is a powerful tool to reveal excited state dynamics in various materials. Conventionally, probe pulses are generated via bulk supercontinuum generation or (noncollinear) optical parametric amplifiers whilst pump pulses are generated separately using (noncollinear) optical parametric amplifiers. These systems are limited by either their spectral density, stability, spectral range, and/or temporal compressibility. Recently, a new intense broadband light source is being developed, the multi-plate compression, which promises to overcome these limitations. In this paper, we analyze the supercontinuum generated by a single Multiple Plate Compression system to set a benchmark for its use in the field of ultrafast pump-probe spectroscopy. We have compressed the supercontinuum to 3.3 fs using chirp mirrors alone, making it an excellent candidate for pump-probe experiments requiring high temporal resolution. Furthermore, the single light source can be used to generate both probe and pump pulses due to its high spectral density (>14.5 nJ/nm) between 490 and 890 nm. The intensity has an average shot-to-shot relative standard deviation of 4.6 % over 490 to 890 nm, calculated over 2,000 sequential shots. By using only 1,000 shot pairs, a Delta T/T noise level of 2.6times 10^{-4} RMS is achieved. Finally, as a proof of concept, the transient absorption spectrum of a methylammonium lead iodide perovskite film is taken, showing great signal to noise with only 1,000 shot pairs. These results show great potential for the employment of this technique in other spectroscopic techniques such as coherent multidimensional spectroscopy.

Simulating an ultra-broadband concept for Exawatt-class lasers

The rapid development of the optical-cycle-level ultra-fast laser technologies may break through the bottleneck of the traditional ultra-intense laser [i.e., Petawatt (PW, 1015 W) laser currently] and enable the generation of even higher peak-power/intensity lasers. Herein, we simulate an ultra-broadband concept for the realization of an Exawatt-class (EW, 1018 W) high peak-power laser, where the wide-angle non-collinear optical parametric chirped-pulse amplification (WNOPCPA) is combined with the thin-plate post-compression. A frequency-chirped carrier-envelope-phase stable super-continuum laser is amplified to high-energy in WNOPCPA by pumping with two pump-beamlets and injected into the thin-plate post-compression to generate a sub-optical-cycle high-energy laser pulse. The numerical simulation shows this hybrid concept significantly enhances the gain bandwidth in the high-energy amplifier and the spectral broadening in the post-compression. By using this concept, a study of a prototype design of a 0.5 EW system is presented, and several key challenges are also examined.

Switching resonance character within merocyanine stacks and its impact on excited-state dynamics

Summary In this study, the optical properties and excited-state dynamics of the unique self-assembled donor-acceptor (DA) merocyanine dye stacks from dimer up to octamer, prepared via dipole-dipole interactions, are reported in terms of coherent exciton dynamics and formation of an excimer-like state. Our findings are based on the steady-state absorption/emission, time-resolved fluorescence, and transient absorption (anisotropy) measurements, including wavepacket analysis and quantum mechanical calculations. Coherent exciton of torsional motions-restricted dye stacks rapidly localizes into the weakly emissive excimer-like state, by shortening the inter-moiety distance and changing the bond-length alternation pattern. The inner merocyanine moiety, having two neighboring units, has a reversed resonance character (non-polar (N) Z) in the ground state. This difference has led to two conclusions: (1) tetramers and octamers exhibit different features of excimer-like state than the dimer, and (2) octamers exhibit slower localization dynamics due to the enhanced homogeneity (six inner-moieties) compared with tetramers (two inner moieties).

High-spatial-resolution ultrafast framing imaging at 15 trillion frames per second by optical parametric amplification

We report a framing imaging based on noncollinear optical parametric amplification (NCOPA), named FINCOPA, which applies NCOPA for the first time to single-shot ultrafast optical imaging. In an experiment targeting a laser-induced air plasma grating, FINCOPA achieved 50 fs-resolved optical imaging with a spatial resolution of ∼83 lp / mm and an effective frame rate of 10 trillion frames per second (Tfps). It has also successfully visualized an ultrafast rotating optical field with an effective frame rate of 15 Tfps. FINCOPA has simultaneously a femtosecond-level temporal resolution and frame interval and a micrometer-level spatial resolution. Combining outstanding spatial and temporal resolutions with an ultrahigh frame rate, FINCOPA will contribute to high-spatiotemporal resolution observations of ultrafast transient events, such as atomic or molecular dynamics in photonic materials, plasma physics, and laser inertial-confinement fusion.

Generation and characterisation of few-pulse attosecond pulse trains at 100 kHz repetition rate

The development of attosecond pump–probe experiments at high repetition rate requires the development of novel attosecond sources maintaining a sufficient number of photons per pulse. We use 7 fs, 800 nm pulses from a non-collinear optical parametric chirped pulse amplification laser system to generate few-pulse attosecond pulse trains (APTs) with a flux of >106 photons per shot in the extreme ultraviolet at a repetition rate of 100 kHz. The pulse trains have been fully characterised by recording frequency-resolved optical gating for complete reconstruction of attosecond bursts (FROG-CRAB) traces with a velocity map imaging spectrometer. For the pulse retrieval from the FROG-CRAB trace a new ensemble retrieval algorithm has been employed that enables the reconstruction of the shape of the APTs in the presence of carrier envelope phase fluctuations of the few-cycle laser system.

Few-cycle fs-pumped NOPA with passive ultrabroadband spectral shaping.

A compact, femtosecond-pumped noncollinear optical parametric amplifier (NOPA) is presented with a passive spectral shaping technique, employed to produce a flat-top-like ultrabroadband output spectrum. The NOPA is pumped by a dedicated 2 mJ, 120 fs Yb3+-based CPA system, which generates both the second harmonic pump pulse and white light supercontinuum as the signal pulse. A chirped mirror pair pre-compensates the material GVD within the optical path of the signal pulse to produce a near-FTL pulse duration at the OPA crystal output. By optimizing both the pump/signal cross angle and the pump/signal delay, the 40 cm × 40 cm footprint, single-pass, fs-pumped, direct NOPA (non-NOPCPA) system generates a record 20 µJ, 11 fs pulses at 820 nm central wavelength with a bandwidth of 230 nm FWHM, to be used as an ultrashort optical probe pulse for relativistic laser-plasma interactions at the petawatt-class POLARIS laser system.

Generation of Terawatt-Scale Vortex Pulses Based on Optical Parametric Chirped-Pulse Amplification

In this letter, we report the demonstration of terawatt (TW)-scale femtosecond vortex laser pulses based on noncollinear optical parametric chirped-pulse amplification (OPCPA) centered at 800 nm. To the best of our knowledge, this is the first experimental study of amplification for OPCPA-based vortex pulses to achieve a powerful ultrafast (TW-scale) vortex pulse output. In this experiment, a 0.5-mJ broadband chirped vortex pulse was amplified to 47 mJ with a 15-mm-long LiB3O5 crystal. The double-pass grating pair compressor with an efficiency of 65% maintained the beam vortex, and a pulse of width 30.1 fs was obtained, corresponding to a peak power of 1.02 TW. This laser can be used in studies on nonlinear optics and relativistic laser-plasma interactions, compact plasma-based accelerators, and light sources.