Femtosecond Source Research Articles

Different Photodissociation Mechanisms in Fe(CO)5 and Cr(CO)6 Evidenced with Femtosecond Valence Photoelectron Spectroscopy and Excited-State Molecular Dynamics Simulations.

Measured and calculated time-resolved photoelectron spectra and excited-state molecular dynamics simulations of photoexcited gas-phase molecules Fe(CO)5 and Cr(CO)6 are presented. Samples were excited with 266 nm pump pulses and probed with 23 eV photons from a femtosecond high-order harmonic generation source. Photoelectron intensities are seen to blue-shift as a function of time from binding energies characteristic of bound electronic excited states via dissociated-state energies toward the energies of the dissociated species for both Fe(CO)5 and Cr(CO)6, but differences are apparent. The excited-state and dissociation dynamics are found to be faster in Cr(CO)6 because the repopulation from bound excited to dissociative excited states is faster. This may be due to stronger coupling between bound and dissociative states in Cr(CO)6, a notion supported by the observation that the manifolds of bound and dissociative states overlap in a narrow energy range in this system.

Non-destructive detection of fructose solutions via Terahertz spectroscopy enhanced by Frequency Selective Surface (FSS)

Terahertz (THz) spectroscopy, combined with Frequency Selective Surfaces (FSS), is emerging as a powerful non-destructive technique for detecting and analysing the properties of biological samples. In this study, we explored the use of THz spectroscopy for detecting fructose solutions with concentrations ranging from 0.2 % to 10 %. Using femtosecond laser light sources, the THz transmission and absorption characteristics of fructose were investigated. The integration of FSS significantly enhanced the sensitivity of THz detection, yielding a 16 % improvement at 1.29 THz and 28 % at 1.67 THz. UV–Vis and Fourier Transform Infrared (FTIR) spectroscopy were employed to compare results with traditional methods, highlighting the superior sensitivity of THz spectroscopy, especially at low concentrations. The findings suggest that THz spectroscopy, enhanced by FSS, has strong potential for advancing non-invasive testing in biological and environmental applications.

Widely wavelength-tunable high-repetition-rate femtosecond pulse source with highest average power up to 28 W

We have proposed and demonstrated a high-repetition-rate ultrashort pulse fiber amplification system based on a wavelength-tunable oscillator. This fiber amplification system produces an average power exceeding 20 W in bursts of 200 pulses with a 578 MHz intra-burst pulse repetition rate and a 1 MHz burst repetition rate. The center wavelength of the amplified pulses can be tuned from 1030 to 1080 nm. By utilizing pre-chirp management nonlinear amplification technique, the achieved shortest pulse duration is 27 fs with an average power of 25 W at 1032 nm. For all the amplified pulses with different wavelengths, the pulse duration after optimal compression is below 60 fs. To the best of our knowledge, this is the first time that a widely wavelength-tunable high-power laser with a repetition rate exceeding 100 MHz and a pulse duration of several tens of femtoseconds has been realized. Additionally, using only common double-cladding Yb-doped fiber as the gain fiber, without any large-mode-area Yb-doped photonic crystal fiber or rod-type Yb-doped fiber, makes the system compact and reliable due to the simple fusion operation.

Photo-induced loss of H2 from H2S, CH4, H2O and SiH4, when and why is it possible

We have explored the possibility of forming H⋅ and H2 from H2S, CH4, H2O and SiH4 in a series of ab initio calculations. The key finding is that H2S can give rise to direct photolytic ultrafast formation of H2 This finding is in agreement with the available experimental data and is a result of a directed pathway that leads toward H2 formation at easily accessible wavelengths. It arises at the (conical) intersection between the two lowest-lying electronic states. This intersection is a result of the valence orbital interaction of the two hydrogen atoms. This interaction is becoming more favorable as the S-H bonds simultaneously becomes longer. The H-S σ-σ∗ bonding interaction cannot compete with the bond formation that takes place between the hydrogens as two bonds stretch simultaneously. For oxygen this interaction it predominant. The reason is that sulfur has a higher principal quantum number and the interaction with the 1s of hydrogen therefore is less favorable. The excited states that are involved in the H2 formation from H2S could be populated by, for example, a two-photon 400 nm excitation. The other hydrides have a more entangled potential energy landscape close to the Franck-Condon region in the direction of the reaction coordinate that leads to H2 loss and as a result the direct loss of a hydrogen atom is favored. A two-photon excitation could be induced by femtosecond laser pulses that at the same time is proposed as a future platform for sensing the H2S molecules with the backward transient absorption scheme. The implication would be that both sensing and photoinduced H2 formation could be in place at the same time which justifies the use of expensive femtosecond light sources getting “two for the price of one”.

165 MHz highly stable femtosecond Er:ZBLAN fiber laser operating at 2.8 µm.

Three-micrometer mid-infrared (MIR) femtosecond pulse sources with a high repetition rate (HRR) have potential applications in a number of fields such as biological imaging, optical frequency combs, and gas detection. In this paper, by optimizing the fiber length and the cavity structure, we demonstrated a highly stable, self-starting mode-locked fluoride fiber laser (MLFFL) with a fundamental repetition rate of ∼165 MHz and a signal-to-noise ratio (SNR) of 90 dB. As far as we know, this stands as the highest fundamental repetition rate ever acquired directly from an ultrafast MLFFL in the >2.5 µm MIR region. Stable 352-fs pulses at 2795 nm with an average output power of 392 mW and a low integrated relative intensity noise (RIN) of 0.018% [10 Hz, 10 MHz] were generated. The root mean square (RMS) power fluctuation is 0.17% over 2 h, which indicates excellent oscillator stability. This high-performance laser offers a practicable scheme both for scaling the repetition frequency in MIR MLFFLs and high-precision ultrafast applications at longer wavelengths.

Spatiotemporal walk-off and improved focusing of plasma THz sources.

High-field THz sources with peak field strengths exceeding MV/cm are essential for nonlinear THz spectroscopy and coherent control of matter on ultrafast time scales. Two-color femtosecond laser plasma sources employing long filamentation have been reported as providing single-cycle, >MV/cm fields, with multi-decade spanning bandwidth and polarization control, making them promising sources for such experiments. In this work, we report the observation of spatiotemporal spreading of the THz pulse when standard off-axis parabolic mirrors are used for collection and focusing of long filament plasma-based THz pulses. This produces a flying focus for THz light, with the axial focal region propagating at a velocity of 1/3 the speed of light. The THz emission is then subsequently spread over a temporal width of ∼10 ps, approximately 100 times the THz pulse duration detected by electro-optic sampling at any single point along the focus. The consequences of this non-ideal focusing are a potential and drastic overestimation of the peak THz electric field based on energy measurements, as well as significant phase noise arising from beam pointing fluctuations. We show that this spatiotemporal spreading can be minimized using a simple axicon lens that perfectly collimates the extended filament source, resulting in improved spatial and temporal focusing of the THz pulse.

790–1000 nm continuously-tunable fiber-based femtosecond laser source

We report a 790–1000 nm tunable femtosecond laser source by second harmonic generation (SHG) of a 1580–2000 nm soliton self-frequency shift (SSFS) fiber laser. The SSFS fiber laser with an all polarization-maintaining fiber configuration consists of passively mode-locked figure-9 Er-doped fiber oscillator, two-stage fiber amplifiers and a nonlinear fiber, delivering femtosecond Raman solitons in a tunable range of 1580 to 2016 nm. The tunable Raman solitons are further injected into a specifically-designed chirped periodically-poled lithium niobite (CPPLN) crystal for efficient SHG, and therefore femtosecond pulses with wide wavelength tuning from 790 to 1000 nm are obtained. The shortest pulse duration is < 100 fs at 890 nm, and the average power is 7.55 mW with a repetition rate of 44.9 MHz. This is, to the best of our knowledge, the first demonstration of a < 1000 nm broadband tunable fiber-based femtosecond source almost covering the whole short-wavelength near-infrared spectrum, which may have important applications in the nonlinear microscopy, biomedical imaging, and material processing.

Ultrashort pulse biphoton source in lithium niobate nanophotonics at 2 μm.

Photonics offers unique capabilities for quantum information processing (QIP) such as room-temperature operation, the scalability of nanophotonics, and access to ultrabroad bandwidths and consequently ultrafast operation. Ultrashort pulse sources of quantum states in nanophotonics are an important building block for achieving scalable ultrafast QIP; however, their demonstrations so far have been sparse. Here, we demonstrate a femtosecond biphoton source in dispersion-engineered periodically poled lithium niobate nanophotonics. We measure 17 THz of bandwidth for the source centered at 2.09 µm, corresponding to a few optical cycles, with a brightness of 8.8 GHz/mW. Our results open new paths toward realization of ultrafast nanophotonic QIP.

Mean-field equation for phase-modulated optical parametric oscillator

The widely established techniques for the generation of ultrashort optical pulses rely on passive mode locking of lasers, with the output pulse duration and emission spectrum determined by the intrinsic lifetime of laser transition in the gain medium. Due to the instantaneous nature of nonlinear gain, optical parametric oscillators (OPOs) are capable of generating optical radiation in all timescales from continuous-wave (cw) to ultrashort femtosecond regime, if driven by laser pump sources in the corresponding time domain. In the ultrashort timescale, operation of OPOs conventionally relies on mode-locked pump lasers, with the concomitant disadvantages of large footprint and high cost. At the same time, the lack of gain storage mandates the use of synchronous pumping, resulting in increased complexity. In this paper, we present the concept of phase-modulated OPO driven by cw pump laser. The approach overcomes the traditional drawbacks of ultrafast OPOs, enabling femtosecond pulse generation without the need for synchronous pumping, resulting in a simplified, compact, and cost-effective architecture using cw input pump lasers. We derive a mean-field equation for a degenerate χ(2) OPO driven by a cw laser with intracavity electro-optic modulator (EOM), and also including dispersion compensation. The equation predicts the formation of stable femtosecond pulses (&lt;200fs), in both normal and anomalous dispersion regimes, with a controllable repetition rate determined by the frequency of the EOM. The remarkable functionality of the proposed scheme paves the way for the development of an alternative class of widely tunable coherent femtosecond light sources in both bulk and integrated format based on χ(2) OPOs using cw pump lasers. Published by the American Physical Society 2024

High-resolution MHz time- and angle-resolved photoemission spectroscopy based on a tunable vacuum ultraviolet source.

The time- and angle-resolved photoemission spectroscopy (trARPES) allows for direct mapping of the electronic band structure and its dynamic response on femtosecond timescales. Here, we present a new ARPES system, powered by a new fiber-based femtosecond light source in the vacuum ultraviolet range, accessing the complete first Brillouin zone for most materials. We present trARPES data on Au(111), polycrystalline Au, Bi2Se3, and TaTe2, demonstrating an energy resolution of 21meV with a time resolution of <360fs, at a high repetition rate of 1MHz. The system is integrated with an extreme ultraviolet high harmonic generation beamline, enabling an excellent tunability of the time-bandwidth resolution.

Bright continuously tunable vacuum ultraviolet source for ultrafast spectroscopy

Ultrafast electron dynamics drive phenomena such as photochemical reactions, catalysis, and light harvesting. To capture such dynamics in real-time, femtosecond to attosecond light sources are extensively used. However, an exact match between the excitation photon energy and a characteristic resonance is crucial. High-harmonic generation sources are advantageous in terms of pulse duration but limited in spectral tunability in the vacuum ultraviolet range. Here, we present a monochromatic femtosecond source continuously tunable around 21 eV photon energy utilizing the second harmonic of an optical parametric chirped pulse amplification laser system to drive high-harmonic generation. The unique tunability of the source is verified in an experiment probing the interatomic Coulombic decay in doped He nanodroplets across the He absorption bands. Moreover, we achieved intensities sufficient for driving collective processes in multiply excited helium nanodroplets, which have been previously observed only at free electron lasers.

Vacuum-free femtosecond fiber laser microplasma X-ray source for radiography.

Radiographic imaging using X-rays is a tool for basic research and applications in industry, materials science, and medical diagnostics. In this article, we present a novel approach for the generation of X-rays using a vacuum-free microplasma by femtosecond fiber laser. By tightly focusing a laser pulse onto a micrometer-sized solid density near-surface plasma from a rotating copper target, we demonstrate the generation of Cu K-photons (8-9 keV) with high yield ∼ 1.6 × 109 phot/s/2π, and with a source size diameter of approximately 10 microns. Femtosecond fiber laser allows working with a high repetition rate (∼2 MHz) and moderate energy levels (10-40 µJ), ensuring the effective quasi-continuous generation of X-ray photons. Furthermore, we introduce a hybrid scheme that combines the tightly focusing laser-plasma X-ray generator with an online control unit for microplasma size source based on the back-reflected second harmonic generated in the laser-induced microplasma. The compactness and high performance of this vacuum-free femtosecond fiber laser microplasma X-ray source makes it a promising solution for advanced radiographic applications. Our preliminary results on the creation of a microfocus X-ray source provide insights into the feasibility and potential of this innovative approach.

High-order femtosecond vortices up to the 30th order generated from a powerful mode-locked Hermite-Gaussian laser

Femtosecond vortex beams are of great scientific and practical interest because of their unique phase properties in both the longitudinal and transverse modes, enabling multi-dimensional quantum control of light fields. Until now, generating femtosecond vortex beams for applications that simultaneously require ultrashort pulse duration, high power, high vortex order, and a low cost and compact laser source has been very challenging due to the limitations of available generation methods. Here, we present a compact apparatus that generates powerful high-order femtosecond vortex pulses via astigmatic mode conversion from a mode-locked Hermite-Gaussian Yb:KGW laser oscillator in a hybrid scheme using both the translation-based off-axis pumping and the angle-based non-collinear pumping techniques. This hybrid scheme enables the generation of femtosecond vortices with a continuously tunable vortex order from the 1st up to the 30th order, which is the highest order obtained from any femtosecond vortex laser source based on a mode-locked oscillator. The average powers and pulse durations of all resulting vortex pulses are several hundred milliwatts and <650 fs, respectively. In particular, 424-fs 11th-order vortex pulses have been achieved with an average power of 1.6 W, several times more powerful than state-of-the-art oscillator-based femtosecond vortex sources.

Generation of 107 W, 1.07 mJ femtosecond pulses from chirped- and divided-pulse Sagnac Yb-fiber amplifiers by suppression of static mode degradation

We investigate the effect of static mode degradation (SMD) on the power scaling of mJ-level Sagnac Yb-fiber amplifiers. We find that SMD can be effectively suppressed by inserting a polarization-filtering device between two rod-type fibers. Consequently, the resulting amplifier system exhibits improved combining efficiency and average power, and it can deliver 240 fs pulses with 1.07 mJ energy and 107 W average power. This mJ femtosecond source of hundred-watt average power is of particular importance for high-field science applications.

Spectrally shaped and pulse-by-pulse multiplexed multimode squeezed states of light

Spectral- and time-multiplexing are currently explored to generate large multipartite quantum states of light for quantum technologies. In the continuous variable approach, the deterministic generation of scalable entangled states requires the generation of a scalable number of squeezed modes. Here, we demonstrate the simultaneous generation of 21 squeezed spectral modes at the repetition rate of our laser, i.e., 156 MHz. We exploit the full repetition rate and the pulse shaping of a femtosecond light source to combine, for the first time, frequency- and time-multiplexing in multimode squeezing. This paves the way for the implementation of multipartite entangled states that are both scalable and fully reconfigurable.

Widely Tunable Femtosecond Sources with Continuously Tailorable Bandwidth Enabled by Self‐Phase Modulation

AbstractGenerating ultrafast pulses with better spectrotemporal control is crucial for optimizing and characterizing nonlinear light–matter responses, yet it is limited by the gain bandwidth of laser media or the phase‐matching geometry of nonlinear processes. This work proposes a simple approach to independently manage a femtosecond source's spectral location and bandwidth. Self‐phase‐modulation‐enabled spectral broadening is first analyzed, which is potentially energy‐scalable using hollow‐core capillaries or multipass cells. It is demonstrated that the outmost lobes in the broadened spectrum show different dependencies on the initial pulse energy and duration. A simple yet effective toy model is introduced that successfully predicts broadband spectral tuning, and the impact of other nonlinear effects, dispersion, and input pulse asymmetry on the experimental scenario is also discussed. Thus a fiber‐based versatile source is demonstrated, which is compressible down to its transform‐limit duration, as short as 12.2 fs centered at 920 nm. In addition, bandwidth‐dependent third‐harmonic generation spectroscopy is performed from a dielectric metasurface with an optimized nonlinear response, and the dependency of laser bandwidth and pulse duration is investigated on the signal‐to‐background ratio of two‐photon images. It is believed that this demonstration will advance the investigation of bandwidth‐dependent nonlinear spectroscopy and microscopy.

Femtosecond IR and UV laser induced periodic structures on steel and copper surfaces

We analyze in detail laser induced periodic surface structures (LIPSS) on steel and copper surfaces. The chosen metals exhibit extreme differences between their thermal conductivity values, which determines the rate of extinguishing of the laser-induced temperature modulation on the surface. Two wavelengths of femtosecond laser radiation sources in IR and UV spectral range were used to inscribe low spatial frequency LIPSS. Regular LIPSS were successfully formed on steel samples for both wavelengths and it was observed that their regularity decreased with shorter wavelength used to induce the structures. For copper samples, LIPSS of considerably lower regularity were formed and even absent for one of the used scanning method at UV wavelength. Experimental results were analyzed in view of the numerical solution of the 2D heat diffusion equation for induced temperature on the surface. It was found that the temperature modulation decreased considerably faster (lasting tens of picoseconds) in copper, and (additionally) the decrease of the modulation is faster at the higher modulation frequency.

Intensity noise in difference frequency generation-based tunable femtosecond MIR sources.

We characterize the intensity noise of two mid-infrared (MIR) ultrafast tunable (3.5-11 μm) sources based on difference frequency generation (DFG). While both sources are pumped by a high repetition rate Yb-doped amplifier delivering 200 μJ 300 fs at a central wavelength of 1030 nm, the first is based on intrapulse DFG (intraDFG), and the second on DFG at the output of an optical parametric amplifier (OPA). The noise properties are assessed through measurement of the relative intensity noise (RIN) power spectral density and pulse-to-pulse stability. The noise transfer mechanisms from the pump to the MIR beam is empirically demonstrated. As an example, improving the pump laser noise performance allows reduction of the integrated RIN (IRIN) of one of the MIR source from 2.7% RMS down to 0.4% RMS. The intensity noise is also measured at various stages and in several wavelength ranges in both laser system architectures, allowing us to identify the physical origin of their variation. This study presents numerical values for the pulse to pulse stability, and analyze the frequency content of the RINs of particular importance for the design of low-noise high repetition rate tunable MIR sources and future high performance time-resolved molecular spectroscopy experiments.

Ultrafast Imaging of the Jahn–Teller Topography in Carbon Tetrachloride

We report the direct time-domain observation of ultrafast dynamics driven by the Jahn-Teller effect. Using time-resolved photoelectron spectroscopy with a vacuum-ultraviolet femtosecond source to prepare high-lying Rydberg states of carbon tetrachloride, our measurements reveal the local topography of a Jahn-Teller conical intersection. The pump pulse prepares a configurationally mixed superposition of the degenerate 1T2 4p-Rydberg states, which then distorts through spontaneous symmetry breaking that we identify to follow the t2 bending motion. Photoionization of these states to three cationic states 2T1, 2T2, and 2E reveals a shift in the center-of-mass of the photoelectron peaks associated with the 2Tn states which reveals the local topography of the Jahn-Teller conical intersection region prepared by the pump pulse. Time-dependent density functional theory calculations confirm that the dominant nuclear motion observed in the spectrum is the CCl4 t2 bending mode. The large density of states in the VUV spectral region at 9.33 eV of carbon tetrachloride and strong vibronic coupling result in ultrafast decay of the excited-state signal with a time constant of 75(4) fs.

Theoretical analysis of self-phase-modulation-enabled spectral selection in hollow-core fibers: effect of ionization

We propose the generation of wavelength-tunable femtosecond pulses with µJ energy based on spectral broadening in hollow-core fibers (HCFs) filled with noble gas. A proper combination of gas type, gas pressure, and the HCF core radius ensures that the broadened spectrum consists of isolated spectral lobes; the selection of the outermost spectral lobes produces nearly transform-limited pulses. We performed a detailed numerical investigation of this method based on an antiresonant HCF with a 20 µm core radius filled with 17.3 bar Xe gas. By using 1.03 µm, 200 fs pulses with up to 20 µJ energy as the excitation pulse, this method can produce 100 fs pulses tuned from 0.74 to 1.25 µm with up to 5 µJ pulse energy. Further energy scaling is limited by the onset of ionization, which reduces the wavelength tuning range and causes a significant spectral blue shift. Increasing the input pulse energy beyond 45 µJ creates a strong spectral lobe peaking in the wavelength range of 0.92–0.95 µm with &gt;10µJ energy. These results represent a two orders of magnitude improvement in the pulse energy compared to current tunable femtosecond sources based on nonlinear wavelength conversion in solid-core optical fibers.