Mid-infrared Pulses Research Articles

3.8 µm pulse burst self-optical parametric oscillator utilizing a programmable step-active Q-switch with Nd:MgO:PPLN crystal

This paper reports a 3.8 µm pulse burst self-optical parametric oscillator (SOPO) employing the Nd:MgO:PPLN crystal, achieving programmable mid-infrared pulse burst output based on step-active Q-switching technology. Building on the intracavity optical parametric oscillator (IOPO) theory, a theoretical model for the step-active Q-switched self-optical parametric oscillator is developed by introducing idler photon and step loss terms. The simulation results elucidate the evolution of population inversion and photon numbers and determine step-active Q-switching loss values for different sub-pulse numbers. Additionally, a 3.8 µm pulse burst laser output with a repetition rate of 10 kHz is experimentally achieved using the step-active Q-switching signal designed from the theoretical simulation. The effective programming of the step-active Q-switching signal achieves control over 2-4 sub-pulses, 260-1000 ns intervals, and any amplitude ratios. The experimental and simulation results demonstrate consistency, offering valuable insights for optimizing the Q-switching technology in other SOPO systems.

High-pulse-energy ultrafast 3 µm laser generation through OPG/DFG in PPMgLN

Abstract We report high-pulse-energy ultrafast 3 µm laser generation through optical parametric generation/difference frequency generation (OPG/DFG) in periodically poled magnesium-oxide-doped lithium niobate (PPMgLN). A commercial 1030 nm femtosecond laser is applied as the pump light and a homemade broadband nanosecond pulse laser around 1580 nm is used as the signal light in DFG. The broadband 1580 nm laser has a master oscillator power amplifier (MOPA) structure with a directly modulated superluminescent light-emitting diode (SLED) as the pulse seed and three stages of Er/Yb fiber amplifiers to lift its average power. A portion of the 1030 nm output pulse is converted to an electronic pulse via a pin detector, which is used as the trigger signal of the SLED driving circuit to ensure synchronization between the signal and the 1030 nm pump pulse. When injecting 2.12 W pump light into the PPMgLN, a broadband mid-infrared (MIR) output of 280 mW can be achieved directly through OPG with a center wavelength around 2.94 μm, a pulse width of 1.38 ps and a pulse repetition frequency of 500 kHz. The corresponding MIR pulse energy is 0.56 µJ. When injecting 2.62 W signal light simultaneously, a MIR output of 300 mW is achieved through the DFG process at the same pulse repetition frequency, corresponding to a pulse energy of 0.6 µJ. The conversion efficiency of the ultrafast pump laser to MIR reaches 14.1%. This high-pulse-energy 3 μm ultrafast laser has great prospects for applications in biological tissue ablation.

Octave-spanning supercontinuum coherent soft x-ray for producing a single-cycle soft x-ray pulse.

This study demonstrates the potential to generate a soft x-ray single-cycle attosecond pulse using a single-cycle mid-infrared pulse from advanced dual-chirped optical parametric amplification (DC-OPA). A super continuum high harmonic (HH) spectrum was generated in argon (80-160 eV) and neon (150-270 eV). The experimental spectra reasonably agree with those calculated by the strong-field approximation model and Maxwell's equations. In addition, simulation results indicate that the dispersion of HHs in argon can be compensated using a 207-nm Zr filter to obtain 40 as (Fourier transform limited (FTL)) pulses (1.1 cycles at 118 eV). For neon, a 278-nm Sn filter can compensate for the dispersion of HH and create 23 as FTL pulses (1.1 cycles at 206 eV). This soft x-ray single-cycle attosecond pulse is expected to be highly valuable for ultrafast science and applications in quantum information science.

Mid-infrared laser pulse excitation for terahertz generation from organic liquids molecules

Strong laser field is able to rotate gas molecules and the rotated gas molecules would emit electromagnetic waves when these molecules transition to the lower rotational energy levels. However, related investigation on liquid molecule rotation has not been reported, let alone the radiation falls in terahertz (THz) range. Here, a theoretical model is proposed to study the mid-infrared femtosecond laser driving organic liquid molecules such as methanol, ethanol, and acetic acid molecules to emit THz radiation. The interaction between laser electric field and liquid molecules are analyzed based on quantum mechanics theory. It is found that the spectrum of the THz radiation from methanol molecules range from 0.1 to 5 THz, while the spectra from ethanol and acetic acid molecules show nearly the same frequency range of 0.1–2 THz. These results indicate that broadband THz radiation can be generated through the transitions of rotational energy levels of the rotational liquid molecules excited by a linear polarization mid-infrared laser.

Sub-attosecond-precision optical-waveform stability measurements using electro-optic sampling

The generation of laser pulses with controlled optical waveforms, and their measurement, lie at the heart of both time-domain and frequency-domain precision metrology. Here, we obtain mid-infrared waves via intra-pulse difference-frequency generation (IPDFG) driven by 16-femtosecond near-infrared pulses, and characterise the jitter of sub-cycle fractions of these waves relative to the gate pulses using electro-optic sampling (EOS). We demonstrate sub-attosecond temporal jitter at individual zero-crossings and sub-0.1%-level relative amplitude fluctuations in the 10-kHz–0.625-MHz band. Chirping the nearly-octave-spanning mid-infrared pulses uncovers wavelength-dependent attosecond-scale waveform jitter. Our study validates EOS as a broadband (both in the radio-frequency and the optical domains), highly sensitive measurement technique for the jitter dynamics of optical waveforms. This sensitivity reveals outstanding stability of the waveforms obtained via IPDFG and EOS, directly benefiting precision measurements including linear and nonlinear (infrared) field-resolved spectroscopy. Furthermore, these results form the basis toward EOS-based active waveform stabilisation and sub-attosecond multi-oscillator synchronisation/delay tracking.

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.

Time-resolved ARPES with probe energy of 6.0 eV and tunable MIR pump at 250 kHz

In this paper, we present a laser source designed specifically for time- and angle-resolved photoemission spectroscopy (TR-ARPES) investigations of light-induced electron dynamics in quantum materials. Our laser source is based on a ytterbium-doped laser that seeds an optical parametric amplifier (OPA) followed by a difference frequency generation (DFG) stage. This configuration enables the generation of tunable near-infrared and mid-infrared laser pulses (1.5 to 8 μm - 0.82 to 0.15 eV) at 250 kHz of repetition rate, serving as the pump for TR-ARPES measurements. The remaining energy of the laser is used to generate the ultraviolet 6 eV probe pulses, which prompt the material to emit photoelectrons. We demonstrate the long-term stability of the source, as well as the characterization of the beam profiles and pulse durations. Additionally, we present preliminary TR-ARPES results obtained on Bi2Te3, a prototypical 3D topological insulator. This paper illustrates the capability of our laser source to probe electronic dynamics in quantum materials.

Propagation of broadband mid-infrared optical pulses in atmosphere

We study and describe the reshaping of ultrashort and broadband mid-IR optical pulses in an ambient atmosphere. While all pulse propagation undergoes dispersion and absorption, which causes pulse reshaping, the effects are strongly pronounced for broadband radiation in the mid-IR due to the orders of magnitude greater oscillator strengths of molecular constituents of our atmosphere. A noticeable macroscopic impact is a transition of the measured autocorrelation function from squared hyperbolic secant to Lorentzian, which we fully explain based on pulse propagation, including molecular free induction decay. Electro-optical sampling directly reveals the light wave response to atmospheric molecular free induction decay, and a Kramers–Kronig-based propagation model thoroughly explains the observation. The findings are essential for applications in sensing, standoff detection, high-energy pulse propagation, and energy delivery.

Tunable UV ∼ IR frequency comb generation via high-order sideband generation

We propose the generation of a widely tunable UV-to-IR frequency comb by high-order sideband generation (HSB) spectrum emitted from semiconductors. In our theoretical simulations, we demonstrate the high-order sideband signals of two series (2m Ωseed + (2n + 1) ωdriver, and (2m + 1) Ωseed + 2 nωdriver ), where m and n are integers of a seed pulse and a driver laser frequency, respectively. The simulations also reveal the intensity of HSB scale with the driver laser power, both perturbatively and non-perturbatively. We find that the harmonic position and spacing of the high-order sideband emission can be controlled by varying the seed pulse and driver photon energies. In the experiment, we applied a visible ( ℏΩseed = 3.1 eV, ∼400 nm) seed pulse and mid-infrared (MIR, ℏωdriver = 0.4 eV, 3.1 μm) driver pulses to ZnSe target. Our experimental observations confirmed the UV (4.7 eV, 263 nm and 3.9 eV, 317 nm) HSB generation.

Modelling of long-wave mid-infrared ultrashort pulse generation via difference frequency generation

In this paper, a model of generating mid-infrared (MIR) ultrashort laser pulse through difference frequency generation (DFG) is established. The pulse evolution relationship among the pump, signal, and idler pulses during the DFG process, as well as the effects of crystal length, pulse energy of the pump and signal lights, pulse width, and other factors on the characteristics of the MIR pulse are explored. Furthermore, through simulations from the time domain to the frequency domain, the spectral characteristics and angular distribution of MIR were analyzed. DFG experimental data are also presented to support the model.

Narrowband mid-infrared optical parametric generator based on a type-II BaGa4Se7 crystal.

In this Letter, we first reported on a mid-infrared double-pass optical parametric generator (OPG) based on a single type-II phase-matching BaGa4Se7 (BGSe) crystal, pumped at 2.1 µm. The OPG achieved a maximum pulse energy of 55 µJ for generating narrowband mid-infrared laser pulses. The signal and idler lights exhibited center wavelengths of 4.04 and 4.33 µm, respectively, with bandwidths of 18.6 nm (11.4 cm-1) and 20.4 nm (10.9 cm-1). To improve the output performance, we utilized a cascaded scheme of type-I ZnGeP2 (ZGP) and type-II BGSe crystals. The spectral bandwidths of the signal and idler lights, nearing 4 µm, were narrower than 170 nm (90 cm-1), representing a significant improvement over the ZGP OPG. The cascaded OPG achieved a remarkable total optical-to-optical conversion efficiency (OOCE) of 14.9% and a maximum pulse energy of 0.329 mJ.

Modeling generation of harmonics in the water window region in hollow core waveguides by mid-infrared femtosecond pulses

We numerically investigate generation of harmonics in the water window region (down to 2.8 nm) by 2 μm femtosecond pulses propagating in hollow core waveguides filled with high pressure He. Numerical calculations are based on a three dimensional macroscopic model, which solves the pulse propagation by a split-step method, uses the strong field approximation to evaluate the single atom response, and integrates it coherently to obtain the harmonic field. Two configurations for the waveguides are considered: the standard one with a constant diameter of 70 μm and a conical one with a decreasing diameter from 70 to 50 μm. We demonstrate that harmonic field enhancement can be obtained in spectral domains of great practical interest, from 2.8 to 20 nm, and identify quasi-phase matching induced by multimode beating as the mechanism responsible for this enhancement.

Background-free mid-infrared absorption spectroscopy using sub-cycle pulses

We have demonstrated highly sensitive single-shot based background-free mid-infrared (MIR) absorption spectroscopy using sub-cycle MIR pulses generated through filamentation. The MIR pulse transmitted through a sample was upconverted with a fast rising and long tailing gate pulse through four-wave difference frequency generation in a silicon membrane. By recording the upconverted spectrum of the free induction decay alone, we successfully measured the absorption spectrum as a positive signal in the wavenumber range from 500 to 4500 cm−1, which covers both the fingerprint and functional group regions. We obtained an absorption spectrum of ∼50 mM of aqueous glucose, which is not detectable with a standard Fourier transform infrared spectrometer.

Multiphoton-initiated laser writing of semiconductors using nanosecond mid-infrared pulses

The advent of more powerful mid-infrared nanosecond laser sources allows using them as attractive tools in material laser processing. For semiconductor bulk processing, laser intensities must remain modest to avoid detrimental nonlinear propagation and pre-focal plasma screening effects. Accordingly, nanosecond pulses are usually appropriate to locally initiate energy deposition by multiphoton absorption and subsequent modification, hardly achievable with ultrashort pulses. Employing a 2.8-μm 2.5-ns laser source, we explore the possibility to modify silicon and other semiconductors. With interactions initiated by three-photon absorption, we modify and determine the surface and bulk modification thresholds of Si, GaAs, and InP. For Si, compared to previous studies at telecom wavelengths, we report on a reduction of the energy threshold for volume modification with processing depth, and repeatable rear-surface modifications. Compared to Si, we find for GaAs and InP important fluctuations in the modification responses, which we attribute to an absorption mechanism initially triggered by a greater presence of defects. We also study germanium, as this narrower bandgap semiconductor very interesting for mid-infrared electro-optical applications is transparent at the newly introduced wavelength. Despite the ability to modify the surface, the bulk of Ge remains inaccessible in this two-photon regime, mainly attributed to beam aberrations and nonlinearities. Nonetheless, we demonstrate the ability to process Si chips integrating Ge layers. All these results showcase the potential of mid-infrared wavelengths to offer new degrees of flexibility for 3D laser processing technologies turned to silicon photonics and microelectronics packaging.

ZnO microwire lasing generated by mid-infrared laser pulses of various polarization

ZnO microwire lasing generated by mid-infrared laser pulses of various polarization

An optical fiber integrated device for nonlinear generation of femtosecond mid-infrared pulses

Compact and broadband mid-infrared (MIR) sources are in high demand because of a wide range of potential applications such as molecular sensing in the fingerprint region. The generation of coherent MIR radiation at arbitrary frequencies typically requires nonlinear mixing between at least two input waves, which is often cumbersome to implement. We present an integrated and, therefore, adjustment-free solution combining few-femtosecond pulse compression in a germanosilicate optical fiber and optical rectification. To this end, a 16-μm-thin GaSe crystal is directly mounted on the end facet of a highly nonlinear fiber assembly exploiting a focused ion beam. With input pulses of a minute energy of 5 nJ and a duration of 120 fs at the telecom wavelength of 1.55 μm, we directly obtain ultrabroadband and phase-stable output transients. Electro-optic sampling in free space reveals single-cycle pulses with spectral components covering the entire MIR from 10 to 120 THz.

Generation and Implementation of Continuum Infrared Pulses for Broadband Detection in 2D IR Spectroscopy.

In recent years, new methods of generating continuum mid-infrared pulses through filamentation in gases have been developed for ultrafast time-resolved infrared vibrational spectroscopy. The generated infrared pulses can have thousands of wavenumbers of bandwidth, spanning the entire mid-IR region while retaining pulse length below 100 fs. This technology has had a significant impact on problems involving ultrafast structural dynamics in congested spectra with broad features, such as those found in aqueous solutions and molecules with strong intermolecular interactions. This study describes the recent advances in generating and characterizing these pulses and the practical aspects of implementing these sources for broadband detection in transient absorption and 2D IR spectroscopy.

Unzipping hBN with ultrashort mid-infrared pulses.

Manipulating the nanostructure of materials is critical for numerous applications in electronics, magnetics, and photonics. However, conventional methods such as lithography and laser writing require cleanroom facilities or leave residue. We describe an approach to creating atomically sharp line defects in hexagonal boron nitride (hBN) at room temperature by direct optical phonon excitation with a mid-infrared pulsed laser from free space. We term this phenomenon "unzipping" to describe the rapid formation and growth of a crack tens of nanometers wide from a point within the laser-driven region. Formation of these features is attributed to the large atomic displacement and high local bond strain produced by strongly driving the crystal at a natural resonance. This process occurs only via coherent phonon excitation and is highly sensitive to the relative orientation of the crystal axes and the laser polarization. Its cleanliness, directionality, and sharpness enable applications such as polariton cavities, phonon-wave coupling, and in situ flake cleaving.

Generation of High-Lying Vibrational States in Carbon Dioxide through Coherent Ladder Climbing.

Mid-infrared laser excitation of molecules into high-lying vibrational states offers a novel route to realize controlled ground-state chemistry. Here we successfully demonstrate vibrational ladder climbing in the antisymmetric stretch of CO2 in the condensed phase by using intense down-chirped mid-infrared pulses. Spectrally resolved pump-probe measurements directly observe excited-state absorptions attributed to vibrational populations up to the v = 9 state, whose corresponding energy of 2.5 eV is 46% of the dissociation energy. By the use of global fitting analysis, important spectroscopic parameters in the high-lying vibrational states, such as transition frequencies and relaxation times, are quantitatively characterized. Remarkably, our analysis shows that 40% of the molecules are excited above the typical activation barriers in the metal-catalyzed CO2 conversions. These results not only demonstrate the promising ability of infrared excitation to produce elevated vibrational states but also represent a significant step toward accelerating CO2 conversions and other chemical processes via mode-specific vibrational excitation.

Efficient single-cycle mid-infrared femtosecond laser pulse generation by spectrally temporally cascaded optical parametric amplification with pump energy recycling.

We proposed spectrally temporally cascaded optical parametric amplification (STOPA) using pump energy recycling to simultaneously increase spectral bandwidth and conversion efficiency in optical parametric amplification (OPA). Using BiB3O6 and KTiOAsO4 nonlinear crystals, near-single-cycle mid-infrared (MIR) pulses with maximum energy conversion efficiencies exceeding 25% were obtained in simulations. We successfully demonstrated sub-two-cycle, CEP-stable pulse generation at 1.8 µm using a four-step STOPA system in the experiment. This method provides a solution to solve the limitations of the gain bandwidth of nonlinear crystals and the low conversion efficiency in broadband OPA systems, which is helpful for intense attosecond pulse generation and strong laser field physics studies.