Sub-cycle Pulses Research Articles

Localized solutions of the wave equation

A family of solutions of the wave equation is presented. The simplest waveforms represent sub-cycle pulses; oscillatory pulses with a dominant wavenumber are also discussed. These solutions are sufficiently localized to have finite energy, momentum, and angular momentum when applied to acoustic and electromagnetic pulses. The energy, momentum, and angular momentum of the pulses are simply expressed in terms of the wavenumber weight function.

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.

Ultra-phase-stable infrared light source at the watt level.

Ultrashort pulses at infrared wavelengths are advantageous when studying light-matter interaction. For the spectral region around 2 µm, multi-stage parametric amplification is the most common method to reach higher pulse energies. Yet it has been a key challenge for such systems to deliver waveform-stable pulses without active stabilization and synchronization systems. Here, we present a different approach for the generation of infrared pulses centered at 1.8 µm with watt-level average power utilizing only a single nonlinear crystal. Our laser system relies on a well-established Yb:YAG thin-disk technology at 1.03 µm wavelength combined with a hybrid two-stage broadening scheme. We show the high-power downconversion process via intra-pulse difference frequency generation, which leads to excellent passive stability of the carrier envelope phase below 20 mrad-comparable to modern oscillators. It also provides simple control over the central wavelength within a broad spectral range. The developed infrared source is employed to generate a multi-octave continuum from 500 nm to 2.5 µm opening the path toward sub-cycle pulse synthesis with extreme waveform stability.

Unraveling photodissociation dynamics by sub-femtosecond ultraviolet pulses: insights into fragmental kinetics and carrier-envelope phase characterization

The duration of laser pulses and the carrier-envelope phase (CEP) play a crucial role in shaping kinetic energy release (KER) spectra. In this study, we performed theoretical calculations on pulse duration-dependent KER spectra, ranging from hundreds to sub-femtoseconds, focusing on the MgH+ scenario. Our findings reveal a distinct shift in KER peaks from sub-cycle pulses, deviating from the resonance energy. Utilizing two-level perturbation theory, we identify that this shift is attributable to the energy-dependent transition matrix elements. Moreover, our investigation uncovers a notable CEP effect in KER from sub-cycle pulses, arising from interference between counter-rotating and rotating terms within a single ultraviolet photon transition. To leverage this insight, we propose a novel pump-probe methodology for precise CEP characterization of ultra-short laser pulses. We hope this method would promise advancements in understanding and manipulating ultrafast processes.

Electric Area Conservation Rule and the Validity of Some Models of Subcycle Pulse Propagation

The validity issues of some approximations widely used to describe subcycle pulse propagation in various non-magnetic media are addressed. As the validity criteria we apply the fundamental electric area conservation rule, which directly follows from Maxwell’s equations in the 1D case. The general relations are derived for the possible values of the electric area in different media. It is shown that several theoretical models do not in general comply with the electric area conservation rule, which implies their limited applicability to correctly describe the subcycle pulse interaction with media. Therefore, any results obtained using such models cannot be taken as scientifically valid and meaningful.

Dual-chirped optical parametric amplification of high-energy single-cycle laser pulses

We demonstrate how a scheme called advanced dual-chirped optical parametric amplification (DC-OPA) that employs two kinds of nonlinear crystal (BiB3O6 and MgO-doped lithium niobate) can generate high-energy, single-cycle mid-infrared laser pulses. In experiments, the advanced DC-OPA scheme achieved carrier-to-envelope phase-stable mid-infrared laser pulses with a bandwidth of over one octave (1.4–3.1 µm) and an output pulse energy of 53 mJ. The pulse duration was compressed to 8.58 fs, which corresponds to 1.05 cycles with a central wavelength of 2.44 µm and a peak power of 6 TW. To our knowledge, the obtained values for the pulse energy and peak power are the highest achieved for optical parametric amplification of single-cycle mid-infrared laser pulses. Moreover, owing to the energy scalability of the advanced DC-OPA scheme, the prospects of the multi-terawatt sub-cycle laser pulses are discussed.

Optical solitons in hollow-core fibres

I review the historical observation and subsequent research on optical soliton dynamics in gas-filled hollow-core optical fibres. I include both large-core hollow capillary fibres, and hollow-core photonic-crystal or microstructured fibres with smaller cores, in particular photonic bandgap and antiresonant guiding fibres. I discuss how the optical guidance properties of these different fibre structures influence the soliton dynamics that can be obtained. The dynamics I consider include: soliton propagation at peak power levels ranging from the megawatt to terawatt level, and pulse energies from sub-microjoule to millijoule range; pulse self-compression, leading to sub-cycle and sub-femtosecond pulse duration; soliton self-frequency shifting due to both the Raman effect, and the influence of photoionisation and plasma formation; and resonant dispersive wave emission, leading to the generation of tuneable few-femtosecond pulses across the vacuum and deep ultraviolet, visible, and near-infrared spectral regions.

Coherent control of a multilevel resonant medium by subcycle pulses

We theoretically demonstrate the possibility of coherent control of the response of a multilevel resonant medium by means of half-cycle unipolar or quasi-unipolar attosecond pulses. We show that despite the ultrabroad spectrum of half-cycle pulses the induced medium polarization can be efficiently steered through the proper choice of the parameters for the excitation pulses. Besides, we found that the response of a multilevel medium for the amplitude of driving subcycle pulses below a certain threshold can be quantitatively well approximated by the two-level model.

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 f-2f 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.

Coherent Subcycle Optical Shock from a Superluminal Plasma Wake.

We propose exploiting the superluminal plasma wake for coherent Cherenkov radiation by injecting a relativistic electron beam (REB) into a plasma with a slowly varying density up-ramp. Using three-dimensional particle-in-cell and far-field time-domain radiation simulations, we show that an isolated subcycle pulse is coherently emitted towards the Cherenkov angle by bubble-sheath electrons successively at the rear of the REB-induced superluminal plasma wake. A theoretical model based on a superluminal current dipole has been developed to interpret such coherent radiation, and agrees well with the simulation results. This radiation has ultrashort attosecond-scale duration and high intensity, and exhibits excellent directionality with ultralow angular divergence and stable carrier envelope phase. Its intensity increases with the square of the propagation length and its central frequency can be easily tuned over a wide range, from the far infrared to the ultraviolet.

Generation of an ultrahigh-repetition-rate optical half-cycle pulse train in the nested quantum wells.

We propose a simple quantum system, namely, a nested quantum-well structure, which is able to generate a train of half-cycle pulses of a few-femtosecond duration when driven by a static electric field. We theoretically investigate the emission of such a structure and its dependence on the parameters of the quantum wells. It is shown that the production of a regular output pulse train with tunable properties and the pulse repetition frequencies of tens of terahertz is possible in certain parameter ranges. We expect the suggested structure can be used as an ultra-compact source of subcycle pulses in the optical range.

Sub-cycle pulse revealed with carrier-envelope phase control of soliton self-compression in anti-resonant hollow-core fiber.

The influence of the carrier-envelope phase (CEP) of a pump pulse on the multioctave supercontinuum (SC) generation in a gas-filled anti-resonant hollow-core fiber (AR HCF) by soliton self-compression (SSC) has been explored. We have shown an octave-wide third harmonic generation (THG) in the visible-to-near-infrared range during the pulse compression down to a sub-cycle duration. The CEP of a multi-cycle pump pulse provides control of interference between the third harmonic (TH) and the SC that indicates the coherent synthesis of a sub-cycle pulse with a duration of about 0.4 optical cycles and a peak power of more than 2 GW at the fiber output.

High-speed scanless entire bandwidth mid-infrared chemical imaging

Mid-infrared spectroscopy probes molecular vibrations to identify chemical species and functional groups. Therefore, mid-infrared hyperspectral imaging is one of the most powerful and promising candidates for chemical imaging using optical methods. Yet high-speed and entire bandwidth mid-infrared hyperspectral imaging has not been realized. Here we report a mid-infrared hyperspectral chemical imaging technique that uses chirped pulse upconversion of sub-cycle pulses at the image plane. This technique offers a lateral resolution of 15 µm, and the field of view is adjustable between 800 µm × 600 µm to 12 mm × 9 mm. The hyperspectral imaging produces a 640 × 480 pixel image in 8 s, which covers a spectral range of 640–3015 cm–1, comprising 1069 wavelength points and offering a wavenumber resolution of 2.6–3.7 cm–1. For discrete frequency mid-infrared imaging, the measurement speed reaches a frame rate of 5 kHz, the repetition rate of the laser. As a demonstration, we effectively identified and mapped different components in a microfluidic device, plant cell, and mouse embryo section. The great capacity and latent force of this technique in chemical imaging promise to be applied to many fields such as chemical analysis, biology, and medicine.

Controlling inversion and time-reversal symmetries by subcycle pulses in the one-dimensional extended Hubbard model

Owning to their high controllability, laser pulses have contributed greatly to our understanding of strongly correlated electron systems. However, typical multicycle pulses do not control the symmetry of systems, which plays an important role in the emergence of novel quantum phases. Here, we demonstrate that subcycle pulses whose oscillation is less than one period within a pulse envelope can control inversion and time-reversal symmetries in the electronic states of the one-dimensional extended Hubbard model. Using an ultrashort subcycle pulse, one can generate a steady electric current (SEC) in a photoexcited state due to an Aharonov-Bohm flux instantaneously introduced through the phase of an electric field. Consequently, time-reversal symmetry is broken. In contrast, a broad subcycle pulse does not induce SEC but instead generates electric polarization, thus breaking inversion symmetry. Both symmetry breakings in a photoexcited state can be monitored by second-harmonic generation. These findings provide a new methodology for designing the symmetries of electronic states and open up a new field of subcycle-pulse engineering.

High-order harmonic generation by sub-cycle laser pulses and associated scaling laws

We studied the high-harmonic generation by the interaction of sub-cycle laser pulses with the He atom. The sub-cycle pulses are modeled using the complex source vector beam model, which is an exact solution to Maxwell's equations and accurately models the sub-cycle field profiles. We observed that the harmonic cutoff could be extended with the variation of the sub-cycle pulse duration, mainly because of the inherent blueshift associated with shorter pulses. The scaling laws for the harmonic yield and harmonic cutoff energy with pulse duration and fundamental driver wavelengths are also deduced. Furthermore, a detailed wavelet analysis of harmonic generation by sub-cycle pulses is carried out. The appropriate filtering and superposition of the harmonics gave rise to a single attosecond pulse of duration ∼100 as.

Scalable sub-cycle pulse generation by soliton self-compression in hollow capillary fibers with a decreasing pressure gradient

Advances in the generation of the shortest optical laser pulses down to the sub-cycle regime promise to break new ground in ultrafast science. In this work, we theoretically demonstrate the potential scaling capabilities of soliton self-compression in hollow capillary fibers with a decreasing pressure gradient to generate near-infrared sub-cycle pulses in very different dispersion and nonlinearity landscapes. Independently of input pulse, gas and fiber choices, we present a simple and general route to find the optimal self-compression parameters which result in high-quality pulses. The use of a decreasing pressure gradient naturally favors the self-compression process, resulting in shorter and cleaner sub-cycle pulses, and an improvement in the robustness of the setup when compared to the traditional constant pressure approach.

Superradiance of a Stopped Polarization Pulse in a Thin Layer of a Five-Level Medium Excited by Subcycle Attosecond Pulses

Using the numerical solution of the system of equations for the amplitudes of bound states, together with the wave equation, we theoretically consider stopped polarization pulse superradiance upon excitation by a pair of half-period attosecond pulses in a thin layer of a five-level resonant medium, the parameters of which are the same as in a hydrogen atom. It is shown that in the case of a multilevel medium, at certain parameters of the exciting field, the superradiance pulse near the medium is also a single-cycle pulse, the shape of which is determined by the first time derivative of the stopped polarization pulse, as in the case when approximate low-level and classical models were used to describe the response of the medium. Keywords: superradiance, attosecond pulses, stopped polarization pulse, unipolar pulses, subcycle pulses.

Peculiarities of Excitation of a Particle in a Single-Level Quantum Well by an Extremely Short Attosecond Pulse

Using the solution of the time-dependent Schrodinger equation, the features of the excitation of a bound state of a particle in a one-dimensional rectangular quantum well of small depth by an extremely short light pulse are studied. The case of a shallow well with only one energy level is considered. In this case, the system is excited by an attosecond pulse whose duration is shorter than the characteristic time associated with the energy of the bound state of the particle in the well. It is shown that in this case the population of the bound state and the ionization probability are determined by the ratio of the electric area of the pulse to its atomic scale, which is inversely proportional to the well width. The calculation results showed that unipolar subcycle pulses with nonzero electric area can excite the system faster and more efficiently than bipolar pulses with zero area. The possibility of using unipolar gamma-ray pulses of zeptosecond duration for deuteron excitation is discussed, and numerical estimates of the required duration and electric area of the pulse are given. Keywords: extremely short pulses attosecond pulses, unipolar pulses, electric area of a pulse, atomic scale of electric area, one-dimensional quantum wells, nanostructures.

Особенности возбуждения частицы в одноуровневой квантовой яме предельно коротким аттосекундным импульсом

Using the solution of the time Schrödinger equation, the features of the excitation of a bound state of a particle in a one-dimensional rectangular quantum well of small depth by an extremely short light pulse are studied. The case of a shallow well with only one energy level is considered. In this case, the system is excited by an attosecond pulse whose duration is shorter than the characteristic time associated with the energy of the bound state of the particle in the well. It is shown that in this case the population of the bound state and the ionization probability are determined by the ratio of the electric area of the pulse to its atomic measure, which is inversely proportional to the well width. The calculation results showed that unipolar subcycle pulses with nonzero electric area can excite the system faster and more efficiently than bipolar pulses with zero area. The possibility of using unipolar gamma-ray pulses of zeptosecond duration for deuteron excitation is discussed, and numerical estimates of the required duration and electric area of the pulse are given.

Principal frequency, superbandwidth, and low-order harmonics generated by superoscillatory pulses

An alternative definition to the main frequency of an ultrashort laser pulse, named principal frequency (${\ensuremath{\omega}}_{P}$), was recently introduced in E. G. Neyra et al. [Phys. Rev. A 103, 053124 (2021)], resulting in a more transparent description of the nonlinear dynamics of a system driven by this coherent source. In this paper, we extend the definition of ${\ensuremath{\omega}}_{P}$ incorporating the spectral phase of the pulse. This upgraded definition allow us to deal with superoscillatory pulses as well as to characterize subcycle pulses with a complex spectral content. Simultaneously, we study the nonlinear interaction between a few-cycle superoscillatory pulse with a gaseous system, analyzing the spectral characteristics of the fundamental, third, and fifth harmonics. Here, we make use of an ab initio quantum mechanical approach, supplemented with a wavelet analysis. We show that the spectral characteristics of the low-order harmonics are very well explained in terms of ${\ensuremath{\omega}}_{P}$, as well as the effective bandwidth of the superoscillatory pulse. Our findings reinforce previous results that showed an increase of the effective bandwidth in the superoscillatory region and the possibility to generate unique frequencies by a linear synthesis. We thus open not only perspectives in ultrafast optics, exploring pathways toward the generation of fully tunable strong and short coherent sources, but also discuss possible extensions of the concepts presented here to other wave phenomena that can be found in acoustics, signal processing, and quantum mechanics.