Few-cycle Light Pulses Research Articles

Field-resolved space–time characterization of few-cycle structured light pulses

Accompanied by the rapid development of ultrafast laser platforms in recent decades, the spatiotemporal manipulation of ultrashort laser pulses has attracted much attention due to the potential for cutting-edge applications of structured light, including optical tweezers, optical communications, super-resolution imaging, time-resolved spectroscopy in molecules and quantum materials, and strong-field physics. Today, techniques capable of characterizing the full spatial, temporal, and polarization state properties of structured light are strongly desired. Here, we demonstrate a technique, termed 3D TIPTOE, for characterizing structured mid-infrared waveforms, which uses only a two-dimensional silicon-based image sensor as both the detector and the nonlinear medium. By combining the advantages of the sub-cycle time resolution afforded by nonlinear excitation and the spatial resolution inherent to the two-dimensional sensor, the 3D TIPTOE technique allows full characterization of structured electric fields, significantly reducing the complexity of detection compared to other techniques. The validity of the technique is established by measuring both few-cycle Bessel–Gaussian pulses and radially polarized femtosecond vector beams.

Full counting statistics of ultrafast quantum transport

Quantum transport in the presence of time-dependent drives is dominated by quantum interference and many-body effects at low temperatures. For a periodic driving, the analysis of the full counting statistics revealed the elementary events that determine the statistical properties of the charge transport. As a result, the noise correlations display quantum oscillation as functions of the ratio of the voltage amplitude and the drive frequency, reflecting the detailed shape of the drive. However, so far only continuous wave excitations were considered, but, recently, transport by few-cycle light pulses were investigated, and the need for a statistical interpretation became eminent. We address the charge transfer generated by single- or few-cycle light pulses. The fingerprints of these time-dependent voltage pulses are imprinted in the full counting statistics of a coherent mesoscopic conductor at zero temperature. In addition, we identify the elementary processes that occur in the form of electron–hole pair creations, which can be investigated by the excess noise. We study the quantum oscillations in the differential noise induced by a wave packet consisting of an oscillating carrier modulated by a Gaussian- or a box-shaped envelope. As expected, the differential noise exhibits an oscillatory behavior with increasing amplitude. In particular, we find clear signature of the so-called carrier-envelope phase in the peak heights and positions of these quantum oscillations. More carrier cycles under the Gaussian envelope diminish the influence of the carrier-envelope phase, while this is not true for the box pulses, probably related to the abrupt onset.

Nonlinear compression toward high-energy single-cycle pulses by cascaded focus and compression.

The advancement of contemporary ultrafast science requires reliable sources to provide high-energy few-cycle light pulses. Through experiments and simulations, we demonstrate an arrangement of pulse postcompression, referred to as cascaded focus and compression (CASCADE), for generating millijoule-level, single-cycle pulses in a compact fashion. CASCADE is realized by a series of foci in matter, whereas pulse compression is provided immediately after each focus to maintain a high efficiency of spectral broadening. By implementing four stages of CASCADE in argon cells, we achieve 50-fold compression of millijoule-level pulses at 1030 nanometers from 157 to 3.1 femtoseconds, with an output pulse energy of 0.98 millijoules and a transmission efficiency of 73%. When driving high harmonic generation, these single-cycle pulses enable the creation of a carrier-envelope phase-dependent extreme ultraviolet continuum with energies extending up to 180 electron volts, providing isolated attosecond pulses at the output.

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.

High-harmonic generation in metallic titanium nitride

High-harmonic generation is a cornerstone of nonlinear optics. It has been demonstrated in dielectrics, semiconductors, semi-metals, plasmas, and gases, but, until now, not in metals. Here we report high harmonics of 800-nm-wavelength light irradiating metallic titanium nitride film. Titanium nitride is a refractory metal known for its high melting temperature and large laser damage threshold. We show that it can withstand few-cycle light pulses with peak intensities as high as 13 TW/cm2, enabling high-harmonics generation up to photon energies of 11 eV. We measure the emitted vacuum ultraviolet radiation as a function of the crystal orientation with respect to the laser polarization and show that it is consistent with the anisotropic conduction band structure of titanium nitride. The generation of high harmonics from metals opens a link between solid and plasma harmonics. In addition, titanium nitride is a promising material for refractory plasmonic devices and could enable compact vacuum ultraviolet frequency combs.

Electromagnetically Induced Gratings Created by Few-Cycle Light Pulses (Brief Review)

Electromagnetically Induced Gratings Created by Few-Cycle Light Pulses (Brief Review)

Few-cycle lightwave-driven currents in a semiconductor at high repetition rate

When an intense, few-cycle light pulse impinges on a dielectric or semiconductor material, the electric field will interact nonlinearly with the solid, driving a coherent current. An asymmetry of the ultrashort, carrier-envelope-phase-stable waveform results in a net transfer of charge, which can be measured by macroscopic electric contact leads. This effect has been pioneered with extremely short, single-cycle laser pulses at low repetition rate, thus limiting the applicability of its potential for ultrafast electronics. We investigate lightwave-driven currents in gallium nitride using few-cycle laser pulses of nearly twice the duration and at a repetition rate 2 orders of magnitude higher than in previous work. We successfully simulate our experimental data with a theoretical model based on interfering multiphoton transitions, using the exact laser pulse shape retrieved from dispersion-scan measurements. Substantially increasing the repetition rate and relaxing the constraint on the pulse duration marks an important step forward toward applications of controlling currents with light.

Broadband phase-shifting mirrors for ultrafast lasers.

Metal-dielectric phase-shifting multilayer optical elements have been developed, providing broadband, virtually dispersion-free polarization manipulation down to the few-cycle level. These optical elements are Ag/Al2O3 mirrors that operate in the spectral range from 500 to 100 nm, exhibiting reflectance higher than 95%, and a differential phase shift between the s- and p-polarization of about 90° distributed over four bounces. The mirrors have been designed, produced, and reliably characterized based on spectral photometric and ellipsometric data using a non-parametric approach as well as a multi-oscillator model. The optical elements were implemented into a few-cycle laser system, where they transformed linearly polarized few-cycle light pulses to circular polarization.

Generation of 3.9-cycle pulses from the coherent synthesis of two continuous-wave injection seeded optical parametric amplifiers at 53 MHz.

A high repetition-rate, few-cycle light pulse is of great importance due to its potential for a variety of applications, including two-dimensional infrared spectroscopy and time-resolved imaging of molecular structures, which benefit from its ultrabroadband spectrum and ultrashort pulse duration. The generation of an ultrabroadband coherent spectrum is one of the frontiers of ultrafast optics, and accessing such few-cycle pulses is presently under active exploration. Here, we demonstrate a simple yet effective pulse synthesizer. It is based on two continuous-wave (cw) injection-seeded high-repetition-rate optical parametric amplification systems and the following self-phase-modulation dominated spectra-broadening processes. The combined spectrum spans from 1250 to 1670nm, and a near Fourier-transform-limited 3.9-cycle (19.2fs) synthesized pulse with a central wavelength of 1470nm is obtained accordingly.

Carrier frequency tuning of few-cycle light pulses by a broadband attenuating mirror.

We demonstrate the performance of a novel multilayer dielectric reflective thin-film attenuator capable of reshaping the super-octave spectrum of near-single-cycle visible laser pulses without deteriorating the phase properties of the reflected light. These novel broadband attenuating mirrors reshape in a virtually dispersion-free manner the incident spectrum such that the carrier wavelength of the reflected pulses shifts from ∼700 nm (Eγ=1.77 eV) to ∼540 nm (Eγ=2.25 eV) or beyond while maintaining their initial near-single-cycle pulse duration. This constitutes a viable approach to convert a number of established few-cycle ultrafast laser systems into sources with a selectable excitation wavelength to meet the requirements of single-color/multicolor high temporal resolution spectroscopic experiments.

Harmonic generation enhancement due to interaction of few-cycle light pulses in nonlinear dielectric coating on a mirror

We theoretically investigate reflection of a few-cycle light pulse from a mirror with nonlinear dielectric coating. We employ a nonlinear equation that describes spatiotemporal evolution of a few-cycle light pulse with a broad spectrum that lies in the transparency range of nonlinear dielectric media. This model is formulated directly for the electric field without slowly varying amplitude approximation. Analytical and numerical analysis shows that counter-propagating wave interactions in thin films can strongly enhance or suppress third harmonic generation of the central frequency, whereas this effect is neglected in the framework of slowly varying amplitude approximation.

Generation of unipolar half-cycle pulses via unusual reflection of a single-cycle pulse from an optically thin metallic or dielectric layer.

We propose a strikingly simple method to form approximately unipolar half-cycle optical pulses via reflection of a single-cycle optical pulse from a thin flat metallic or dielectric layer. Unipolar pulses in reflection arise due to specifics of one-dimensional pulse propagation. Namely, we show that the field emitted by the layer is proportional to the velocity of the oscillating charges in the medium, instead of their acceleration. Besides, the oscillation velocity of the charges can be forced to keep a constant sign throughout the pulse duration. That is, reflection of ultrashort pulses from broad-area layers with nanometer-scale thickness can be very different from the common reflection in the case of longer pulses and thicker layers. This suggests a possibility of unusual transformations of few-cycle light pulses in completely linear optical systems.

Atomic coherence effects in few-cycle pulse induced ionization*

The interaction of a short, few-cycle light pulse and an atom which is prepared initially in a superposition of two stationary states is shown to exhibit strong signatures of atomic coherence. For a given waveform of the laser pulse, appropriate quantum mechanical relative phase between the constituents of the initial superposition can increase the ionization probability by a factor of three. A similarly strong effect can be observed when the waveform of the ionizing pulse is changed. These results allow for intuitive explanations, which are in agreement with the numerical integration of the time dependent Schr\"{o}dinger equation.

The interaction of excited atoms and few-cycle laser pulses

This work describes the first observations of the ionisation of neon in a metastable atomic state utilising a strong-field, few-cycle light pulse. We compare the observations to theoretical predictions based on the Ammosov-Delone-Krainov (ADK) theory and a solution to the time-dependent Schrödinger equation (TDSE). The TDSE provides better agreement with the experimental data than the ADK theory. We optically pump the target atomic species and measure the ionisation rate as the a function of different steady-state populations in the fine structure of the target state which shows significant ionisation rate dependence on populations of spin-polarised states. The physical mechanism for this effect is unknown.

Carrier envelope phase shifter for broadband terahertz pulses.

We demonstrated controlled shifting of the internal phase of broadband terahertz (THz) pulses. The internal phase of an ultrashort pulse is called the carrier envelope phase (CEP), which is an important parameter in the interaction of few-cycle light pulses and matter. Our CEP shifter utilizes the ultra-broadband feature of prism wave plates. We analytically derived the amount of CEP shift achievable by the CEP shifter using Jones matrixes. THz time-domain measurements clearly showed the shift of the CEP, and the results agreed well with the calculated values. The CEP shift was as high as 2π, indicating that any CEP values can be chosen using our CEP shifter.

Transmission of a few-Cycle Femtosecond Pulse Through an Optically Thin Plate

The article examines the interaction of a few-cycle optical pulse with an optically thin transparent and/or absorbing layer. The reflection of light energy is shown to be nonmonotone depending on layer thickness. The interaction of a few-cycle light pulse with the layer may produce total transparency of the layer for pulses of a certain carrier frequency. Absorption in the layer also has a nonmonotone effect on both reflected and transmitted light energy. The energy absorbed in the layer may decrease with increasing layer absorption coefficient due to the increase of energy reflection from the layer. The layer thickness when the reflected energy is maximized depends on the electrical conductivity of the medium. Under certain conditions, the interaction of the light pulse with the optically thin plate may essentially alter the spectrum of the reflected pulse and, in particular, its absolute phase, which depends on plate thickness. This property can be exploited in applications to generate few-cycle pulses with the required absolute phase.

Dissociation of D2+by UV and THz light pulses

The dissociation of D${}_{2}$${}^{+}$ in the few-cycle UV and THz light pulses is studied by numerically simulating the time-dependent Schr\odinger equation. With only the UV pulse, we find the dissociation probability does not increase monotonously with the increasing of the UV pulse intensity or duration. The UV-triggered dissociation is streaked by the time-delayed THz light pulse, i.e., the nuclear momentum oscillates with the half of the THz period when the UV-THz time delay or the carrier envelope phase of the THz pulse is scanned. The difference of the maximum and minimum nuclear momenta equals the THz laser vector potential. The classical calculation of the Newtonian equation for a mass point moving on the THz light-modified molecular potential curves reproduces the quantum simulation results and therefore intuitively explores the physical scenario: The nuclear wave packets propagate along the THz field-dressed molecular potential curves adiabatically but make a fully diabatic transition, while the THz electric field changes direction. This study offers a visual angle to understand the molecular dissociation in the strong laser field with very long wavelengths.

Plasmonic enhancement of High Harmonic Generation revisited: Predominance of Atomic Line Emission

We demonstrate nanostructure-enhanced extreme ultraviolet fluorescence from noble gases driven by low-energy, few-cycle light pulses. Despite suffi cient local inten- sities, plasmon-enhanced high harmonic generation is not observed, which follows from the small, nanometer-size coherent source volume.

Subexawatt few-cycle lightwave generation via multipetawatt pulse compression

We identify the physical scenarios of nonlinear spatiotemporal dynamics of extreme-power laser fields enabling compression of a broad-beam ultrafast multipetawatt laser output to subexawatt few-cycle light pulses focusable to pulse intensities up to 1025W/cm2. We show that, with a careful control over the key limiting physical effects, which include dispersion, pulse self-steepening, small-scale self-focusing, and ionization effects, enhanced self-phase modulation of multipetawatt laser waveforms in a solid medium can provide spectral bandwidths compressible to few-cycle pulse widths with output beam profiles focusable to ultrarelativistic intensities.

Above-threshold ionization in atomic hydrogen using intense, few-cycle laser pulses

The interaction of intense few-cycle light pulses and matter has given rise to a number of high-field physical processes that are of great interest. The high non-linearity of such interactions necessitates complex numerical simulations in order to retrieve useful physical measurements from the experimental data. Here we demonstrate quantitative agreement at the 10% level between experimentally obtained integrated photoelectron spectra and numerical simulations for above-threshold ionization in the intense few-cycle regime. The use of atomic hydrogen provides a key experimental innovation as it is the only electronic system for which ab initio simulations in this regime are available.