Optical Cycles Research Articles

Study of the effect of higher-order dispersions on photoionisation induced by ultrafast laser pulses applying a classical theoretical method

We investigated the effect of higher order dispersion on ultrafast photoionisation with Classical Trajectory Monte Carlo (CTMC) method for hydrogen and krypton atoms. In our calculations we used linearly polarised ultrashort 7 fs laser pulses, 6.5 times 10^{14} mathrm {W/cm^{2}} intensity, and a central wavelength of 800 nm. Our results show that electrons with the highest kinetic energies are obtained with transform limited (TL) pulses. The shaping of the pulses with negative second- third- or fourth- order dispersion results in higher ionisation yield and electron energies compared to pulses shaped with positive dispersion values. We have also investigated how the Carrier Envelope Phase (CEP) dependence of the ionisation is infuenced by dispersion. We calculated the left-right asymmetry as a function of energy and CEP for sodium atoms employing pulses of 4.5 fs, 800 nm central wavelength, and 4 times 10^{12}mathrm {W/cm^{2}} intensity. We found that the left-right asymmetry is more pronounced for pulses shaped with positive Group Delay Dispersion (GDD). It was also found that shaping a pulse with increasing amounts of GDD in absolute value blurs the CEP dependence, which is attributed to the increasing number of optical cycles.

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.

Carrier-envelope phase effect on light bullet dynamics

A light bullet (LB) is a wave packet of a few optical cycles that is extremely compressed in space and time, which is formed in the bulk transparent dielectric during femtosecond filamentation under anomalous group velocity dispersion. We demonstrate for the first time that the carrier-envelope phase shift during propagation of a near single-cycle LB causes synchronous oscillations of the spatial, temporal and energy parameters of its core with the period decreasing with increasing carrier wavelength. When analyzing the structure of color centers and induced plasma channels in fluorides, it was experimentally found that LB parameter oscillations lead to a periodic change in the nonlinear optical interaction with the dielectric.

Photoionization cross sections of ultracold 88Sr in 1P1 and 3S1 states at 390 nm and the resulting blue-detuned magic wavelength optical lattice clock constraints.

We present the measurements of the photoionization cross sections of the excited 1P1 and 3S1 states of ultracold 88Sr atoms at 389.889 nm wavelength, which is the magic wavelength of the 1S0-3P0 clock transition. The photoionization cross section of the 1P1 state is determined from the measured ionization rates of 88Sr in the magneto-optical trap in the 1P1 state to be 2.20(50)×10-20 m2, while the photoionization cross section of 88Sr in the 3S1 state is inferred from the photoionization-induced reduction in the number of atoms transferred through the 3S1 state in an operating optical lattice clock to be 1.38(66) ×10-18 m2. Furthermore, the resulting limitations of employing a blue-detuned magic wavelength optical lattice in strontium optical lattice clocks are evaluated. We estimated photoionization induced loss rates of atoms at 389.889 nm wavelength under typical experimental conditions and made several suggestions on how to mitigate these losses. In particular, the large photoionization induced losses for the 3S1 state would make the use of the 3S1 state in the optical cycle in a blue-detuned optical lattice unfeasible and would instead require the less commonly used 3D1,2 states during the detection part of the optical clock cycle.

10-µJ few-cycle 12-µm source based on difference-frequency generation driven by a 1-kHz mid-wave infrared OPCPA.

We report on high-energy, few-cycle pulse generation in the long-wave infrared spectral region via difference-frequency generation (DFG) in GaSe and AgGaSe2 nonlinear crystals. The DFG is driven by the signal at 3.5 µm and idler at 5 µm of a high-power mid-wave infrared optical parametric chirped pulse amplification (OPCPA) system operating at a 1-kHz repetition rate. The DFG pulses contain up to 17 µJ of energy and cover a spectrum from 8.5 µm to 14.5 µm. They are generated with a conversion efficiency of 2.1 %. Compression results in 10.2-μJ pulses with sub-150-fs duration, corresponding to less than four optical cycles.

Scalable high-repetition-rate sub-half-cycle terahertz pulses from spatially indirect interband transitions

Intense phase-locked terahertz (THz) pulses are the bedrock of THz lightwave electronics, where the carrier field creates a transient bias to control electrons on sub-cycle time scales. Key applications such as THz scanning tunnelling microscopy or electronic devices operating at optical clock rates call for ultimately short, almost unipolar waveforms, at megahertz (MHz) repetition rates. Here, we present a flexible and scalable scheme for the generation of strong phase-locked THz pulses based on shift currents in type-II-aligned epitaxial semiconductor heterostructures. The measured THz waveforms exhibit only 0.45 optical cycles at their centre frequency within the full width at half maximum of the intensity envelope, peak fields above 1.1 kV cm−1 and spectral components up to the mid-infrared, at a repetition rate of 4 MHz. The only positive half-cycle of this waveform exceeds all negative half-cycles by almost four times, which is unexpected from shift currents alone. Our detailed analysis reveals that local charging dynamics induces the pronounced positive THz-emission peak as electrons and holes approach charge neutrality after separation by the optical pump pulse, also enabling ultrabroadband operation. Our unipolar emitters mark a milestone for flexibly scalable, next-generation high-repetition-rate sources of intense and strongly asymmetric electric field transients.

Versatile few-cycle high-energy MID-IR OPCPA for nonlinear optics, spectroscopy and imaging

High-power, high-energy, ultrashort, mid-infrared (MID-IR) laser systems operating at high repetition rates are of considerable interest for many science applications, such as coherent vibrational spectroscopy, label-free imaging, time-resolved pump-probe and high-harmonic generation studies. We developed an optical parametric chirped-pulse amplifier (OPCPA) system employing a difference-frequency generation in a lithium gallium sulfide nonlinear crystal in the final amplifier stage, which provides in principle the possibility for passive carrier-envelop-phase (CEP) stability. The OPCPA efficiently down-converts a 1 μm 200 μJ Yb-YAG pump pulse into the MID-IR spectral range generating μJ-level pulses at a repetition rate of 200 kHz. Two modes of operations providing complimentary MID-IR pulse properties are presented. Depending on the envisaged application, one can switch between (a) a wavelength-tunable (4.2–11 μm) source and (b) a broadband source centered at ≈8.5 μm by controlling the group-delay dispersion of the signal pulse. The broadband, high-energy MID-IR pulses have a short pulse duration of 74±2 fs, which corresponds to only ≈3 optical cycles at the central wavelength of 8.5 μm.

Numerical investigation of the nonlinear spectral broadening aiming at a few-cycle regime for 10 ps level Nd-doped lasers

We present a cascaded nonlinear spectral broadening scheme for Nd-doped lasers, featuring with long pulse duration and high average power. This scheme is based on two multi-pass cells (MPCs) and one multiple-plate supercontinuum generation (MPSG), and the numerical investigation is driven by a home-made Nd-doped fiber laser with 12 ps pulse duration, 50 kHz repetition rate and 100 W average power. The MPC-based first two stages allow us to broaden the pulse spectrum to 4 nm and 43 nm respectively, and subsequently, the MPSG-based third stage allows us to reach 235 nm spectral bandwidth. This broadened spectrum can support a Fourier-transfer-limited pulse duration of 9.8 fs, which is shorter than three optical cycles. To the best of our knowledge, it is the first time to demonstrate the possibility of few-cycle pulses generation based on the 10 ps level Nd-doped lasers. Such few-cycle and high average power laser sources should be attractive and prospective, benefiting from the characteristics of structure compact, low-cost and flexibility.

Sub-optical-cycle electron pulse trains from metal nanotips

The coherent modulation of swift electron beams with strong laser fields has enabled the generation of attosecond electron pulses, opening up new research avenues in ultrafast science. Here we study a comparatively simple alternative, the production of electron pulse trains directly at the source. In our theory work, we show that sub-optical-cycle electron bursts induced by tunneling photoemission from a metal nanotip can retain the temporal fingerprint of their emission dynamics in a typical low-energy point-projection microscope setup. We find that strong acceleration by a static field, a short propagation distance and a sufficiently large optical cycle duration mitigate temporal smearing due to matter-wave dispersion. Our approach enables studies of coherent interactions of slow electrons with matter on sub-femtosecond and nanometer scales, a regime which has hitherto remained inaccessible.

Nonlinear propagation effect in x-ray parametric amplification during high harmonic generation

We report the realization and characterization of parametric amplification in high harmonic generation around 100 eV using He gas in a double gas jet arrangement. The delay of the seed extreme ultraviolet (XUV) pulse with respect to the amplifier gas jet was scanned by changing the distance between the gas jets. Experiments and numerical calculations show that parametric amplification occurs within a temporal window of several optical cycles. Strong correlation between the seed and amplifier was observed in a shorter, few optical cycles delay range, which appeared as a modulation of the XUV intensity with an unexpected one optical cycle periodicity instead of half optical cycle. Simulations revealed that the strong correlation and also the unusual periodicity was the consequence of the nonlinear effect produced by plasma dispersion on the parametric amplification process during propagation in the amplifier jet.

Li+/Al3+ Composite Solid Electrolyte Based Electro‐Thermal Dual Responsive Devices with Optimized Optical Contrast and Cycle Durability

AbstractThe limited optical contrast and band adjustment range are the main factors that restrict chromic materials. In this study, Li+/Al3+ composite solid electrolyte is incorporated between VO2 and WO3 chromic functional layers to construct a new type of VO2 based electrothermal dual responsive devices. The dual responsive devices deliver optical contrast over 50% and independent modulation of visible and near infrared band. In addition to displaying four reversible optical states in response to environmental temperature and external voltage, the devices effectively utilize the synergistic effect of Li+/Al3+ hybrid ions. Furthermore, the optimized Li+/Al3+ composite electrolyte is proved to effectively control phase transition of VO2 and significantly improve the electrochromic properties of WO3 as well. Finally, the electro‐thermal dual responsive devices show excellent service stability in simulated outdoor environment of over 10 000 cycles. Combined with the above advantages, it is expected to develop smart windows and derivative products with large size, long life, remarkable energy saving effect and pleasant comfort.

Efficient generation of few-cycle pulses beyond 10\xa0\u03bcm from an optical parametric amplifier pumped by a 1-\xb5m laser system

Nonlinear vibrational spectroscopy profits from broadband sources emitting in the molecular fingerprint region. Yet, broadband lasers operating at wavelengths above 7 μm have been lacking, while traditional cascaded parametric frequency down-conversion schemes suffer from exceedingly low conversion efficiencies. Here we present efficient, direct frequency down-conversion of femtosecond 100-kHz, 1.03-μm pulses to the mid-infrared from 7.5 to 13.3 μm in a supercontinuum-seeded, tunable, single-stage optical parametric amplifier based on the wide-bandgap material Cd0.65Hg0.35Ga2S4. The amplifier delivers near transform-limited, few-cycle pulses with an average power > 30 mW at center wavelengths between 8.8 and 10.6 μm, at conversion efficiencies far surpassing that of optical parametric amplification followed by difference-frequency generation or intrapulse difference-frequency generation. The pulse duration at 10.6 μm is 101 fs corresponding to 2.9 optical cycles with a spectral coverage of 760–1160 cm−1. CdxHg1−xGa2S4 is an attractive alternative to LiGaS2 and BaGa4S7 in small-scale, Yb-laser-pumped, few-cycle mid-infrared optical parametric amplifiers and offers a much higher nonlinear figure of merit compared to those materials. Leveraging the inherent spatial variation of composition in CdxHg1−xGa2S4, an approach is proposed to give access to a significant fraction of the molecular fingerprint region using a single crystal at a fixed phase matching angle.

Attosecond-Resolved Coherent Control of Lattice Vibrations in Thermoelectric SnSe.

Manipulating lattice vibrations is the cornerstone to achieving ultralow thermal conductivity in thermoelectrics. Although spatial control by novel material designs has been recently reported, temporal manipulation, which can shape thermoelectric properties under nonequilibrium conditions, remains largely unexplored. Here, taking SnSe as a representative, we have demonstrated that in the ultrafast pump-pump-probe spectroscopy, electronic and lattice coherences inherited from optical excitations can be exploited independently to manipulate phonon oscillations in a highly selective manner. Specifically, when the pump-pump delay time (tmod) is in the electronic coherence time range, the amplitude, frequency, and lifetime of all phonon modes are simultaneously following the optical cycle. While extending tmod into the lattice coherence time range, the amplitude of each coherent phonon mode can be selectively manipulated according to its intrinsic period without changing the frequency and lifetime. This work opens up exciting avenues to temporally and discriminatorily manipulate phononic processes in thermoelectric materials.

Laser-coolable AcOH+ ion for CP -violation searches

The ${\mathrm{AcOH}}^{+}$ molecular ion is identified as a prospective system to search for $\mathcal{CP}$-violation effects. According to our study ${\mathrm{AcOH}}^{+}$ belongs to the class of laser-coolable polyatomic molecular cations implying a large coherence time in the experiments to study symmetry-violating effects of fundamental interactions. We perform both nuclear and high-level relativistic coupled cluster electronic structure calculations to express the experimentally measurable $\mathcal{T},\mathcal{P}$-violating energy shift in terms of fundamental quantities such as the nuclear magnetic quadrupole moment (MQM), electron electric dipole moment ($e\mathrm{EDM}$) and dimensionless scalar-pseudoscalar nuclear-electron interaction constant. We further express nuclear MQM in terms of the strength constants of $\mathcal{CP}$-violating nuclear forces: quantum chromodynamics vacuum angle $\overline{\ensuremath{\theta}}$ and quark chromo-EDMs. The equilibrium structure of ${\mathrm{AcOH}}^{+}$ in the ground and the four lowest excited electronic states was found to be linear. The calculated Franck-Condon factors and transition dipole moments indicate that the laser cooling using an optical cycle involving the first excited state is possible for the trapped ${\mathrm{AcOH}}^{+}$ ions with the Doppler limit estimated to be $\ensuremath{\sim}$4 nK. The lifetime of the ($0,{1}^{1},0$) excited vibrational state considered as a working one for MQM and $e\mathrm{EDM}$ search experiments is estimated to be $\ensuremath{\sim}0.4$ s.

Spectral phase sensitivity of frequency resolved optical switching for broadband IR pulse characterization.

In this work, we demonstrate the sensitivity of the frequency-resolved optical switching (FROSt) technique to detect a small amount of spectral phase shift for the precise characterization of ultrashort laser pulses. We characterized fs pulses centered at 1.75 µm that are spectrally broadened up to 700 nm of bandwidth in a hollow-core fiber and subsequently compressed down to 2.3 optical cycle duration by propagation in the air at atmospheric pressure. By inserting thin fused silica windows of different thicknesses in the beam path, we accurately retrieve group delay dispersion (GDD) variations as small as 10 fs2. Such GDD variations correspond to a change of the pulse duration of only 0.2 fs for a Fourier transform limited 2-cycle pulse at 1.75 µm (i.e., 11.8 fs). The capability to measure such tiny temporal variations thus demonstrates that the FROSt technique has sufficient sensitivity to precisely characterize single-cycle pulses.

The role of asymmetry in few-cycle, mid-IR pulses during THz pulse generation

The efficiency of terahertz (THz) pulse generation improves at longer driving wavelengths. For this reason, the use of mid-infrared (MIR) sources is more advantageous compared to visible or near-infrared systems. In this work, we investigate how single-color and two-color schemes of MIR pulses with few-cycle pulse durations compare in producing THz pulses. The results reveal that as the duration of the driving pulses decreases, the second harmonic generation crystal can be omitted from the system. Our numerical study pinpointed three regions where the optimal pulse parameters are fundamentally different for the most efficient THz pulse generation. The first is the two-color approach, where the two-color scheme is dominant at 3.2 optical cycles and over. The second is the single-color approach, where the single-color scheme becomes dominant at 1.7 optical cycles and below. Therefore, it simplifies the traditional two-color scheme for THz pulse generation. There is also a third transitional region where the two-color scheme still prevails, but the sign of the relative phase between the input pulses becomes important. Considering the effect of the relative phase and the carrier to envelope phase (CEP) effect on the THz pulse generation, the results have shown that as the pulse duration become shorter, the role of the CEP becomes important for efficient THz generation. By measuring the efficiency of the THz generation in this optical arrangement, quantifying the CEP becomes possible, which could become an important experimental tool for few-cycle, MIR laser technology.

Identifying the complexity of the holographic structures in strong field ionization

We present numerical investigations of the strong-field attosecond photoelectron holography by analyzing the holographic interference structures in the two-dimensional photoelectron momentum distribution (PMD) in hydrogen atom target induced by a strong infrared laser pulse. The PMDs are calculated by solving the full-dimensional time-dependent Schrödinger equation. The effect of the number of optical cycles on the PMD is considered and analyzed. We show how the complex interference patterns are formed from a single-cycle pulse to multi-cycle pulses. Furthermore, snapshots of the PMD during the time evolution are presented for a single-cycle pulse in order to track the formation of the so-called fish-bone like holographic structure. The spider- and fan-like holographic structures are also identified and investigated. We found that the fan-like structure could only be identified clearly for pulses with three or more optical cycles and its symmetry depends closely on the number of optical cycles. In addition, we found that the intensity and wavelength of the laser pulse affect the density of interference fringes in the holographic patterns. We show that the longer the wavelength, the more the holographic structures are confined to the polarization axis.

Precise control of intracycle interference with a phase-stabilized polarization-gated laser pulse

We investigate photoelectron momentum distribution (PMD) from strong-field ionization of Ar by a polarization-gated (PG) pulse constructed by a left circularly polarized and a time-delayed right circularly polarized carrier-envelope phase stabilized few-cycle laser pulse. We experimentally demonstrate the feasibility of using a PG pulse to precisely control the interferences between electron wave packets (EWPs) released at different times within one optical cycle. In contrast to previous works where the various types of intracycle interferences are usually hardly resolved and separated, our work shows that, with this specific PG control scheme, it becomes possible to create a highly distinct interference pattern composed of well-separated structures produced by different types of intracycle interferences in the measured PMD. Quantum trajectory Monte Carlo simulations reproduce well the experimental findings and uncover the physical mechanism behind this subcycle control of EWPs with a PG pulse.

Control of spectral shift, broadening, and pulse compression during mid-IR self-guiding in high-pressure gases and their mixtures.

Precise control of the nonlinear optical phenomena is the limiting factor for the spectral broadening and pulse compression techniques for high-power laser systems. Here we demonstrate that generation of the blue and red components under filamentation of 4.55-μm mid-IR pulses can be easily adjusted independently through the use of inert and molecular gases, while uniform broadening up to 1-μm bandwidth at the 1/e2 level relies on the proper choice of gas mixture and its compounds partial pressure. Such synthesized media provide a feasible route for the free of damage control of pulse spectral broadening and compression for gigawatt peak power laser systems operating in the mid-IR. Additional management of a generated spectrum can be realized through the adjustment of focusing conditions. The resulted pulse is compressed by a factor of 2.6 down to 62 fs pulse duration (4.1 optical cycles) with additional dispersion compensation. Controllable nonlinear compression down to four optical cycles keeping the millijoule energy level of a mid-IR laser pulse provides direct access to extreme nonlinear optics.

Single-cycle-pulse generation in a coherently mode-locked laser with an ultrashort cavity

We theoretically investigate the possibility of a passive mode-locking regime in a two-section laser with an ultrashort cavity of the length around ten wavelengths of the medium resonant transition or even less. It is shown that such a regime is enabled through the coherent mode-locking phenomena arising due to the self-induced transparency when the gain and absorption bandwidths do not impose any restrictions on the duration of the generated pulse. Under such conditions, a laser with an ultrashort cavity could produce output pulses with the terahertz (THz) repetition rate and the duration up to a single optical cycle. Moreover, several scaling rules were derived, which allow for further shortening of the output pulse duration with the respective scaling of the media parameters.