Time-delayed Pulse Research Articles

Resonance-enhanced high-order harmonic generation by combination of an infrared laser field and a time-delayed attosecond XUV pulse

Resonance-enhanced high-order harmonic generation by combination of an infrared laser field and a time-delayed attosecond XUV pulse

Complex dynamics in nonlinear small time-delayed optoelectronic oscillator and application in fast reservoir computing and pulse generation

We investigated a time-delayed optoelectronic oscillator (OEO) that displays a wide range of complex dynamic behavior under small time delay. The phase-space trajectory distributions in different dynamic regimes were compared which brings a new perspective on the underlying mechanism of the transition process. It was found that bifurcation is always possible no matter how small the time delay is even if the universal adiabatic approximation model is invalid. Hereby we proposed a versatile simple oscillator which has a potential capacity as memory carrier and high-dimensional state spatial mapping ability that brings 1000 times computing-efficiency improvements of reservoir computing over the large time delay one. Furthermore, we demonstrated a new approach for a tunable optoelectronic pulse generator (repetition rate at 0.2 MHz and 0.25 GHz) which depends critically on time-delayed input electrical pulse. The proposed oscillator is also a promising system for the applications of fast chaos-based communication.

New Instrument for Time-Resolved OH and HO2 Quantification in High-Pressure Laboratory Kinetics Studies.

We have constructed a new time-resolved high-pressure fluorescence assay by gas expansion (HP-FAGE) apparatus, optimized for the detection of OH and HO2 radicals in complex gas-phase reactions. The new instrument fills a gap in the existing experimental toolkit for chemical kinetics by enabling the quantification of two key reactive species with microsecond time resolution from high-pressure sources, which was previously not attainable. The HP-FAGE is interfaced with a flow reactor, designed for pressures up to 100 bar and temperatures up to 1000 K, in which reactions are initiated by laser photolysis of radical precursors at repetition rates of 1-10 Hz. The HP-FAGE samples gas out of the reactor into a miniature FAGE chamber, where OH is detected by resonant laser-induced fluorescence using a time-delayed probe laser pulse. HO2 is converted to OH via reaction with NO and then detected by OH fluorescence. The novel FAGE design places the probe region very close to the gas expansion, minimizing the transport time of sampled molecules and resulting in time resolution better than 20 μs for both OH and HO2. We calibrate the sensitivity of HP-FAGE, validate its performance with measurements of well-known reaction kinetics (OH + CH4, OH + OH, OH + HO2, and HO2 + HO2), and discuss prospects for its future use.

Microwave re-excitation of femtosecond laser tagging for highly flexible velocimetry.

Molecular tagging velocimetry is typically species specific and limited by excited state/species lifetimes. We utilize laser-generated ionization, long-lived anions, and a time-delayed microwave pulse to monitor the tagged region up to several milliseconds. This non-resonant excitation and microwave interaction is demonstrated in a range of gas mixtures. Signal levels show up to 1000-fold improvement, and the flexibility in interrogation time allows for velocity measurements over a large dynamic range (1-100 m/s) with single-shot precision of <5%. This approach has the potential for wide application over a range of relevant gas compositions, temperatures, and pressures.

Enhanced persistent orientation of asymmetric-top molecules induced by cross-polarized terahertz pulses

We investigate the persistent orientation of asymmetric-top molecules induced by time-delayed THz pulses that are either collinearly or cross polarized. Our theoretical and numerical results demonstrate that the orthogonal configuration outperforms the collinear one, and a significant degree of persistent orientation—approximately 10% at 5 K and nearly 3% at room temperature—may be achieved through parameter optimization. The dependence of the persistent orientation factor on temperature and field parameters is studied in detail. The proposed application of two orthogonally polarized THz pulses is both practical and efficient. Its applicability under standard laboratory conditions lays a solid foundation for future experimental realization of THz-induced persistent molecular orientation. Published by the American Physical Society 2024

Attosecond Probing of Nuclear Vibrations in the D2+ and HeH+ Molecular Ions.

We study the ultrafast photodissociation of small diatomic molecules using attosecond laser pulses of moderate intensity in the (extreme) ultraviolet regime. The simultaneous application of subfemtosecond laser pulses with different photon energies─resonant in the region of the molecular motion─allows one to monitor the vibrational dynamics of simple diatomics, like the D2+ and HeH+ molecular ions. In our real-time wave packet simulations, the nuclear dynamics is initiated either by sudden ionization (D2+) or by explicit pump pulses (HeH+) via distortion of the potential energy of the molecule. The application of time-delayed attosecond pulses leads to the breakup of the molecules, and the information on the underlying bound-state dynamics is imprinted in the kinetic energy release (KER) spectra of the outgoing fragments. We show that the KER-delay spectrograms generated in our ultrafast pump-probe schemes are able to reconstruct the most important features of the molecular motion within a given electronic state, such as the time period or amplitude of oscillations, interference patterns, or the revival and splitting of the nuclear wave packet. The impact of probe pulse duration, which is key to the applicability of the presented mapping scheme, is investigated in detail.

Role of the Cohen-Fano interference in recoil-induced rotation.

We study the rotational dynamics induced by the recoil effect in diatomic molecules using time-resolved two-color x-ray pump-probe spectroscopy. A short pump x-ray pulse ionizes a valence electron inducing the molecular rotational wave packet, whereas the second time-delayed x-ray pulse probes the dynamics. An accurate theoretical description is used for analytical discussions and numerical simulations. Our main attention is paid to the following two interference effects that influence the recoil-induced dynamics: (i) Cohen-Fano (CF) two-center interference between partial ionization channels in diatomics and (ii) interference between the recoil-excited rotational levels manifesting as the rotational revival structures in the time-dependent absorption of the probe pulse. The time-dependent x-ray absorption is computed for the heteronuclear CO and homonuclear N2 molecules as showcases. It is found that the effect of CF interference is comparable with the contribution from independent partial ionization channels, especially for the low photoelectron kinetic energy case. The amplitude of the recoil-induced revival structures for the individual ionization decreases monotonously with a decrease in the photoelectron energy, whereas the amplitude of the CF contribution remains sufficient even at the photoelectron kinetic energy below 1eV. The profile and intensity of the CF interference depend on the phase difference between the individual ionization channels related to the parity of the molecular orbital emitting the photoelectron. This phenomenon provides a sensitive tool for the symmetry analysis of molecular orbitals.

Suppressing Metal Nanoparticle Ablation with Double-Pulse Femtosecond Laser Sintering.

As a branch of laser powder bed fusion, selective laser sintering (SLS) with femtosecond (fs) lasers and metal nanoparticles (NPs) can achieve high precision and dense submicron features with reduced residual stress, due to the extremely short pulse duration. Successful sintering of metal NPs with fs laser is challenging due to the ablation caused by hot electron effects. In this study, a double-pulse sintering strategy with a pair of time-delayed fs-laser pulses is proposed for controlling the electron temperature while still maintaining a high enough lattice temperature. We demonstrate that when delay time is slightly longer than the electron-phonon coupling time of Cu NPs, the ablation area was drastically reduced and the power window for successful sintering was extended by about two times. Simultaneously, the heat-affected zone can be reduced by 66% (area). This new strategy can be adopted for all the SLS processes with fs laser and unlock the power of SLS with fs lasers for future applications.

Picosecond Ultrasonics for Studying Elastic Modulus of Polycrystalline Chromium Nanofilms: Thickness Dependence and Stiffness Enhancement

Accurate measurement of elastic constants in thin films is still an important issue to understand the scale behavior of nanosized materials. In the present study, we introduced an advanced non-destructive method, picosecond ultrasonics (PU), for measuring the out-of-plane elastic modulus of thin chromium (Cr) films. The femtosecond light pulse is focused on the Cr film to excite the longitudinal acoustic phonons (LAP), which propagate along the thickness direction and repeat reflections inside the Cr film. Then, the propagation/distribution of LAP is detected by the time-delayed probe light pulse through the photoelastic effect. Therefore, we can determine the out-of-plane modulus by measuring the periodic pulse echoes or the breathing mode vibrations within the Cr film. For most Cr films, the determined modulus is smaller than the corresponding bulk value and decreases with the decreasing thickness, while for some Cr films, it closes and may exceed the bulk value. This work describes the thickness-dependent elasticity of thin Cr films and provides evidence of the stiffness enhancement in Cr films on the Si substrate. In addition, since LAP with central frequency up to 310 GHz is excited in Cr films on the SiO2 substrate, we also demonstrate the potential of Cr films as high-frequency photoacoustic transducers.

Steering thermal photoassociation of magnesium atoms by two time-delayed femtosecond laser pulses

By solving the full-dimensional time-dependent Schrödinger equation with the thermal-random-phase wavepacket method, we investigate the photoassociation (PA) process of hot (1000 K) magnesium atoms induced by two time-delayed femtosecond laser pulses. Driven by the 840 nm fs laser pulses, the Mg2 molecules can be formed on the four excited states, (1)1Πg, (1)1Πu, (2)1Πu, and (2)1Σu+, from the initial electronic ground state X1Σg+. It is found that the three-photon couplings between X1Σg+ and the three ungerade states [(1)1Πu (2)1Πu, and (2)1Σu+], play dominant roles in the population transfer process. By scanning the pulse duration τ from 50 to 200 fs, and varying the delay time δt0 from 0 to 2τ fs, we find that the final PA population is strongly dependent on the two parameters. For a given δt0, the parameter τ can induce a significant variation (2 ∼ 6.8 times) for the final PA population transfer, and for a given τ, one can also obtain a significant variation (2.7 ∼ 3.5 times) of the final PA population by varying δt0. Additionally, the dynamics of the coherently vibrational wavepackets of the four excited states are also influenced by the two parameters.

Visualizing ultrafast weak-field-induced rotational revivals of air molecules at room temperature.

The ability to observe quantum coherence and interference is crucial for understanding quantum effects in nonlinear optical spectroscopy and is of fundamental interest in quantum mechanics. Here, we present an experimental study combined with theoretical analysis and numerical simulations to identify the underlying process behind the rotational revivals induced by a pair of time-delayed ultrafast femtosecond laser pulses for air molecules under ambient conditions. Our time-resolved two-dimensional alignment measurements confirm that one-step non-resonant Raman transitions from initial states of mixed molecules play a dominant role, showing a signature of weak-field-induced rotational revivals. Furthermore, we demonstrate that such rotational revival spectra can simultaneously measure the entire pure rotational Raman spectra and observe the quantum interference between two transition pathways from a given initial state. This work provides a powerful tool to observe, control, and identify the rotational dynamics of mixed molecular samples under weak-field excitations.

Stimulated Raman adiabatic passage with trains of weak pulses* *This work is dedicated to Bruce Shore, a brilliant and inspiring physicist, a pioneer in coherent light–matter interaction theory, a mentor and a friend.

We consider coherent population transfer in multilevel quantum systems driven by time-delayed pulse trains. We show how to choose the parameters of the trains so that the population dynamics tracks the behavior of a Λ-type three-level system under stimulated Raman adiabatic passage (STIRAP). Efficient population transfer can be achieved regardless of the order and with or without overlap of the pump and the Stokes sub-pulses of the trains. Generalized STIRAP schemes of population transfer in N-level system with sequential couplings are also examined. The mechanism of the population transfer and the robustness of the proposed schemes are discussed.

Quantum Interference Paves the Way for Long-Lived Electronic Coherences.

The creation and dynamical fate of a coherent superposition of electronic states generated in a polyatomic molecule by broadband ionization with extreme ultraviolet pulses is studied using the multiconfiguration time-dependent Hartree method together with an ionization continuum model Hamiltonian. The electronic coherence between the hole states usually lasts until the nuclear dynamics leads to decoherence. A key goal of attosecond science is to control the electronic motion and design laser control schemes to retain this coherence for longer timescales. Here, we investigate this possibility using time-delayed pulses and show how this opens up the prospect of coherent control of charge migration phenomenon.

Controlling electron recollision with combined linear and circular polarization

We theoretically investigate the non-sequential double ionization of Ar atoms in the combined fields of linearly polarized laser and circularly polarized laser through 3D semiclassical simulations. By partially overlapping the two time-delayed multicycle laser pulses, we construct an optical waveform whose polarization ellipticity increase slowly for consecutive optical cycles. This composite laser pulses with the time-dependent ellipticity can tunnel-ionize atoms and steer the first tunneling electron to recollision with the second bound electron through different trajectories, in which the recollision occurs with different return times of the first ionized electron. Through tuning delay time between the two laser pulses, the double ionization yields and recollision trajectories with different return times can be controlled. The time-dependent ellipticity with different delay time can enhance or suppress the probability of different return times. This work provides a scheme exploring electron dynamics in few optical cycle or even subcycle time scale in a multicycle laser field without having to be limited to near-single-cycle laser pulses.

All-optical valley switch and clock of electronic dephasing.

2D materials with broken inversion symmetry posses an extra degree of freedom, the valley pseudospin, that labels in which of the two energy-degenerate crystal momenta, K or K', the conducting carriers are located. It has been shown that shining circularly-polarized light allows to achieve close to 100% of valley polarization, opening the way to valley-based transistors. Yet, switching of the valley polarization is still a key challenge for the practical implementation of such devices due to the short valley lifetimes. Recent progress in ultrashort laser technology now allows to produce trains of attosecond pulses with controlled phase and polarization between the pulses. Taking advantage of such technology, we introduce a coherent control protocol to turn on, off and switch the valley polarization at faster timescales than electron-hole decoherence and valley depolarization, that is, an ultrafast optical valley switch. We theoretically demonstrate the protocol for hBN and MoS2 monolayers calculated from first principles. Additionally, using two time-delayed linearly-polarized pulses with perpendicular polarization, we show that we can extract the electronic dephasing time T2 from the valley Hall conductivity.

Creating alignment echoes using a phase-shaped femtosecond laser pulse

In recent years, molecular alignment echoes induced by a pair of time-delayed femtosecond laser pulses have been proposed and have aroused wide research interest. However, we demonstrate that an alignment echo can be alternatively produced by a shaped femtosecond laser pulse with a V-style spectral phase modulation. The full, fractional, and imaginary alignment echoes are formed by the excitation of the tailored two time-delayed sub-pulses. Both the delay time and the ratio of intensity between the two sub-pulses can be easily manipulated by designing the modulation parameters to induce various types of echoes. We further show that the optimal ratio of intensity between the two sub-pulses, which results in the maximal alignment degrees of the full echo, closely correlates with the energy of the sub-pulse. When the pulse energy is relatively low, the maximal alignment degree of the full echo is obtained when the two sub-pulses have equal intensity. The optimal ratio of intensity increases with the excitation energy of the first pump pulse.

All-Optical Switching on the Nanometer Scale Excited and Probed with Femtosecond Extreme Ultraviolet Pulses

Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path toward future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by the interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range. The subsequent ultrafast evolution of the magnetization pattern is probed by diffraction of a third, time-delayed pulse tuned to the Gd N-edge at a wavelength of 8.3 nm. By examining the simultaneously recorded first and second order diffractions and by performing reference real-space measurements with a wide-field magneto-optical microscope with femtosecond time resolution, we can conclusively demonstrate the ultrafast emergence of all-optical switching on the nanometer length scale.

On the rigidity of four hundred Pickering-stabilised microbubbles

This study explores the rigidity of Pickering-stabilised microbubbles subjected to low-amplitude ultrasound. Such microbubbles might be suitable ultrasound contrast agents. Using an adapted Rayleigh–Plesset equation, we modelled the dynamics of microbubbles with a 7.6-N m−1 shell stiffness under 1-MHz, 0.2-MPa sonication. Such dynamics were observed experimentally, too, using high-speed photography. The maximum expansions were agreeing with those predicted for Pickering-stabilised microbubbles. Subjecting microbubbles to multiple time-delayed pulses yielded the same result. We conclude that Pickering-stabilised microbubbles remain very stable at low acoustic amplitudes.

Optical Frequency Comb-Based Direct Two-Photon Cooling for Cold Atom Clock

The performance of the cold atom clock based on coherent population trapping (CPT) improved when the temperature decreased. In order to obtain a lower temperature in the cold atom clock, we proposed a cooling scheme in this paper that employs direct two-photon transition using optical frequency combs (OFCs). Two trains of time-delayed pulses from opposite directions were utilized to interact with atoms. It was found that the temperature of the cold atoms reached the minimum if the pulse area was π and the time delay between the absorption pulse and the stimulated emission pulse was in the range from 0.7τ to τ. In this paper, it was confirmed that the proposed cooling process allowed for faster and more efficient momentum exchange between light and atoms, and the proposed cooling process could be applied to the atoms or molecules that could not be cooled to desired temperature through the single-photon cooling process. The 87Rb cooling, together with the CPT interrogating scheme using OFCs reduced the ratio value of linewidth/contrast, and the frequency stability of the cold atom clock hence improved by more than six times as per our calculation.

Accurate optically pumped magnetometer based on Ramsey-style interrogation.

Light-atom interactions during spin preparation and readout in optically pumped magnetometers can lead to inaccuracies. We demonstrate a novel, to the best of our knowledge, detection strategy that exploits an interrogation sequence in the pulsed free-induction-decay modality to suppress these systematic errors. The technique is predicated on monitoring the dynamics of preoriented atomic spins as they evolve unperturbed during a dark interval, by subsequently applying a time-delayed optical pulse to infer the spin state's phase. This detection mode reduced light shift inaccuracies to within 0.6 nT, and could be employed in a wide variety of high-precision atomic magnetometry experiments.