Ultrashort Time Scales Research Articles

Non-thermal evolution of dense plasmas driven by intense x-ray fields

The advent of x-ray free-electron lasers has enabled a range of new experimental investigations into the properties of matter driven to extreme conditions via intense x-ray-matter interactions. The femtosecond timescales of these interactions lead to the creation of transient high-energy-density plasmas, where both the electrons and the ions may be far from local thermodynamic equilibrium. Predictive modelling of such systems remains challenging because of the different timescales at which electrons and ions thermalize, and because of the vast number of atomic configurations required to describe highly-ionized plasmas. Here we present CCFLY, a code designed to model the time-dependent evolution of both electron distributions and ion states interacting with intense x-ray fields on ultra-short timescales, far from local thermodynamic equilibrium. We explore how the plasma relaxes to local thermodynamic equilibrium on femtosecond timescales in terms of the charge state distribution, electron density, and temperature.

The defect-state-assisted enhancement of high harmonic generation in bulk ZnO

Optical modulation of high harmonic generation (HHG) at ultrashort timescales is of fundamental interest and central importance for emerging photonic applications. Traditionally, this modulation is realized by injecting incoherent electrons into the conduction band, which can only result in the suppression of HHG intensity. In this work, we have proposed and demonstrated an all-optical route to amplify a specific order of high harmonic generation in (11-20)-cut wurtzite zinc oxide (ZnO) based on the pump-probe configuration. Specifically, intensity enhancement is demonstrated by tuning the wavelength of the generation middle-infrared pulse when the wavelength of HHG matches the energy of a specific defect state. The maximum enhancement factor is observed to be 1.8, while the modulation speed varies with different defect states, which are 0.1 ps for the 5th HHG and 1.5 ps for the 4th HHG. This work might enlighten a new path for ultrafast modulation of HHG in solids for the future development of all-optical devices.

Selection rules for ultrafast laser excitation and detection of spin correlation dynamics in a cubic antiferromagnet

Exchange interactions determine the correlations between microscopic spins in magnetic materials. Probing the dynamics of these spin correlations on ultrashort length and time scales is, however, rather challenging, since it requires simultaneously high spatial and high temporal resolution. Recent experimental demonstrations of laser-driven two-magnon modes---zone-edge excitations in antiferromagnets governed by exchange coupling---posed questions about the microscopic nature of the observed spin dynamics, the mechanism underlying its excitation, and their macroscopic manifestation enabling detection. Here, on the basis of a simple microscopic model, we derive the selection rules for cubic systems that describe the polarization of pump and probe pulses required to excite and detect dynamics of nearest-neighbor spin correlations and can be employed to isolate such dynamics from other magnetic excitations and magneto-optical effects. We show that laser-driven spin correlations contribute to optical anisotropy of the antiferromagnet even in the absence of spin-orbit coupling. In addition, we highlight the role of subleading anisotropy in the spin system and demonstrate that the dynamics of the antiferromagnetic order parameter occurs only in next-to-leading order, determined by the smallness of the magnetic anisotropy as compared to the isotropic exchange interactions in the system. We expect that our results will stimulate and support further studies of magnetic correlations on the shortest length and time scales.

Ultrafast Control of the Optical Transition in Type-II Colloidal Quantum Wells

Manipulating the optical transition in semiconductors at ultrashort timescales is of both fundamental interest and central importance for emerging photonic applications. Traditionally, this manipulation is realized by electrostatic gating via Stark effects or band-gap renormalizations. Here, we report an ultrafast and all-optical route to engineer an indirect transition in core–crown colloidal quantum wells (CQWs), namely, CdSe/CdTe, with a type-II band alignment. Following the intense laser pulse excitation, the indirect band transition energy exhibits a pronounced blueshift–redshift crossover on the picosecond timescale, stemming from the formation and dissipation of the transient electric field (E-field) that forms upon photoexcitation to compensate for the driving force provided by the band offsets. Both the energy shift and dynamics of the transient E-field can be modulated optically by tuning the laser pulse excitation fluence. Our finding demonstrates a strong analogy between the type-II heterojunction and a p–n junction with respect to carrier equilibrium processes, which holds promise to facilitate the integration of CQWs within optical switching networks.

The role of symmetric vibrational modes in the decoherence of correlation-driven charge migration.

Due to the electron correlation, the fast removal of an electron from a molecule may create a coherent superposition of cationic states and in this way initiate pure electronic dynamics in which the hole-charge left by the ionization migrates throughout the system on an ultrashort time scale. The coupling to the nuclear motion introduces a decoherence that eventually traps the charge, and crucial questions in the field of attochemistry include how long the electronic coherence lasts and which nuclear degrees of freedom are mostly responsible for the decoherence. Here, we report full-dimensional quantum calculations of the concerted electron-nuclear dynamics following outer-valence ionization of propynamide, which reveal that the pure electronic coherences last only 2-3fs before being destroyed by the nuclear motion. Our analysis shows that the normal modes that are mostly responsible for the fast electronic decoherence are the symmetric in-plane modes. All other modes have little or no effect on the charge migration. This information can be useful to guide the development of reduced dimensionality models for larger systems or the search for molecules with long coherence times.

Förster Blockade and Excitation Transfer Behaviors of Two-Photon Rabi Oscillations of Exciton–Biexciton Levels in Coupled Quantum Dots

We provide a theoretical study for the dynamical behavior of two-photon Rabi oscillations in two coupled quantum dots. Each dot is a three-level quantum system (ground, one-exciton, and biexciton states). We describe the optical dynamics within the density matrix formalism framework. The two-photon Rabi oscillations are found to be significantly affected by the strength of the interdot dipolar interaction. Using a detuned laser pulse with an exciton state of the driven quantum dot in our numerical simulations, a direct coherent excitation between the biexciton states can be established, but whether Rabi oscillations can be observed depend mainly on the strength of the dipolar interaction and bandwidth of the excitation laser. When the strength of the dipolar coupling is less than the excitation laser bandwidth, the time-dependent populations of the various two biexciton states of the system exhibit coherent oscillations with several frequencies. However, as we increase the dipolar coupling strength, the population transfer between the quantum dots levels amazingly becomes forbidden, and the excitation gets trapped at the initial state. The reduction of the influence of the dipolar interaction leads to a manipulation of two-photon Rabi oscillation in an ultrashort timescale (∼ps), opening possibilities to achieve ultrafast quantum state control and quantum logic gate generation.

Recent Development of Ultrafast Optical Characterizations for Quantum Materials.

The advent of intense ultrashort optical pulses spanning a frequency range from terahertz to the visible has opened a new era in the experimental investigation and manipulation of quantum materials. The generation of strong optical field in an ultrashort time scale enables the steering of quantum materials nonadiabatically, inducing novel phenomenon or creating new phases which may not have an equilibrium counterpart. Ultrafast time-resolved optical techniques have provided rich information and played an important role in characterization of the nonequilibrium and nonlinear properties of solid systems. Here, some of the recent progress of ultrafast optical techniques and their applications to the detection and manipulation of physical properties in selected quantum materials are reviewed. Specifically, the new development in the detection of the Higgs mode and photoinduced nonequilibrium response in the study of superconductors by time-resolved terahertz spectroscopy are discussed.

Inertial spin waves in ferromagnets and antiferromagnets

Inertial effects in spin dynamics are theoretically predicted to emerge at ultrashort time scales, but their experimental signatures are often ambiguous. Here, we calculate the spin-wave spectrum in ferromagnets and two-sublattice antiferromagnets in the presence of inertial effects. It is shown how precession and nutation spin waves hybridize with each other, leading to the renormalization of the frequencies, the group velocities, the effective gyromagnetic ratios and the effective damping parameters. Possible ways of distinguishing between the signatures of inertial dynamics and similar effects explainable within conventional models are discussed.

Validity of the Empatica E4 wristband to estimate resting-state heart rate variability in a lab-based context

Lab research might benefit from the advantages of wearable devices, such as their ease of use, to estimate pulse rate (PR) and pulse rate variability (PRV) as an equivalent for heart rate (HR) and heart rate variability. However, before implementing them in a lab context, the validity of the PR and PRV, also on ultra-short time scales (e.g., 30s), needs to be confirmed. We recorded heart activity simultaneously with an E4 wristband and an ECG device in a seated resting condition for 5 min. Our results showed that HR, RMSSD, SDNN and LF, but not HF, were validly estimated by the E4 wristband. Furthermore, the E4 wristband could validly estimate PR with recording lengths as short as 10s. RMSSD and SDNN were validly estimated using 30s or 120 s or an average of multiple short intervals (10s), while HF likely requires longer recording intervals. Based on this study, we formulated several recommendations for using the E4 wristband in a lab context.

Design of Mode-Locked Fibre Laser with Non-Linear Power and Spectrum Width Transfer Functions with a Power Threshold

There is a growing demand for higher computational speed and energy efficiency of machine learning approaches and, in particular, neural networks. Optical implementation of neural networks can address this challenge. Compared to other neuromorphic platforms, fibre-based technologies can unlock a wide bandwidth window and offer flexibility in dimensionality and complexity. Moreover, fibre represents a well-studied, low-cost and low-loss material, widely used for signal processing and transmission. At the same time, mode-locked fibre lasers offer flexibility and control, while the mode-locking effect can be crucial for unlocking ultra-short timescales and providing ultra-fast processing. Here, we propose a mode-locked fibre laser with a non-linear power threshold in both power and spectrum. The advantage of the proposed system is a spectrum width two-branch function dependent on the input signal power. The effect is caused by a transition between two operating regimes and is governed by the input signal power. The proposed design enables receiving a non-linear transfer function in amplitude with a power threshold as an optical analogue of biological neurons with the additional advantage of a non-linear two-branch transfer function in spectrum width. The latter property is similar to the frequency-varied response dependent on stimulus properties in biological neurons. Thus, our work opens new avenues in research into novel types of artificial neurons with a frequency spectrum width variable response and, consequently, spiking neural networks and neural-rate-based coding with potential applications in optical communications and networks with flexible bandwidth, such as 5G and emerging 6G.

Angular Momentum Transfer via Relativistic Spin-Lattice Coupling from First Principles.

The transfer and control of angular momentum is a key aspect for spintronic applications. Only recently, it was shown that it is possible to transfer angular momentum from the spin system to the lattice on ultrashort timescales. To contribute to the understanding of angular momentum transfer between spin and lattice degrees of freedom we present a scheme to calculate fully relativistic spin-lattice coupling parameters from first principles. In addition to the dipole-dipole interactions often discussed in the literature, these parameters give, in particular, access to the spin-lattice effects controlled by spin-orbit coupling. By treating changes in the spin configuration and atomic positions at the same level, closed expressions for the atomic spin-lattice coupling parameters can be derived in a coherent manner up to any order. Analyzing the properties of these parameters, in particular their dependence on spin-orbit coupling, we find that even in bcc Fe the leading term for the angular momentum exchange between the spin system and the lattice is a Dzyaloshiskii-Moriya-type interaction, which is due to the symmetry breaking distortion of the lattice.

Heat Transport on Ultrashort Time and Space Scales in Nanosized Systems: Diffusive or Wave-like?

The non-Fourier effects, such as wave-like temperature propagation and boundary temperature jumps, arise in nanosized systems due to the multiple time and space scales nature of out-of-equilibrium heat transport. The relaxation to equilibrium occurs in successive time and space scales due to couplings between different excitations, whose relaxation times have different physical meanings and may differ significantly in magnitude. The out-of-equilibrium temperature evolution is described by a hierarchy of partial differential equations of a higher order, which includes both the diffusive and wave modes of heat transport. The critical conditions of transition from wave to diffusive modes are identified. We demonstrate that the answer to the question concerning which of these modes would be detected by experimental measurements may also depend on the accuracy of the experimental setup. Comparisons between the proposed approach and other non-Fourier models, such as the Guyer–Krumhansl and Jeffreys type, are carried out. The results presented here are expected to be useful for the theoretical and experimental treatment of non-Fourier effects and particularly heat wave phenomena in complex nanosized systems and metamaterials.

Determination of sub-ps lattice dynamics in FeRh thin films

Understanding the ultrashort time scale structural dynamics of the FeRh metamagnetic phase transition is a key element in developing a complete explanation of the mechanism driving the evolution from an antiferromagnetic to ferromagnetic state. Using an X-ray free electron laser we determine, with sub-ps time resolution, the time evolution of the (–101) lattice diffraction peak following excitation using a 35 fs laser pulse. The dynamics at higher laser fluence indicates the existence of a transient lattice state distinct from the high temperature ferromagnetic phase. By extracting the lattice temperature and comparing it with values obtained in a quasi-static diffraction measurement, we estimate the electron–phonon coupling in FeRh thin films as a function of laser excitation fluence. A model is presented which demonstrates that the transient state is paramagnetic and can be reached by a subset of the phonon bands. A complete description of the FeRh structural dynamics requires consideration of coupling strength variation across the phonon frequencies.

Production of high fluence laser beams using ion wave plasma optics

Optical components for laser beams with high peak and averaged powers are being developed worldwide using stimulated plasma scattering that occurs when plasmas interact with intense, coherent light. After decades of pursuit of pulse compressors, mirrors, and other plasma based components that can be created by stimulated scattering from electron density perturbations forming on ultra-short time scales (e.g., via Stimulated Raman Scattering), more recent work has produced optical components on longer time scales allowing ion motion as well [via Stimulated Brillouin Scattering (SBS)]. In the most recent work, ion wave plasma optics have had success in producing pulses of focusable coherent light with high energy and fluence by operating on ns time scales and now promise to enable numerous applications. Experiments have further shown that in some parameter regimes, even simple plasma response models can describe the output of such optics with sufficient accuracy that they can be used as engineering tools to design plasma optics for future applications, as is already being done to control power deposition in fusion targets. In addition, the development of more sophisticated models promises to enable still higher performance from SBS driven plasma optical components under a wider range of conditions. The present status and most promising directions for future development of ion wave plasma optic techniques are discussed here.

Ultrafast time-evolution of chiral N\xe9el magnetic domain walls probed by circular dichroism in x-ray resonant magnetic scattering

Non-collinear spin textures in ferromagnetic ultrathin films are attracting a renewed interest fueled by possible fine engineering of several magnetic interactions, notably the interfacial Dzyaloshinskii-Moriya interaction. This allows for the stabilization of complex chiral spin textures such as chiral magnetic domain walls (DWs), spin spirals, and magnetic skyrmions among others. We report here on the behavior of chiral DWs at ultrashort timescale after optical pumping in perpendicularly magnetized asymmetric multilayers. The magnetization dynamics is probed using time-resolved circular dichroism in x-ray resonant magnetic scattering (CD-XRMS). We observe a picosecond transient reduction of the CD-XRMS, which is attributed to the spin current-induced coherent and incoherent torques within the continuously varying spin texture of the DWs. We argue that a specific demagnetization of the inner structure of the DW induces a flow of spins from the interior of the neighboring magnetic domains. We identify this time-varying change of the DW texture shortly after the laser pulse as a distortion of the homochiral Néel shape toward a transient mixed Bloch-Néel-Bloch texture along a direction transverse to the DW.

Element-selective ultrafast magnetization dynamics of hybrid Stoner-Heisenberg magnets

Stoner and Heisenberg excitations in magnetic materials are inherently different. The first involves an effective reduction of the exchange splitting, whereas the second comprises excitation of spin waves. In this work, we test the impact of these two excitations in the hybrid Stoner-Heisenberg system of FePd. We present a microscopic picture of ultrafast demagnetization dynamics in this alloy, which represents both components of strong local exchange splitting in Fe and induced polarization in Pd. We identify the spin-orbit coupling (SOC) and the optical intersite spin transfer (OISTR) as the two dominant factors for demagnetization at ultrashort timescales. Remarkably, the drastic difference in the origin of the magnetic moment of the Fe and Pd species is not deciding the initial magnetization dynamics in this alloy. By tuning the external laser pulse, the extrinsic OISTR can be manipulated for site-selective demagnetization on femtosecond timescales providing the fastest way for optical and selective control of the magnetization dynamics in alloys. Saliently, our results signify why various experiments demonstrating OISTR might obtain conflicting results.

Broadband Nonlinear Optical Absorption Induced by Bandgap Renormalization in CVD-Grown Monolayer MoSe2.

Optical modulation on ultrashort time scales is both of central importance and an essential operation for applications in photonics and optoelectronics. Here, with a giant bandgap renormalization due to a high density of carrier injected by a femtosecond pulse, we realize an expected broadband saturable absorption in chemical vapor deposition grown monolayer transition-metal dichalcogenide MoSe2. Our findings reveal the band edge shift from ∼1.53 to ∼0.52 eV under the pump excitation of 0.80 eV, which is induced by the nonequilibrium occupation of electron-hole states after a Mott transition as well as the increase of carrier temperature.

A perspective on nonlinearities in coherent magnetization dynamics

The recent thrust in ultrafast magnetization dynamics aims at extending spintronic functionalities to terahertz frequencies. Deterministic manipulation of magnetization at the corresponding ultrashort timescales requires minute control not only over the magnetization itself but also the reservoirs it is interacting with. Although the various intricate couplings between spins, phonons, and electrons—all of which are susceptible to ultrashort laser pulses—lead to many (often nonlinear) coupling routes, magnetization-dynamical nonlinearities have remained largely underexplored. In this Perspective, we highlight recent advances and foresee future developments in the rapidly evolving field of nonlinear magnetization dynamics. Given the elementary character of coherent excitations, we put particular emphasis on their nonlinearities. We briefly review theoretical aspects and assess excitation mechanisms to reach the nonlinear regime of magnetic excitations in a broad class of magnetic materials, such as ferromagnets, antiferromagnets, and ferrimagnets. We present an overview of the groundbreaking experiments that showcase the unique insights provided by magnetic nonlinearities. We conclude by discussing open challenges and opportunities that underpin the potential of nonlinear magnetization dynamics for the advancement of spintronics and cavity quantum electrodynamics with spin waves at terahertz frequencies.

Trends in angle-resolved molecular photoelectron spectroscopy.

The field of angle-resolved molecular photoelectron spectroscopy is reviewed, with emphasis on foundations and most recent applications in different regimes of light-matter interaction. The basic formalism underlying one-photon electron angular distributions is presented, from the primary molecular frame (MF) photoemission i.e. emission from fully oriented molecules to laboratory frame (LF) observables produced from randomly oriented targets, extensions to multiphoton and strong field processes being briefly described, followed by a survey of current quantum mechanical computational approaches. The description of experimental developments is focused on the advancements in two major instrumentation fields for angle-resolved PES of molecules in the last two decades, namely charged-particle imaging spectrometers and adiabatically or impulsively laser-induced molecular alignment, together with their interplay with the remarkable characteristics achieved nowadays by the ionizing light sources and the challenging control of complex molecules in the gas phase. Aspects and applications of LF angular observables from unoriented targets are presented, with contemporary applications, especially as probes of the target electronic structure, including higher angular observables, in particular photoelectron circular dichroism (PECD) from chiral molecules, which is confirmed as a powerful chiral technique, and higher terms arising from multiphoton or non-dipole terms. Molecular frame photoelectron angular distributions (MFPADs), which stand out as the most complete observables of molecular photoionization stereodynamics in different excitation regimes, now broadly extended to characterize molecular structure and dynamics, are then discussed stemming from fully oriented molecules tackled by electron-ion momentum coincidence techniques, or from laser aligned samples. Finally, novel developments and challenging perspectives, notably the implementation of PAD in time-resolved schemes at ultrashort time scales, high energy, and high intensity regimes are drawn.

Nonequilibrium dynamics of α-RuCl3 - a time-resolved magneto-optical spectroscopy study.

We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate α-RuCl3 to investigate the nonequilibrium dynamics of its antiferromagnetically ordered zigzag groundstate after photoexcitation. A systematic study of the transient magnetic linear dichroism under different experimental conditions (temperature, external magnetic field, photoexcitation density) gives direct access to the dynamical interplay of charge excitations with the zigzag ordered state on ultrashort time scales. We observe a rather slow initial demagnetization (few to 10s of ps) followed by a long-lived non-thermal antiferromagnetic spin-disordered state (100-1000s of ps), which can be understood in terms of holons and doublons disordering the antiferromagnetic background after photoexcitation. Varying temperature and fluence in the presence of an external magnetic field reveals two distinct photoinduced dynamics associated with the zigzag and quantum paramagnetic disordered phases. The photo-induced non-thermal spin-disordered state shows universal compressed-exponential recovery dynamics related to the growth and propagation of zigzag domains on nanosecond time scales, which is interpreted within the framework of the Fatuzzo-Labrune model for magnetization reversal. The study of nonequilibrium states in strongly correlated materials is a relatively unexplored topic, but our results are expected to be extendable to a large class of Mott-Hubbard insulator materials with strong spin-orbit coupling.