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We present a concept for selective excitation of magnetostatic surface waves with a quasi-discrete spectrum using spatially patterned femtosecond laser pulses inducing either an ultrafast change of magnetic anisotropy or an inverse Faraday effect. We micromagnetically simulate the excitation of the waves with a periodically patterned uni- or bipolar laser impact. Such excitation yields multiple wavepackets propagating with different group velocities, whose dispersion corresponds to the set of quasi-discrete points. In addition, we show that the frequency of the spectral peaks can be controlled by the polarity of the periodic impact and its spatial period. The presented consideration of multiple spatially periodic magnetostatic surface wave sources as a whole enables implementation of a comprehensive toolkit of spatiotemporal optical methods for tunable excitation and control of spin-wave parameters. [ABSTRACT FROM AUTHOR]

One of the main methods for obtaining information about the generation of sound pulses in metals is to measure the reflection coefficient of a probe wave. Various theoretical models are used to interpret the results of measuring the contribution to reflection coefficient Δ R (t) due to sound-generated displacements of lattice atoms. The purpose of this paper is to establish the degree of accuracy of models used in the case of sound generation in thin films exposed to a femtosecond pulse. It is shown below that the assumption of uniform heating used for thin films is justified if the film thickness is less than the film heating depth and for thicker films at times greater than the film heating time over the entire thickness. For optically thick films, a relatively simple expression for the field can be used. If the film thickness is less than the skin layer depth of the pump field, then it is necessary to consider the field reflection from a substrate. In this case, depending on the optical properties of the metal and the substrate, taking into account reflection can lead to either an increase or a decrease in Δ R (t). It has been established that if the skin layer at the frequency of probe radiation is less than the film heating depth, then taking into account temperature gradients in the equation for the displacement of lattice atoms leads to small changes in Δ R (t). This makes it possible to significantly simplify calculations of the displacement of lattice atoms. [ABSTRACT FROM AUTHOR]

The use of semiconductor nanocrystals in scalable quantum technologies requires characterization of the exciton coherence dynamics in an ensemble of electronically isolated crystals in which system–bath interactions are nevertheless strong. In this communication, we identify signatures of Fano-like interference between excitons and photocarriers in the coherent two-dimensional photoluminescence excitation spectral lineshapes of mixed lead-halide perovskite nanocrystals in dilute solution. Specifically, by tuning the femtosecond-pulse spectrum, we show such interference in an intermediate coupling regime, which is evident in the coherent lineshape when simultaneously exciting the exciton and the free-carrier band at higher energy. We conclude that this interference is an intrinsic effect that will be consequential in the quantum dynamics of the system and will thus dictate decoherence dynamics, with consequences in their application in quantum technologies. [ABSTRACT FROM AUTHOR]

Ultrafast laser technology presents the unique capacity to process glass materials with an outstanding processing quality; however, combining high quality and high throughput is still a crucial issue because glass is brittle and highly heat sensitive. One strategy to overcome this limitation is to split in space the main laser beam into multiple beams for process parallelization. In the present paper, the simultaneous interaction of several femtosecond laser beams at the surface of fused silica targets is addressed experimentally and theoretically. This work is devoted to highlight the beams cooperation for inducing stress in the material. The experiment consists in irradiating the target with multiple laser pulses with a wavelength of 1030 nm and a duration of 500 fs. The induced stress is observed through post-mortem cross-polarized microscopy. A multiscale and multiphysics model describing laser energy deposition into the material and its mechanical response is developed. The influence of various laser parameters is studied: number and position of laser beams, repetition rate, and fluence. Both experimental and modeling results, which are in a good agreement, show significant cooperative effects for stress formation with large enough laser energy deposition, possibly leading to detrimental cracks. [ABSTRACT FROM AUTHOR]

When used as pump pulses in transient absorption spectroscopy measurements, femtosecond laser pulses can produce oscillatory signals known as quantum beats. The quantum beats arise from coherent superpositions of the states of the sample and are best studied in the Fourier domain using Femtosecond Coherence Spectroscopy (FCS), which consists of one-dimensional amplitude and phase plots of a specified oscillation frequency as a function of the detection frequency. Prior works have shown ubiquitous amplitude nodes and π phase shifts in FCS from excited-state vibrational wavepackets in monomer samples. However, the FCS arising from vibronic-exciton states in molecular aggregates have not been studied theoretically. Here, we use a model of vibronic-exciton states in molecular dimers based on displaced harmonic oscillators to simulate FCS for dimers in two important cases. Simulations reveal distinct spectral signatures of excited-state vibronic-exciton coherences in molecular dimers that may be used to distinguish them from monomer vibrational coherences. A salient result is that, for certain relative orientations of the transition dipoles, the key resonance condition between the electronic coupling and the frequency of the vibrational mode may yield strong enhancement of the quantum-beat amplitude and, perhaps, also cause a significant decrease of the oscillation frequency to a value far lower than the vibrational frequency. Future studies using these results will lead to new insights into the excited-state coherences generated in photosynthetic pigment–protein complexes. [ABSTRACT FROM AUTHOR]

Electro-optic sampling of terahertz waves by noncollinearly propagating femtosecond laser pulses in electro-optic crystals can provide high efficiency and high spectral resolution of terahertz detection with various types of crystals and laser wavelengths, unlike the conventional collinear scheme. We develop an analytical theory of noncollinear electro-optic sampling detection technique that describes the modulation of the probe laser beam polarization as a result of nonlinear interaction between the optical and terahertz fields. The theory accounts for finite widths of the terahertz and probe beams. It is found that noncollinear scheme operates as a low-pass terahertz filter with the frequency cut-off determined by the width of the probe beam and the crossing angle of the terahertz and probe beams. We apply the theory to two practical situations: sampling of terahertz waves by fiber laser pulses (1.55 μ m wavelength) in a GaAs crystal and sampling by Ti:sapphire laser pulses (800 nm wavelength) in a LiNbO 3 crystal. [ABSTRACT FROM AUTHOR]

Interaction of intense ultrashort laser pulse with gases generates a transient spatiotemporal electron density distribution via field ionization, which may lead to the spatiotemporal reshaping of the pulse, viz., its beam profile, pulse width, etc. Here, we present an experimental study on ultrashort laser pulse interaction with argon gas sheath in an ionization saturation intensity regime (∼1015–1017 W/cm2). The present investigation has been performed using a 6 mJ, 1 kHz, and 55−60 fs Ti:Sapphire laser pulse interaction with a ∼2.5 mm long argon sheath. After the laser gas interaction, the laser spatial profile exhibits a multi-ring structure around a central maximum spot. Laser gas interaction parameters, such as laser intensity, gas pressure, etc., affect the ring pattern significantly. Under optimum parameter conditions, the laser pulse has two rings in spatial profile, and the pulse width of the central spot is self-compressed to ∼35 fs. A theoretical calculation reveals that the laser beam's spatiotemporal profile evolves as it propagates inside the gas sheath. The calculation also demonstrates that the gas ionization profile plays a crucial role in the spatiotemporal reshaping and self-compression of the laser beam. The calculation also shows that the generation of concentric ring patterns in the spatial profile is mainly due to the ionization of argon atoms into Ar+, Ar2+, and Ar3+ species in the interaction region. Such self-compressed laser pulses with concentric ring beam profiles may be useful for high-harmonic generation and shorter attosecond pulse trains. [ABSTRACT FROM AUTHOR]

Alkali trimers, Ak3, located on the surface of He nanodroplets are triply ionized following multiphoton absorption from an intense femtosecond laser pulse, leading to fragmentation into three correlated Ak+ ions. Combining the information from threefold covariance analysis of the emission direction of the fragment ions and their kinetic energy distributions P(Ekin), we find that Na3, K3, and Rb3 have an equilateral triangular structure, corresponding to that of the lowest lying quartet state A 2 ′ 4 , and determine the equilibrium bond distance Req(Na3) = 4.65 ± 0.15 Å, Req(K3) = 5.03 ± 0.18 Å, and Req(Rb3) = 5.45 ± 0.22 Å. For K3 and Rb3, these values agree well with existing theoretical calculations, while for Na3, the value is 0.2–0.3 Å larger than the existing theoretical results. The discrepancy is ascribed to a minor internuclear motion of Na3 during the ionization process. In addition, we determine the distribution of internuclear distances P(R) under the assumption of fixed bond angles. The results are compared to the square of the internuclear wave function |Ψ(R)|2. [ABSTRACT FROM AUTHOR]

In this study, the hydrodynamic expansion and splitting effect of ultrafast laser-induced plasma plume for multi-element alloys were studied. A fully coupled hydrodynamic model for femtosecond laser ablation of multi-element alloys was presented to study the ambipolar electric field during the plume expansion process. The model utilized a level-set equation to capture the interface between the condensed phase and the gaseous phase and accounted for the reaction between different species. A time-gate direct fluorescence measurement was conducted for the target material of brass, a Cu–Zn alloy, to validate the simulation results. The simulation results showed good agreement with the experimental results and were able to predict the plume-splitting effect. The ambipolar electric field induced by charged particle distribution difference was studied in detail. It was found that the ambipolar electric field was the dominant cause for the acceleration of ions, which yielded plume splitting during the expansion process. The fully coupled HD model was further used to explore the effect of the beam spot size, laser fluence, and the pulse width on plasma plume splitting. [ABSTRACT FROM AUTHOR]

This paper presents a self-consistent multi-dimensional mathematical model and a numerical approach for simulating the low-temperature plasma induced by the femtosecond laser filament. Addressing limitations in current models, we analyze key aspects of the laser plasma behavior, including plasma generation, detailed chemical kinetics, energy exchange channels, total energy balance, and hydrodynamics. The developed model and LOTASFOAM code are applied to study the temporal and spatial decay of the plasma produced by a femtosecond laser pulse in pure nitrogen at atmospheric pressure. The paper also includes a discussion on the spatial and temporal dynamics of electronically excited states of nitrogen in the decaying laser plasma. [ABSTRACT FROM AUTHOR]

The potential of KD 2 PO 4 (or DKDP) crystal as a terahertz generator is demonstrated, despite its extremely strong terahertz absorption. By combining the Cherenkov radiation scheme and surface-emitting geometry, femtosecond Ti:sapphire laser pulses of ∼ 200 − 300 μ J energy were converted to broadband (∼ 4 THz bandwidth) terahertz transients with the efficiency of ∼ 8 × 10 − 6 . The transients produced electro-optic signals of a ∼ 0.15 modulation depth and ∼ 10 3 dynamic range in a 1-mm thick ZnTe detector crystal. This suggests DKDP as a potential generator crystal for terahertz time-domain spectroscopy. From our measurements, we estimated the nonlinear coefficient d 36 ≈ 3 pm/V of DKDP for optical rectification, which is an order of magnitude larger than the value known from second-harmonic-generation experiments. At the same time, the obtained value of d 36 is an order of magnitude smaller than the value calculated from the clamped electro-optic coefficient r 63 for the MHz frequency range. At high pump intensities, we observed multiple filamentation of the pump beam and white light generation, spatially separated from terahertz generation. [ABSTRACT FROM AUTHOR]

Ultrafast optically excited ferromagnetic (FM)/nonmagnetic (NM) multilayer heterostructures have been demonstrated recently as efficient, high-power, and broadband sources of terahertz (THz) electromagnetic radiation. Since these spintronic THz emitters exploit the conversion from ultrafast spin to charge current, either in bulk or at the interface, the THz pulses inhere all the characteristics of the involved mechanisms and dynamics associated with spin-charge interconversion processes. Deconvolving the same requires meticulous and careful experimentation and analysis. In this article, we review the current state-of-the-art in this field and provide a perspective on the emerging phenomena, which are prospering as new research avenues and demonstrate application potential for futuristic THz technologies. In the process of developing efficient spintronic THz emitters by optimizing various conditions including those with material parameters and excitation light, it turns out that THz emission spectroscopy itself can be a unique experimental tool for probing microscopic dynamical magnetic and spintronic effects, induced by femtosecond laser pulse excitation, in a noncontact and noninvasive manner. Several breakthroughs can be listed from the literature in this regard from the last decade. Just recently, ultrafast orbitronics is another dimension that is taking shape and will impact the field immensely. A fair account to this topic is also presented in the article. [ABSTRACT FROM AUTHOR]

Ultrafast spectroscopy is a powerful technique that utilizes short pulses on the femtosecond time scale to generate and probe coherent responses in molecular systems. While the specific ultrafast methodologies vary, the most common data analysis tools rely on discrete Fourier transformation for recovering coherences that report on electronic or vibrational states and multi-exponential fitting for probing population dynamics, such as excited-state relaxation. These analysis tools are widely used due to their perceived reliability in estimating frequencies and decay rates. Here, we demonstrate that such "black box" methods for parameter estimation often lead to inaccurate results even in the absence of noise. To address this issue, we propose an alternative approach based on Bayes probability theory that simultaneously accounts for both population and coherence contributions to the signal. This Bayesian inference method offers accurate parameter estimations across a broad range of experimental conditions, including scenarios with high noise and data truncation. In contrast to traditional methods, Bayesian inference incorporates prior information about the measured signal and noise, leading to improved accuracy. Moreover, it provides estimator error bounds, enabling a systematic statistical framework for interpreting confidence in the results. By employing Bayesian inference, all parameters of a realistic model system may be accurately recovered, even in extremely challenging scenarios where Fourier and multi-exponential fitting methods fail. This approach offers a more reliable and comprehensive analysis tool for time-resolved coherent spectroscopy, enhancing our understanding of molecular systems and enabling a better interpretation of experimental data. [ABSTRACT FROM AUTHOR]

We report on the observation of a nonlinear intensity dependence of the terahertz radiation-induced ratchet effects in bilayer graphene with asymmetric dual-grating gate lateral lattices. These nonlinear ratchet currents are studied in structures of two designs with dual-grating gates fabricated on top of boron nitride encapsulated bilayer graphene and beneath it. The strength and sign of the photocurrent can be controllably varied by changing the bias voltages applied to individual dual-grating subgates and the back gate. The current consists of contributions insensitive to the radiation's polarization state, defined by the orientation of the radiation electric field vector with respect to the dual-grating gate metal stripes, and the circular ratchet sensitive to the radiation helicity. We show that intense terahertz radiation results in a nonlinear intensity dependence caused by electron gas heating. At room temperature, the ratchet current saturates at high intensities of the order of hundreds to several hundreds of kW cm − 2 . At T = 4 K, the nonlinearity manifests itself at intensities that are one or two orders of magnitude lower; moreover, the photoresponse exhibits a complex dependence on the intensity, including a saturation and even a change of sign with increasing intensity. This complexity is attributed to the interplay of the Seebeck ratchet and the dynamic carrier-density redistribution, which feature different intensity dependencies and nonlinear behavior of the sample's conductivity induced by electron gas heating. The latter is demonstrated by studying the THz photoconductivity. Our study demonstrates that graphene-based asymmetric dual-grating gate devices can be used as terahertz detectors at room temperature over a wide dynamic range, spanning many orders of magnitude of terahertz radiation power. Therefore, their integration together with current-driven read-out electronics is attractive for the operation with high-power pulsed sources. [ABSTRACT FROM AUTHOR]

Femtosecond laser excitation of crystal materials can produce coherent longitudinal acoustic phonons (CLAPs), which possess the capability to interact with various quasiparticles and influence their dynamics. The manipulation of CLAPs' behavior is thus of significant interest for potential applications, particularly in achieving ultrafast modulations of material properties. In this study, we present our findings on the propagation of laser-induced CLAPs at thin-film interfaces and heterojunctions using ultrafast optical reflectivity and ultrafast x-ray diffraction measurements. We observe that CLAPs can efficiently propagate from a LaMnO3 thin-film to its SrTi O 3 substrate due to the matching of their acoustic impedance, and the oscillation period increases from 54 to 105 GHz. In contrast, in ultrafast x-ray diffraction experiments, we discover that CLAPs are partially confined within an Au (111) thin film due to the mismatch of acoustic impedance with the substrates, leading to an oscillation period of 122 ps. However, interestingly, when examining L a 0.7 C a 0.175 S r 0.125 Mn O 3 / B a 0.5 S r 0.5 Ti O 3 bilayers, no oscillations are observed due to the favorable impedance matching between the layers. Our findings demonstrate that acoustic impedance can serve as an effective means to control coherent phonons in nanometer-thin films and may also play a crucial role in phonon engineering at interfaces or heterostructures. [ABSTRACT FROM AUTHOR]

Multiphoton ionization (MPI) of alkyl iodides (RI, R = CnH2n+1, n = 1–4) has been investigated with femtosecond laser pulses centered at 800 and 400 nm along with photoelectron imaging detection. In addition, the ultraviolet (UV)–vacuum ultraviolet (VUV) absorption spectra of gas-phase RIs have been measured in the photon energy range of 5–11 eV using the VUV Fourier transform spectrometer at the VUV DESIRS beamline of the synchrotron SOLEIL facility. The use of high-laser-field strengths in matter–radiation interaction generates highly non-linear phenomena, such as the Stark shift effect, which distorts the potential energy surfaces of molecules by varying both the energy of electronic and rovibrational states and their ionization energies. The Stark shift can then generate resonances between intermediate states and an integer number of laser photons of a given wavelength, which are commonly known as Freeman resonances. Here, we study how the molecular structure of linear and branched alkyl iodides affects the UV–VUV absorption spectrum, the MPI process, and the generation of Freeman resonances. The obtained results reveal a dominant resonance in the experiments at 800 nm, which counter-intuitively appears at the same photoelectron kinetic energy in the whole alkyl iodide series. The ionization pathways of this resonance strongly involve the 6p(2E3/2) Rydberg state with different degrees of vibrational excitation, revealing an energy compensation effect as the R-chain complexity increases. [ABSTRACT FROM AUTHOR]

We investigate the electron emission from 3D chiral silver alloy nanohelices initiated by femtosecond laser pulses with a central photon energy of hν = 1.65 eV, well below the work function of the material. We find hot but thermally distributed electron spectra and a strong anisotropy in the electron yield with left- and right-circularly polarized light excitations, which invert in sign between left- and right-handed helices. We analyze the kinetic energy distribution and discuss the role of effective temperatures. Measurements of the reflectance and simulations of the absorbance of the helices based on retarded field calculations are compared to the anisotropy in photoemission. We find a significant enhancement of the anisotropy in the electron emission in comparison to the optical absorption. Neither simple thermionic nor a multiphoton photoemission can explain the experimentally observed asymmetries. Single photon deep-UV photoemission from these helices together with a change of the work function suggests a contribution of the chirally induced spin selectivity effect to the observed asymmetries. [ABSTRACT FROM AUTHOR]

This paper is concerned with a theoretical analysis of the behavior of optically excited spin currents in bilayer and multilayer systems of ferromagnetic and normal metals. As the propagation, control, and manipulation of the spin currents created in ferromagnets by femtosecond optical pulses is of particular interest, we examine the influence of different thicknesses of the constituent layers for the case of electrons excited several electronvolts above the Fermi level. Using a Monte-Carlo simulation framework for such highly excited electrons, we first examine the spatiotemporal characteristics of the spin current density driven in a Fe layer, where the absorption profile of the light pulse plays an important role. Further, we examine how the combination of light absorption profile, spin-dependent transmission probabilities, and iron layer thickness affects spin current density in a Fe/Au bilayer system. For high-energy electrons studied here, the interface and secondary electron generation have a small influence on spin transport in the bilayer system. However, we find that spin injection from one layer to another is most effective within a certain range of iron layer thicknesses. [ABSTRACT FROM AUTHOR]

Ultra-intense lasers that ionize atoms and accelerate electrons in solids to near the speed of light can lead to kinetic instabilities that alter the laser absorption and subsequent electron transport, isochoric heating, and ion acceleration. These instabilities can be difficult to characterize, but X-ray scattering at keV photon energies allows for their visualization with femtosecond temporal resolution on the few nanometer mesoscale. Here, we perform such experiment on laser-driven flat silicon membranes that shows the development of structure with a dominant scale of 60 nm in the plane of the laser axis and laser polarization, and 95 nm in the vertical direction with a growth rate faster than 0.1 fs−1. Combining the XFEL experiments with simulations provides a complete picture of the structural evolution of ultra-fast laser-induced plasma density development, indicating the excitation of plasmons and a filamentation instability. Particle-in-cell simulations confirm that these signals are due to an oblique two-stream filamentation instability. These findings provide new insight into ultra-fast instability and heating processes in solids under extreme conditions at the nanometer level with possible implications for laser particle acceleration, inertial confinement fusion, and laboratory astrophysics. Ultrafast relativistic plasma instabilities accompany and influence laser matter interactions that accelerate particlebeams with potential applications in e.g radiotherapy or fussion fast ignition scenarios. Here, the authors use Small Angle X-ray Scattering to observe such instabilities on a femtosecond, tens of nanometer scale in solids, and draw conclusions on the underlying plasma dynamics. [ABSTRACT FROM AUTHOR]

The measurement of the spatial distribution of the nearly monocyclic terahertz (THz) fields by a raster scanning diaphragm is the widely used approach in THz pulse time-domain holography (PTDH) applied in imaging, optical component design, and wavefront sensing tasks. However, it is historically plagued by a compromise between the balance between the signal-to-noise ratio (SNR) and resolution. To address this challenge and keep both parameters at a high level, we proposed to replace the scanning aperture with the scanning module containing a conjugated diaphragm and lens. This solution allowed us for the first time to experimentally investigate the spatio-temporal dynamics of a Gauss–Bessel beam generated in a widespread low-energy THz system based on a femtosecond laser with a pulse energy of around a dozen nanojoules and a repetition rate of tens of megahertz. In particular, this allowed us to observe the temporal spectrum of the THz Gauss–Bessel field at the beam periphery with SNR ≈ 0.5 , which was not possible using a conventional raster scanning system. A careful numerical analysis of the proposed solution reveals a signal enhancement in the spectral domain of approximately 2.5 times compared to the THz PTDH raster scan detection employing only a diaphragm. Moreover, we have shown that the given solution ensures the temporal profiles remain unaffected by the quadratic phase aberration experienced in conventional raster field scanning with only a single aperture. [ABSTRACT FROM AUTHOR]

Compared to mode‐locked oscillators, gain‐switched diodes (GSD) have the key advantage of repetition‐rate agility. Yet, large pulse duration and poor coherence of the GSD pulses greatly limit their applications. Here, a GSD‐pumped Raman fiber amplifier is demonstrated, which can effectively generate femtosecond laser pulses with both repetition‐rate and wavelength agility. It is proved that both nonlinear optical gain and single‐frequency seed in the fiber amplifier play critical roles for improving the coherence of the generated laser pulses. In the experimental demonstration, pumped by 1065 nm GSD pulses, the nonlinear fiber amplifier can generate highly coherent 1121 nm femtosecond Raman pulses with up to 80.2% conversion efficiency. The Raman pulses can maintain high performance within the repetition‐rate tuning range from 1 to 150 MHz. The potential for generating 1178 nm femtosecond Raman pulses is also demonstrated with an optical conversion efficiency of 63.8%. This all‐fiber based femtosecond laser with both repetition‐rate and wavelength agility is a promising light source for applications such as nonlinear microscopy and micromachining. [ABSTRACT FROM AUTHOR]

Creating heterojunctions or composites by incorporating noble metals offers a remarkable means to modulate the electronic charge transfer and the nonlinear optical (NLO) properties in 2D transition metal dichalcogenides (TMDCs). The response of such 2D‐TMDC‐noble metal composites to femtosecond (fs) infrared (IR) and terahertz (THz) radiation, however, remains vastly unexplored. While the linear optical characteristics of a prototypical 2D‐TMDC, namely, MoSe2 nanosheets incorporated with noble metal (such as Au, Pt, and Ag) nanoparticles in the UV–Vis and the THz spectral range, the NLO characteristics are measured using a 70‐fs pulse at 800 nm excitation is investigated. The results demonstrate a clear reduction of band gap with the incorporation of noble metals in MoSe2, indicating an effective charge transfer mechanism at play. Notably, the MoSe2‐noble metal nanocomposites depicted a significant enhancement in the THz conductivities. In addition, a dramatic 4‐fold enhancement in the third‐order nonlinear coefficient and ≈2‐fold enhancement in the third‐order NLO susceptibility is achieved in MoSe2‐Ag nanocomposite. These results univocally suggest that the noble metal‐based composites with suitable charge transfer channels promote enhanced carrier mobilities and tunable electron transfer dynamics, making these hybrid materials promising candidates for optoelectronic applications both at IR and THz frequencies. [ABSTRACT FROM AUTHOR]

The development of next-generation data storage devices relies on the efficient control of topological spin textures at ultrafast timescales with minimal energy consumption. Here, we theoretically investigate the switching of the magnetic skyrmion in ferrimagnetic GdFeCo utilizing the helicity-independent all-optical switching (HI-AOS) driven by femtosecond laser pulses. Our study demonstrates the switching of Néel skyrmion between the two degenerate skyrmion ground states having opposite polarity and chirality. A systematic study was done by varying the laser fluence, and we found that single-shot skyrmion switching is observed for a range of fluence values, where optically induced magnetization switching is observed. The present study proves that HI-AOS is a potential mechanism for switching magnetic skyrmion at ultrafast timescales. Our results offer significant insight into implementing optical writing skyrmion-based memory devices. [ABSTRACT FROM AUTHOR]

Femtosecond laser-induced valence state conversion (VC) in solid materials has attracted significant research attention due to its potential application in ultra-high density optical storage, boasting advantages such as ultra-high recording speed, easy reading, and high signal-to-noise ratio. However, identifying appropriate materials and technological solutions conducive to efficient single-laser-shot recording remains a pivotal challenge for practical applications. In this work, we report single femtosecond laser pulse–induced VC in BaFCl: Sm3+ nanocrystals utilizing a 4F-configuration optical imaging system comprising two-dimensional scan galvo mirrors. For the first time, we experimentally reveal the luminescence mechanisms and channels of multiphoton absorption-induced Sm2+ ions under both single and multiple 800 nm fs laser pulses. Leveraging the highly efficient single femtosecond laser pulse induced VC, we demonstrate a prototype optical storage experiment by sweeping the recording laser pulse. Remarkably, a threshold pulse energy as low as ∼100 nJ for effective single-laser-shot recording in BaFCl: Sm3+ nanocrystals is obtained under the current experimental conditions. Our investigations offer profound insights into the physical mechanisms underlying femtosecond laser induced VC in solid materials, thereby promoting the prospects of VC based optical storage toward practical applications. [ABSTRACT FROM AUTHOR]

In partial onset epilepsy, seizures arise focally in the brain and often propagate. Patients frequently become refractory to medical management, leaving neurosurgery, which can cause neurologic deficits, as a primary treatment. In the cortex, focal seizures spread through horizontal connections in layers II/III, suggesting that severing these connections can block seizures while preserving function. Focal neocortical epilepsy is induced in mice, sub‐surface cuts are created surrounding the seizure focus using tightly‐focused femtosecond laser pulses, and electrophysiological recordings are acquired at multiple locations for 3–12 months. Cuts reduced seizure frequency in most animals by 87%, and only 5% of remaining seizures propagated to the distant electrodes, compared to 80% in control animals. These cuts produced a modest decrease in cortical blood flow that recovered and left a ≈20‐µm wide scar with minimal collateral damage. When placed over the motor cortex, cuts do not cause notable deficits in a skilled reaching task, suggesting they hold promise as a novel neurosurgical approach for intractable focal cortical epilepsy. [ABSTRACT FROM AUTHOR]

The broken inversion symmetry at the ferromagnet (FM)/heavy‐metal (HM) interface leads to spin‐dependent degeneracy of the energy band, forming spin‐polarized surface states. As a result, the interface serves as an effective medium for converting spin accumulation into 2D charge current through the inverse Rashba–Edelstein effect. Exploring and assessing this spin‐to‐charge conversion (SCC) phenomenon at the FM/HM interface can offer a promising avenue to surpass the presumed limits of SCC in bulk HM layers. Spintronic heterostructures are utilized as a platform to measure the SCC experienced by photoexcited spin currents. Therefore, FM/HM heterostructures emitting terahertz electric field upon illumination by femtosecond laser pulses enable quantitative measure of the ultrafast SCC process. This results demonstrate a robust interfacial spin‐to‐charge conversion (iSCC) within a synthetic antiferromagnetic heterostructure, specifically for the NiFe/Ru/NiFe configuration, by isolating the SCC contribution originating from the interface and the bulk heavy‐metal (HM). Through the measurements of the emitted terahertz pulse, the iSCC at the NiFe/Ru interface is identified to be ≈27% of the strength as compared to SCC from the highest spin‐Hall conducting heavy‐metal, Pt. The results thus highlight the significance of interfacial engineering as a promising pathway for achieving efficient ultrafast spintronic devices. [ABSTRACT FROM AUTHOR]

Femtosecond lasers have garnered widespread attention owing to their subdiffraction processing capabilities. However, their intricate natures, involving intrapulse feedbacks between transient material excitation and laser propagation, often present significant challenges for near-field ablation predictions and simulations. To address these challenges, the current study introduces an improved finite-difference time-domain method (FDTD)–plasma model (plasma)–two-temperature model (TTM) framework for simulating the ablation processes of various nanospheres on diverse substrates, particularly in scenarios wherein dynamic and heterogeneous excitations significantly influence optical-field distributions. Initially, FDTD simulations of a single Au nanosphere on a Si substrate reveal that, with transitions in the excitation states of the substrate, the field-intensity distribution transforms from a profile with a single central peak to a bimodal structure, consistent with experimental reports. Subsequently, simulations of a polystyrene nanosphere array on a SiO2 substrate reveal that different excitation states of the nanospheres yield two distinct modes, namely near-field enhancement and masking. These modes cannot be adequately modeled in the FDTD simulations. Our combined model also considers the intrapulse feedback between the electromagnetic-field distribution resulting from near-field effects and material excitations. Furthermore, the model can quantitatively analyze subsequent electron–phonon coupling and material removal processes resulting from thermal-phase transitions. Consequently, our model facilitates predictions of the femtosecond-laser ablation of single nanospheres or nanosphere arrays with varying sizes and materials placed on substrates subjected to near-field effects. [ABSTRACT FROM AUTHOR]

Although often viewed as detrimental, fluctuations carry valuable information about the physical system from which they emerge. Femtosecond noise correlation spectroscopy (FemNoC) has recently been established to probe the ultrafast fluctuation dynamics of thermally populated magnons by measurement of their amplitude autocorrelation. Subharmonic lock-in detection is the key technique in this method, allowing us to extract the pulse-to-pulse polarization fluctuations of two femtosecond optical pulse trains transmitted through a magnetic sample. Here, we present a thorough technical description of the subharmonic demodulation technique and the FemNoC measurement system. We mathematically model the data acquisition process and identify the essential parameters that critically influence the signal-to-noise ratio of the signals. Comparing the model calculations to real datasets allows validating the predicted parameter dependences and provides a means to optimize FemNoC experiments. [ABSTRACT FROM AUTHOR]

Metallic nanoparticles have gained attention in technological fields, particularly photonics. The creation of silver/gold (Ag/Au) alloy NPs upon laser exposure of an assembly of these NPs was described. First, using the Nd: YAG pulsed laser ablation's second harmonic at the same average power and exposure time, Ag and Au NPs in distilled water were created individually. Next, the assembly of Ag and Au NP colloids was exposed again to the pulsed laser, and the effects were examined at different average powers and exposure times. Furthermore, Ag/Au alloy nanoparticles were synthesized with by raising the average power and exposure time. The absorption spectrum, average size, and shape of alloy NPs were obtained by using an ultraviolet-visible (UV–Vis) spectrophotometer and transmission electron microscope instrument. Ag/Au alloy NPs have been obtained in the limit of quantum dots (<10 nm). The optical band gap energies of the Ag/Au alloy colloidal solutions were assessed for different Ag/Au alloy NP concentrations and NP sizes as a function of the exposure time and average power. The experimental data showed a trend toward an increasing bandgap with decreasing nanoparticle size. The nonlinear optical characteristics of Ag/Au NPs were evaluated and measured by the Z-scan technique using high repetition rate (80 MHz), femtosecond (100 fs), and near-infrared (NIR) (750–850 nm) laser pulses. In open aperture (OA) Z-scan measurements, Ag, Au, and Ag/AuNPs present reverse saturation absorption (RSA) behavior, indicating a positive nonlinear absorption (NLA) coefficient. In the close-aperture (CA) measurements, the nonlinear refractive (NLR) indices (n2) of the Ag, Au, and Ag/Au NP samples were ascribed to the self-defocusing effect, indicating an effective negative nonlinearity for the nanoparticles. The NLA and NLR characteristics of the Ag/Au NPs colloids were found to be influenced by the incident power and excitation wavelength. The optical limiting (OL) effects of the Ag/Au alloy solution at various excitation wavelengths were studied. The OL effect of alloy NPs is greater than that of monometallic NPs. The Ag/Au bimetallic nanoparticles were found to be more suitable for optical-limiting applications. [ABSTRACT FROM AUTHOR]

In this work, laser‐induced periodic surface structures (LIPSS) are generated on the surface of thin films of poly(trimethylene terephthalate) (PTT) fabricated by spin coating on silicon. Previous studies have shown the appearance of LIPSS in this type of materials with femtosecond laser pulses in the near‐infrared region of the spectrum, despite the extremely low absorption of the polymer. The present work consists of an exploration of the effect of adding complexity to the femtosecond laser fields employed for irradiation. Changes in the repetition rate of the pulse train, the pulse duration, and the pulse temporal chirp are explored, and conditions for optimum LIPSS formation are identified. The effects of these modifications on the polymer surface topography, assessed by atomic force microscopy, are described and discussed. [ABSTRACT FROM AUTHOR]

In this paper, the Kundu–Eckhaus equation which describes the propagation of ultrashort pulses or femtosecond light pulses in nonlinear optics is investigated using the new mapping method. As a result, different structures of chirped solitary and periodic waves were yielded. The dynamic of the soliton and kink soliton chirp waves were illustrated from which we can conclude that the sign of the Raman parameter identifies the chirp wave function direction. [ABSTRACT FROM AUTHOR]

In collisionless plasma, the function of an externally imposed static electric field has been investigated for facilitating the generation of high-power terahertz (THz) radiation. A nonlinear transient current density occurs at THz radiation frequency due to the optical rectification of high-power laser pulse having secant hyperbolic temporal intensity profile. This transient current driving a THz radiation is found to be strongly depended on the pulse width of laser, electron plasma frequency, and externally applied electric field. The effect of mismatched phase between the generated THz wave and laser has also been studied. Numerical simulations show that the strength of THz amplitude initially increases with propagation distance and then decreases. [ABSTRACT FROM AUTHOR]

Efficient laser-driven plasma acceleration of ion beams requires precision control of the target–plasma profile, which is crucial to optimize the laser energy transfer. Along the laser propagation direction, this can be achieved by tailoring the temporal structure of the laser pulse. We show for the first time that frequency-doubling of a short pulse (hundreds-femtosecond range) petawatt-class mixed-glass laser system, which results in temporal intensity contrast enhancement, enables surface and volumetric laser–energy coupling, and the acceleration of proton beams from few-nanometer-thick foil targets. Experimentally, maximum ion energies and laser-to-proton energy conversion efficiencies were found to be both maximized at optimum laser and target conditions manifested when the normalized target density nearly equalizes the normalized laser vector potential, which is in agreement with theory and simulations. These signatures are recognized as a unique indication of the interaction between ultra-intense laser pulses with high temporal intensity contrast and ultra-thin nanometer-scale targets. Transverse modulations of accelerated proton beams in the form of bubble- and ring-like structures measured in the thinnest targets provide additional evidence of volumetric laser-driven particle acceleration regimes and transitional features in ultra-thin foil targets specific to laser–plasma interactions characterized by a high temporal intensity contrast. These results open avenues in the generation of high contrast laser pulses from short-pulse-femtosecond petawatt mixed-glass laser systems and demonstrate the feasibility of this technique for applications requiring high laser intensity contrast with high efficiency. [ABSTRACT FROM AUTHOR]

Filamentation of high-power femtosecond laser pulses in air is accompanied by a fairly strong release of optical energy into the propagation medium due to laser-induced ionization of air molecules and production of an underdense plasma of charged species. We present the results of our laboratory experiments and numerical simulations aimed at estimating the energy deposition amount by laser filament upon propagation in air depending on the conditions of spatial focusing, pulse energy, and radiation wavelength. Importantly, our study reveals a more than 50% decrease in the filament energy deposited in air in the range of moderate numerical aperture values, approximately from 0.003 to 0.007, at carrier wavelengths of 740 and 470 nm. We attribute such a considerable reduction in the laser pulse energy release for femtosecond plasma to the competing effects of Kerr self-focusing and geometric divergence of focused laser pulse. [ABSTRACT FROM AUTHOR]

During the process of terahertz (THz) wave generation via femtosecond laser filamentation in air, as well as through the mixing of THz waves with externally injected plasma filaments, THz waves engage in interactions with the plasma. A characteristic feature of this interaction is the modulation of the THz radiation spectrum by the plasma, which includes the generation of THz spectral dips. This information is essential for understanding the underlying mechanisms of THz–plasma interactions or for inferring plasma parameters. However, a current debate exists on the number of THz spectral dips observed after the interaction, with different opinions of single versus multiple dips, thus leaving the interaction mechanisms still ambiguous. In this work, we retrospectively analyzed the experimental appearance of multiple dips in the THz spectrum and found that the current observations of such dips are predominantly a result of the water vapor absorption with a low spectral resolution. Additionally, we observed that altering the acquisition width of the temporal THz signal also influenced the dips' number. Hence, in future research, simultaneous attention should be paid to the following two aspects of THz–plasma interactions: (1) It is necessary to ensure a sufficiently wide time-domain window to accurately represent the spectral dip characteristics. (2) The spectral dips should be carefully distinguished from the water absorption lines before being further studied. On the other hand, for the case of a single dip in the THz spectrum, we also put forward a new viewpoint of the resonance between surface plasmon waves and THz waves, which should also be taken into consideration in future studies. [ABSTRACT FROM AUTHOR]

The dissociative ionization of CHBr2Cl molecules in femtosecond laser fields at 800 nm and 400 nm is investigated to enhance the comprehension of ultrafast dynamics phenomena. The kinetic energy distribution of the resulting ions following photo-dissociation is analyzed using time-of-flight mass spectrometry in combination with DC-sliced ion velocity map imaging. The findings from the experimental study indicate that the presence of low kinetic energy components is attributed to the dissociative ionization processes of CHBr2Cl molecules. The complexity of individual dissociation pathways remains unaffected by the laser fields but is determined by factors such as bond energy, ionization energy of neutral groups, and charge distribution. In the case of 400 nm laser fields, distinct elimination channels enable CHBr2Cl+ ions to circumvent the transition state, leading to the formation of BrCl+ and Br2+ fragments. [ABSTRACT FROM AUTHOR]

A 2D numerical model based on the finite-difference time-domain (FDTD) method had been developed to investigate the correspondence between the spatio-temporal aspects and intensity evolution of a focused laser beam after the propagation through micro-structured dispersive materials under the pulse duration variation in the few-cycle regime. In parallel with the laser field intensification investigations, a spatio-temporal analysis of the electromagnetic field in the focal point is elaborated as a function of the relative spatial extension of the pulse in order to provide a complex description of this approach. The numerical computations indicate that shorter and more intense pulses may be obtained in well-defined conditions. Also, the major contribution played by the input laser beam profile, numerical aperture, and the dispersive material features in the intensity enhancement process in the focal point is pointed out. The present approach can be used as a versatile method for field intensification in various ultra-short and ultra-intense few-cycle laser pulse experiments. [ABSTRACT FROM AUTHOR]

Presented in this study is a validated semiempirical model of the effects of femtosecond laser pulse energy on the effective z-position of the resulting cut after laser-induced optical breakdown. Different energy levels (for the same spot spacings, i.e., different doses) running from 1.07 × (~60 nJ) to 3.8 × (~215 nJ) of the laser-induced optical breakdown (LIOB) threshold (~56 nJ) were used to perform flat cuts within flat poly(methyl methacrylate) (PMMA) samples at the same nominal focus position (depth within the material). The z-locations of the effective cut and the anterior surface of the PMMA were confocally determined. The difference (PMMA_surface—Cut_plane) was used as a surrogate for the effective shift in the z-position of the cut. A consistent and continuous shift towards less deep cuts was observed for increasing pulse energies. The z-shift spreads by up to 22 µm thinner cuts for the largest pulse energy (3.8× LIOBTh, ~215 nJ). Higher pulse energies seem to significantly reduce the cutting depth. The results for PMMA are in good agreement with the moving LIOB model. [ABSTRACT FROM AUTHOR]

The study of conductive oxides has gained momentum within the photonics community due to their unique linear and nonlinear optical properties. Despite recent experiments reporting on high harmonic generation from thin films, the optical/electronic behavior of these compounds at the nanoscale is still not fully understood due to the lack of a suitable theoretical model. In the present work, aluminum zinc oxide is excited near its epsilon‐near‐zero crossing point using incident femtosecond pulses having peak power densities in the 1 TW cm−2 range. A relatively efficient frequency up‐conversion including even and odd harmonics up to the seventh order is observed. A hydrodynamic‐Maxwell theoretical approach is adopted, capable of simultaneously taking into account linear and nonlinear dispersions, nonlocal effects, surface, magnetic, and bulk nonlinearities in a spectral region that spans over two and a half octaves from the UV to the NIR region. The study enables a deeper understanding of the fundamental material parameters regulating optical nonlinearities, providing important insights to engineer this class of materials for applications in sensing, ultra‐fast physics, and spectroscopy. [ABSTRACT FROM AUTHOR]

We theoretically investigate the polarized terahertz (THz) generation in laser–gas interaction using circularly polarized (CP) two-color laser pulses with uncommon frequencies. We show that these laser pulses can be applied to generate polarized THz radiation, and the polarization of THz radiation, which ranges from linear to circular, can be controlled in a flexible manner by manipulating the laser parameters, such as the relative phase and phase angle. Furthermore, in contrast to traditional harmonic frequency combinations, the polarization states of the incommensurate lasers undergo complex evolution with the phase angle, resulting in a noteworthy influence on the THz yield. The obtained results could deepen our understanding of polarized THz radiation generation. [ABSTRACT FROM AUTHOR]

Laser-driven compact particle accelerators can provide ultrashort pulses of broadband X-rays, well suited for undertaking X-ray absorption spectroscopy measurements on a femtosecond timescale. Here the Extended X-ray Absorption Fine Structure (EXAFS) features of the K-edge of a copper sample have been observed over a 250 eV window in a single shot using a laser wakefield accelerator, providing information on both the electronic and ionic structure simultaneously. This capability will allow the investigation of ultrafast processes, and in particular, probing high-energy-density matter and physics far-from-equilibrium where the sample refresh rate is slow and shot number is limited. For example, states that replicate the tremendous pressures and temperatures of planetary bodies or the conditions inside nuclear fusion reactions. Using high-power lasers to pump these samples also has the advantage of being inherently synchronised to the laser-driven X-ray probe. A perspective on the additional strengths of a laboratory-based ultrafast X-ray absorption source is presented. Laser-driven X-rays can provide ultrashort pulses of broadband light, well suited for femtosecond timescale absorption spectroscopy. Here the authors measure the extended X-ray absorption features of a copper sample using a laser wakefield accelerator, in a single shot; important for studying samples driven to extreme and non-equilibrium states. [ABSTRACT FROM AUTHOR]

We experimentally demonstrate that terahertz emission yield from single-color filament plasma can be increased by more than 3 times by ordinary laser pulse chirping at constant energy. The enhancement is spectrally selective, for each terahertz frequency there is an optimal laser pulse duration providing maximal terahertz emission. This provides a prospective tool for tailoring both spectrum and energy of the terahertz emission from a single-color filament. [ABSTRACT FROM AUTHOR]

Spontaneous symmetry breaking (SSB) is key for our understanding of phase transitions and the spontaneous emergence of order. In this work, we report that, for a two-dimensional (2D) periodic metasurface with gain, SSB occurs in the lasing transition. We study diffractive hexagonal plasmon nanoparticle lattices, where the K-points in momentum space provide two modes that are degenerate in frequency and identically distributed in space. Using femtosecond pulses to energize the gain medium, we simultaneously capture single-shot real-space and Fourier-space images of laser emission. By combining Fourier and real space, we resolve the two order parameters for which symmetry breaking simultaneously occurs: spatial parity and U(1) (rotational) symmetry breaking, evident respectively as random relative mode amplitude and phase. The methodology reported in this work is generally applicable to 2D plasmonic and dielectric metasurfaces and opens numerous opportunities for the study of SSB and the emergence of spatial coherence in metaphotonics. [ABSTRACT FROM AUTHOR]

The generation of terahertz radiation via laser-induced plasma from two-color femtosecond pulses in air has been extensively studied due to its broad emission spectrum and significant pulse energy. However, precise control over the temporal properties of these ultra-broadband terahertz pulses, as well as the measurement of their polarization state, remain challenging. In this study, we review our latest findings on these topics and present additional results not previously reported in our earlier works. First, we investigate the impact of chirping on the fundamental wave and the effect of manipulating the phase difference between the fundamental wave and the second-harmonic wave on the properties of generated terahertz pulses. We demonstrate that we can tune the time shape of terahertz pulses, causing them to reverse polarity or become bipolar by carefully selecting the correct combination of chirp and phase. Additionally, we introduce a novel technique for polarization characterization, termed terahertz unipolar polarimetry, which utilizes a weak probe beam and avoids the systematic errors associated with traditional methods. This technique is effective for detecting polarization-structured terahertz beams and the longitudinal component of focused terahertz beams. Our findings contribute to the improved control and characterization of terahertz radiation, enhancing its application in fields such as nonlinear optics, spectroscopy, and microscopy. [ABSTRACT FROM AUTHOR]

This study introduces a compact, portable femtosecond fibre laser system designed for synchronization with SPring‐8 synchrotron X‐ray pulses in a uniform filling mode. Unlike traditional titanium–sapphire mode‐locked lasers, which are fixed installations, our system utilizes fibre laser technology to provide a practical alternative for time‐resolved spectroscopy, striking a balance between usability, portability and cost‐efficiency. Comprehensive evaluations, including pulse characterization, timing jitter and frequency stability tests revealed a centre wavelength of 1600 nm, a pulse energy of 4.5 nJ, a pulse duration of 35 fs with a timing jitter of less than 9 ps, confirming the suitability of the system for time‐resolved spectroscopic studies. This development enhances the feasibility of experiments that combine synchrotron X‐rays and laser pulses, offering significant scientific contributions by enabling more flexible and diverse research applications. [ABSTRACT FROM AUTHOR]

Understanding and controlling the structure and function of liquid interfaces is a constant challenge in biology, nanoscience and nanotechnology, with applications ranging from molecular electronics to controlled drug release. X‐ray reflectivity and grazing incidence diffraction provide invaluable probes for studying the atomic scale structure at liquid–air interfaces. The new time‐resolved laser system at the LISA liquid diffractometer situated at beamline P08 at the PETRA III synchrotron radiation source in Hamburg provides a laser pump with X‐ray probe. The femtosecond laser combined with the LISA diffractometer allows unique opportunities to investigate photo‐induced structural changes at liquid interfaces on the pico‐ and nanosecond time scales with pump–probe techniques. A time resolution of 38 ps has been achieved and verified with Bi. First experiments include laser‐induced effects on salt solutions and liquid mercury surfaces with static and varied time scales measurements showing the proof of concept for investigations at liquid surfaces. [ABSTRACT FROM AUTHOR]

Laser-induced fluorescence spectroscopy (LIFS) is actively used for remote sensing of atmospheric aerosols and is currently one of the most sensitive and selective techniques for determining small concentrations of substances inside particles. The use of high-power femtosecond laser sources for LIFS-based remote sensing of aerosols contributes to the development of new-generation fluorescence atmospheric lidars since it makes it possible to overcome the energy threshold for the nonlinear-optical effects of multiphoton absorption in particles and receive the emission signal at long distances in the atmosphere. Our study is aimed at the development and experimental demonstration of the technique of nonlinear laser-induced fluorescence spectroscopy (NLIFS) based on the remote excitation of aerosol fluorescent emission stimulated by a spatially structured high-power femtosecond laser pulse. Importantly, for the first time to our knowledge, we demonstrate the advances in using stochastically structured plasma-free intense light channels (postfilaments) specially formed by the propagation of femtosecond laser radiation through a turbulent air layer to improve NLIFS efficiency. A multiple increase in the received signal of two-photon-excited fluorescence of polydisperse-dyed aqueous aerosols by the structured postfilaments is reported. [ABSTRACT FROM AUTHOR]

Here, the concept of generating higher‐order dispersive waves (DWs) via quasi‐phase‐matching (QPM) in periodically dispersion‐modulated liquid‐core fibers are demonstrated by generating distinct narrowband sidebands generated outside the conventional supercontinuum (SC) spectrum. Through controlled partial core collapse, the commonly used phase‐matching (PM) condition is amended by an additional grating‐related term. This results in the generation of ultrashort higher‐order DWs controlled by the grating parameters, extending the conventional SC spectrum up to 3 μm$\umu {\rm m}$. Of particular interest is the excellent overlap of the QPM‐peaks obtained from experiments, simulations, and PM considerations, showing the quality of the implementation approach and allowing for controlled narrowband peaks generation even for femtosecond input pulses. In summary, this multicolor generation concept embodies a versatile photonic platform with unique dispersion control capabilities for the transfer of spectral power into selected narrowband spectral intervals. It stands out with its unique capabilities, making it well‐suited for applications in diverse fields like bioanalytics, life sciences, quantum technology, and metrology. [ABSTRACT FROM AUTHOR]

In this Letter, we investigate coherent phonon dynamics in the incommensurate LaVS3 crystal by femtosecond pump-probe spectroscopy. Two coherent phonon modes are systematically observed in the transient reflectivity, centered at 1.8 and 2.85 THz, respectively, while a third mode centered at 4.5 THz is observed only at high pump fluence. The experimental results obtained at two different polarization configurations as well as a comparison with recent theoretical results allow to assign the two main modes to the interlayer shearing mode and to an intralayer mode, respectively. Two possible assignments are discussed for the third mode, by invoking a possible emergence of nonlinear phonon processes. [ABSTRACT FROM AUTHOR]

With strong electron–phonon coupling, self‐trapped excitons (STEs) are typically formed in perovskite materials, and radiative recombination of STEs can produce broadband emission with large Stokes shifts. STEs are essential to further improve the optoelectronic properties of materials. Surprisingly, 2D system is the edge case, with low even no self‐trapping barriers, leading to effortless formation of STEs. In this work, 2D strontium titanate (SrTiO3) with defects is prepared using supercritical carbon dioxide (SC CO2) and its carrier transport and transition are studied. The appearance of wide photoinduced positive absorption signals in the femtosecond transient absorption spectra is direct evidence for the formation of STEs. The presence of STEs is further supported by the increased Stokes shift and full width at half maximum in the steady‐state photoluminescence spectra. [ABSTRACT FROM AUTHOR]