Ultrafast Research Articles

On-chip deep subwavelength optomagnetic bistable memory based on inverse Faraday effect related nonlinearity in graphene waveguide ring resonators

Integrated optical devices that possess bistable characteristics are key elements for optical digital signal processing and all-optical computing. In this paper we report on an optomagnetic bistable memory based on the inverse Faraday effect related nonlinearity in graphene waveguide ring resonators. The effective magnetic field via the plasmon-induced inverse Faraday effect in the graphene resonator has two discrete stable states that represent logic one and logic zero and magnetic switching for memory operation can be achieved by injecting an optical pulse and momentarily blocking the bias input light. Our proposed optomagnetic bistable device based on a graphene magnetoplasmonic configuration has great potential for the development of next generation magnetic memory. It has benefits of ultrafast magnetization switching, simplicity of the considered structure, on-chip compatibility, and a deep subwavelength platform. It also enhances the nonlinear interaction due to strong confinement of the graphene plasmon modes and high-quality factor of traveling modes in the graphene ring resonator, and tunability and robustness by adjusting the gate voltages of the graphene sheets. These advantages will satisfy the demand for fast magnetization switching, low-energy consumption, and high-density recording required in future magnetic memories. Published by the American Physical Society 2024

Efficient Simultaneous Second Harmonic Generation and Dispersive Wave Generation in Lithium Niobate Thin Film

AbstractLithium niobate thin film (LNTF) is a promising platform for ultra‐low loss nonlinear integrated photonics. Here, the simultaneous generation of second harmonic wave (SHW) and dispersive wave (DW) are demonstrated in a single LNTF under the pump of a femtosecond pulse laser, with a conversion efficiency exceeding 25%. The second harmonic generation (SHG) uses the modal phase matching mechanism based on the second‐order nonlinear effect, while the DW generation is based on the perturbations of soliton dynamics caused by self‐phase modulation and higher‐order dispersion. Notably, significant and symmetrical SHW and DW patterns are observed, which exhibit strong spatial dispersion properties. A comprehensive analysis of the phase‐matching conditions are conducted for SHG and DW generation and provide a clear elucidation of the spectral properties of different regions of the emitted light patterns. Additionally, the evolution of the pump light in LNTF is thoroughly investigated, and the solutions of the generalized Schrödinger equation are in good agreement with these experimental results. This work sheds new light on the rich physics of nonlinear optical interactions on LNTF, and by utilizing the synergistic effect of second‐order and third‐order nonlinear effects, this study anticipates achieving efficient and high energy on‐chip broadband frequency conversion and supercontinuum generation across octaves.

The Analysis of Electron Densities: From Basics to Emergent Applications.

The electron density determines all properties of a system of nuclei and electrons. It is both computable and observable. Its topology allows gaining insight into the mechanisms of bonding and other phenomena in a way that is complementary to and beyond that available from the molecular orbital picture and the formal oxidation state (FOS) formalism. The ability to derive mechanistic insight from electron density is also important with methods where orbitals are not available, such as orbital-free density functional theory (OF-DFT). While density topology-based analyses such as QTAIM (quantum theory of atoms-in-molecules) have been widely used, novel, vector-based techniques recently emerged such as next-generation (NG) QTAIM. Density-dependent quantities are also actively used in machine learning (ML)-based methods, in particular, for ML DFT functional development, including machine-learnt kinetic energy functionals. We review QTAIM and its recent extensions such as NG-QTAIM and localization-delocalization matrices (LDM) and their uses in the analysis of bonding, conformations, mechanisms of redox reactions excitations, as well as ultrafast phenomena. We review recent research showing that direct density analysis can circumvent certain pitfalls of the FOS formalism, in particular in the description of anionic redox, and of the widely used (spherically) projected density of states analysis. We discuss uses of density-based quantities for the construction of DFT functionals and prospects of applications of analyses of density topology to get mechanistic insight with OF-DFT and recently developed time-dependent OF-DFT.

Generalized Coherent Wave Control at Dynamic Interfaces

AbstractCoherent wave control is of key importance across a broad range of fields such as electromagnetics, photonics, and acoustics. It enables us to amplify or suppress the outgoing waves via engineering amplitudes and phases of multiple incidences. However, within a purely spatially (temporally) engineered medium, coherent wave control requires the frequency of the associated incidences to be identical (opposite). In this work, this conventional constraint is broken by generalizing coherent wave control into a spatiotemporally engineered medium is broken, i.e., the system featuring a dynamic interface. Owing to the broken translational symmetry in space and time, both the subluminal and superluminal interfaces allow interference between scattered waves regardless of their different frequencies and wavevectors. Hence, one can flexibly eliminate the backward‐ or forward‐propagating waves scattered from the dynamic interfaces by controlling the incident amplitudes and phases. The work not only presents a generalized way for reshaping arbitrary waveforms but also provides a promising paradigm to generate ultrafast pulses using low‐frequency signals. It has also implemented suppression of forward‐propagating waves in microstrip transmission lines with fast photodiode switches.

Nonlinear Optical Properties of the Topological Material Bi2Se3 Family for the Application of an Ultrafast Pulse Laser Based on the Occupied and Unoccupied Band Structures.

The Bi2Se3 family can exhibit many intriguing topological insulator properties, including a narrow bandgap and strong surface states, which show excellent nonlinear optical properties. Thinning bulk Bi2Se3 family materials to create a low-cost photoelectric modulation device and explaining the mechanisms of nonlinear optical differences in different types of materials remain challenges. Based on liquid-phase exfoliation technology and tapered fiber, this work prepared optoelectronic modulation devices for various samples within the Bi2Se3 family, quantitatively compared their nonlinear optical properties, and analyzed the sources of differentiation using the occupied and unoccupied multiband structure theory. The results correspond well to the phenomena observed in the ultrafast laser, which will provide strong support for the design of higher performance photoelectric devices based on topological insulators.

Temporal airy pulses efficiency in thin glass dicing

Abstract Ultrashort pulse laser sources are useful tools for micro- and nano-processing large band gap dielectric materials. One of the biggest advantages of these pulses is the possibility to reach high intensity peaks that promote absorption even in materials transparent to the laser wavelength. In addition, if the pulse temporal distribution is modified, energy absorption enables the ablation of small diameter holes with large depths. In this work, we present preliminary results that implement three types of pulses as precursors for glass dicing: Bandwidth-limited (30 fs at 785 nm), positively, and negatively dispersed Temporal Airy Pulses (TAP). The material of choice was 170 μm thick soda-lime glass, inscribed at 1 kHz repetition rate in tight (50× objective) and loose (20× objective) focusing conditions for different laser energies and scanning speeds. After laser processing, the glass was diced by mechanical stress, with a home built four-point bending stage. We analyzed the quality of the scribed lines at the surface and in cross-section after breaking, as well as the necessary breaking force for all three types of laser pulses. We report that positive TAP produced a neat, flat-cut edge on the glass samples compared with the other implemented pulses.

Sensors: future tools for detecting young patient's stress during a dental invasive versus a non-invasive dental treatment-a pilot study.

A reliable tool to visualise children's early stress signs to prevent dental fear development is needed. The aim was to evaluate the commercially available, CE marked, Shimmer3 GSR + unit's ability to indicate for stress as a reaction of fear or pain for a non-invasive dental treatment (NI) and an invasive dental treatment (I). Patients 14-16years old were invited to undergo an oral check-up (NI) or an orthodontic premolar extraction (I), respectively. Digital data, measured via electrodes and optical pulse probe, placed on the wrist and fingers, monitored by the Shimmer3 GSR + unit, was transferred via Bluetooth to the HP-laptop. The observed digital parameters were: heart rate based on photoplethysmography (PPG), galvanic skin response (GSR), and 3-axis gyroscope and accelerometer signals for hand movements. Protocols for patient self-report scales were used: coloured analogue scale for pain intensity, facial analogue scale for the mood, and a dental fear scale. Descriptive statistics was performed. The NI-group: 20 patients, (14.6 ± 0.5years), underwent 20 oral check-ups. The I-group: 14 patients, (15.3 ± 0.5years), underwent 28 premolar extractions. All patients tolerated the Shimmer3 GSR + unit well. The GSR signal increased significantly, at start and during the oral injection, in the I-group. The GSR amplitudes persisted throughout and post the dental injection. No general uniform pattern or high GSR amplitudes were produced regarding NI-group. Considering the limitations of this study, the following conclusions can be made: the invasive treatment resulted in a specific unison GSR pattern, while the non-invasive procedure showed individually scattered GSR reactions. The commercially available CE-marked Shimmer3 GSR + device indicated the patient's stress response triggered by the invasive anaesthetic procedure.

Discerning TGF and Leader Current Pulse in ASIM Observation

AbstractTerrestrial gamma ray flash (TGF) observations made by the Atmosphere‐Space Interaction Monitor (ASIM) have demonstrated that these TGFs are accompanied by a prominent optical pulse from a hot leader channel. It is hard to confidently resolve the true sequence of the events in the source region due to temporal proximity of the involved processes. Here we report a bright long duration TGF together with its associated optical recordings showing clear temporal separation between the TGF and the optical pulse. In this observation the optical pulse is clearly distinct and subsequent relative to the TGF. The corresponding lightning discharge occurred at the very end of the TGF. We conclude that the current surge inside the lightning leader channel cannot be responsible for generation of this TGF. The current surge that produced the associated optical pulse can itself be conditioned by the TGF and may be responsible for the TGF termination.

Comparison of the effects of laser systems and cold atmospheric plasma on the surface roughness and shear bond strength of flexible hybrid ceramics.

The aim of this study was to compare the effects of laser systems and cold atmospheric plasma (CAP) on the surface roughness (Ra) and shear bond strength (SBS) of flexible hybrid ceramics (FHCs). Eighty FHC samples were divided into 5 groups to be subjected to surface treatments (hydrofluoric acid (HFA), HFA + 5W Er: YAG laser (HFA + 5WE), HFA + 3W Er: YAG laser (HFA + 3WE), HFA + ultrafast fiber laser (HFA + FL), and CAP). The Er: YAG laser (AT Fidelis Plus III, Fotona, Slovenia) was operated with a 0.9mm diameter tip, delivering 250mJ and 150mJ per pulse, with output powers of 5W and 3W, and fluences of 23,623J/cm² and 14,157J/cm², respectively, at a frequency of 20Hz and a pulse duration of 600 µs for 30s. The FL (FiberLAST Inc., Turkey) was applied with a 7mm spot size, 1mJ pulse energy, 20W output power, 100kHz repetition rate, ultrashort pulse length (100 ns), and the fluence of 1,820J/cm² for 7s. The CAP (PiezoBrush PZ3, Relyon Plasma, Germany) applied to the surfaces for 80s at a treatment speed of 5 cm2/s and 100% plasma power. After the Ra values were measured, each group was divided into 2 subgroups to be cemented with total-etch (TE) and self-adhesive (SA) resin cements. The SBS of all the samples was measured. One sample was randomly selected from each group, and the fractured surfaces were examined by SEM analysis. The significance level was at P < 0.05. HFA + FL had the highest Ra values, and there was no significant difference between HFA + FL and HFA + 5WE (P > 0.05). There was no difference in Ra between CAP and HFA (P > 0.05). The highest SBS values were observed for the samples cemented with TE after HFA + FL. The difference between the SBS values of the groups cemented with TE after CAP, HFA + 5WE, HFA + 3WE, and HFA + FL was not significant (P < 0.05). The use of FL may be a promising method to improve SBS without causing thermal damage when using TE or SA cements. CAP can be recommended as a practical and safe treatment with SA cement because it is suitable for chairside use with a handheld device and does not change the physical properties of the material.

Optoacoustic Entanglement in a Continuous Brillouin-Active Solid State System

Entanglement in hybrid quantum systems comprised of fundamentally different degrees of freedom, such as light and mechanics, is of interest for a wide range of applications in quantum technologies. Here, we propose to engineer bipartite entanglement between traveling acoustic phonons in a Brillouin active solid state system and the accompanying light wave. The effect is achieved by applying optical pump pulses to state-of-the-art waveguides, exciting a Brillouin Stokes process. This pulsed approach, in a system operating in a regime orthogonal to standard optomechanical setups, allows for the generation of entangled photon-phonon pairs, resilient to thermal fluctuations. We propose an experimental platform where readout of the optoacoustics entanglement is done by the simultaneous detection of Stokes and anti-Stokes photons in a two-pump configuration. The proposed mechanism presents an important feature in that it does not require initial preparation of the quantum ground state of the phonon mode. Published by the American Physical Society 2024

Signature of Attochemical Quantum Interference upon Ionization and Excitation of an Electronic Wave Packet in Fluorobenzene

Ultrashort pulses can excite or ionize molecules and populate coherent electronic wave packets, inducing complex dynamics. In this Letter, we simulate the coupled electron-nuclear dynamics upon ionization to different electronic wave packets of (deuterated) benzene and fluoro-benzene molecules, quantum mechanically and in full dimensionality. In fluoro-benzene, the calculations unravel both interstate and intrastate quantum interferences that leave clear signatures of attochemistry and charge-directed dynamics in the shape of the autocorrelation function. The latter are in agreement with experimental high-harmonic spectroscopy measurements of benzenes and fluoro-benzene. Published by the American Physical Society 2024

Plasmonic gold-enhanced GaAs for femtosecond laser generation

Surface plasmon resonance (SPR) can significantly enhance the local electromagnetic fields, facilitating the interaction between light and matter at the nanoscale. However, its ultrafast photonics application in lasers remains unexplored, especially for femtosecond pulsed laser generation. In this work, we investigate the femtosecond pulse generation based on SPR-enhanced nonlinear absorption characteristics in GaAs for the first time, to the best of our knowledge. The gold nanoparticles (GNPs)+GaAs bilayer saturation absorber (SA) decorated on the tapered fiber generates a modulation depth of 2.02% and a saturable intensity of 3.13 MW/cm2. Stable mode-locked pulses can be obtained in an erbium-doped fiber cavity, as demonstrated here. The signal-to-noise ratio (SNR) of the pulses is 75 dB and the shortest pulse duration can reach 384 fs, highlighting the potential of the SPR effect in manufacturing ultrafast optical devices.

180 mW, 1 MHz, 15 fs carrier-envelope phase-stable pulse generation via polarization-optimized down-conversion from gas-filled hollow-core fiber

Gas-filled hollow core fibers allow the generation of single-cycle pulses at megahertz repetition rates. When coupled with difference frequency generation, they can be an ideal driver for generating carrier-envelope phase stable, octave-spanning pulses in the short-wavelength infrared. In this work, we investigate the dependence of the polarization state in gas-filled hollow-core fibers (HCF) on the subsequent difference frequency generation stage. We show that by adjusting the input polarization state of light in geometrically symmetric systems, such as hollow-core fibers, one can achieve precise control over the polarization state of the output pulses. This manipulation preserves the temporal characteristics of the generated ultrashort pulses, especially when operating at a near single-cycle regime. We leverage this property to boost the downconversion efficiency of the near single-cycle pulses in a type I difference frequency generation stage. Our technique overcomes the bandwidth and dispersion constraints of the previous methods that rely on broadband waveplates or adjustment of crystal axes relative to the laboratory frame. This advancement is crucial for experiments demanding pure polarization states in the eigenmodes of the laboratory frame.

On the theory of spectral compression-assisted optical temporal differentiation

Bandwidth limitation represents a significant factor that degrades the performance of optical devices. The dimensions, composition and configuration of optical devices impose intrinsic constraints on processing broadband optical pulse signals. The enhancement of the response bandwidth of optical devices represents a significant challenge. In this study, we put forward the theory of self-similar spectral compression (SSSC), which involves solving the nonlinear Schrödinger equation with variable coefficients by using the Taylor expansion and residual theorem. The spectral waveform can be precisely preserved in the process of SSSC, leading to a predictable compression factor without pedestals. To demonstrate the effectiveness of the proposed SSSC, we present a case study by designing an on-chip optical time-domain differentiator (OTD) system including a silicon-based tapered spiral waveguide. A 200-fs chirped pulse is well differentiated at multiple orders in the OTD system. Although the linear loss of spiral waveguide has a detrimental impact on SSSC, the broadband spectrum can still be self-similarly compressed, leading to a reduction of differentiation deviation of 22.5 times. The proposed SSSC theory offers valuable guidance for designing all-optical signal processing systems with high spectral resolution and low signal error.

Selective Ablation and Laser-Induced Periodical Surface Structures (LIPSS) Produced on (Ni/Ti) Nano Layer Thin Film with Ultra-Short Laser Pulses

The interaction of ultra-short laser pulses (USLP) with Nickel/Titanium (Ni/Ti) thin film has been presented. The nano layer thin film (NLTF), composed of ten alternating Ni and Ti layers, was deposited on silicon (Si) substrate by ion-sputtering. A single and multi-pulse irradiation was performed in air with focused and linearly polarized laser pulses. For achieving selective ablation of one or more surface layers, without reaching the Si substrate, single pulse energy was gradually increased from near the ablation threshold value to an energy value that caused the complete removal of the NLTF. In addition to single-pulse selective ablation, the multi-pulse USLP irradiation and production of laser-induced periodic surface structures (LIPSSs) were also studied. In the presented experiment, we found the optimal combination of accumulated pulse number and pulse energy to achieve the LIPSS formation on the thin film. The laser-induced morphology was examined with optical microscopy, scanning electron microscopy, and optical profilometry. To interpret the experimental observations, a theoretical simulation has been performed to explore the thermal response of the NLTFs after irradiation with single laser pulses.

Ultra‐Broadband Visible‐DUV Supercontinuum Generation by Non‐Resonant Coherent Raman Scattering in Air

AbstractTo date, supercontinuum light in the visible and near‐infrared ranges is readily realizable by the optical Kerr effect through self‐phase modulation of ultrashort laser pulses in transparent media. However, it is still a challenge to extend the supercontinuum spectrum down to the deep‐ultraviolet (DUV) range, which is particularly needed for exploring ultrafast dynamics in chemistry, materials, and biology. Here, an approach of non‐resonant coherent Raman scattering is developed to generate ultra‐broadband visible‐DUV supercontinuum in ambient air with a spectral range spanning over 250 nm and a wavelength down to 220 nm. A rovibrational coherence is established in air molecules by filamentation of a near‐infrared femtosecond 800 nm pulse and two femtosecond Raman laser pulses at 267 and 400 nm are introduced into the coherent media to induce non‐resonant coherent Stokes and anti‐Stokes Raman scatterings, which serve as the spectral bridges to link the neighboring Raman pump laser spectra, resulting in ultra‐broadband supercontinuum light. The mechanism is further verified by examining the broadening of picosecond N2+ laser lines with narrow bandwidths (10–30 cm−1), which forms a supercontinuum spectrum spanning over 150 nm. The work provides a viable route for the establishment of coherent DUV supercontinuum in the gas media at designed wavelength ranges.

Highly Tunable Moiré Superlattice Potentials in Twisted Hexagonal Boron Nitrides.

Moiré superlattice of twisted hexagonal boron nitride (hBN) has emerged as an advanced atomically thin van der Waals interfacial ferroelectricity platform. Nanoscale periodic ferroelectric moiré potentials in twisted hBN allow the hosting of remote Coulomb superlattice potentials to adjacent 2D materials. Therefore, the new strategies for engineering moiré length, angle, and potential strength are essential for developing programmable quantum materials. Here, it demonstrates the realization of twisted hBN-based moiré superlattice platforms and visualizes the moiré domains and ferroelectric properties using Kelvin probe force microscopy (KPFM). Also, the regular moiré superlattice in the large area is reported. It offers the possibility to reproduce uniform moiré structures with precise control piezo stage stacking and heat annealing. It demonstrates cumulative multi-ferroelectric polarization and multi-level domains with multiple angle mismatched interfaces. Additionally, it observes the quasi-1D anisotropic moiré domains and show the highest resolution analysis of the local built-in strain between adjacent hBN layers compared to the conventional methods. Furthermore, in-situ manipulation of moiré potential is demonstrated using femtosecond pulse laser, which results in the optical phonon-induced atomic displacement at the hBN moiré interfaces. The results pave the way to develop precisely programmable moiré superlattice platforms and investigate strongly correlated physics.

A Refined Model for Ablation Through Cavitation Bubbles with Ultrashort Pulse Lasers

A Refined Model for Ablation Through Cavitation Bubbles with Ultrashort Pulse Lasers

Interatomic and intermolecular decay processes in quantum fluid clusters.

In this comprehensive review, we explore interatomic and intermolecular correlated electronic decay phenomena observed in superfluid helium nanodroplets subjected to extreme ultraviolet (XUV) radiation. Helium nanodroplets, known for their distinctive electronic and quantum fluid properties, provide an ideal environment for examining a variety of non-local electronic decay processes involving the transfer of energy, charge, or both between neighboring sites and resulting in ionization and the emission of low-kinetic energy electrons. Key processes include interatomic or intermolecular Coulombic decay (ICD) and its variants, such as electron transfer-mediated decay (ETMD). Insights gained from studying these light-matter interactions in helium nanodroplets enhance our understanding of the effects of ionizing radiation on other condensed-phase systems, including biological matter. We also emphasize the advanced experimental and computational techniques that make it possible to resolve electronic decay processes with high spectral and temporal precision. Utilizing ultrashort pulses from free-electron lasers, the temporal evolution of these processes can be&#xD;followed, significantly advancing our comprehension of the dynamics within quantum fluid clusters and non-local electronic interactions in nanoscale systems.

Ultrafast laser direct writing of in-line polarizers based on nano-gratings

Ultrafast laser direct writing of in-line polarizers based on nano-gratings