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Results for “ultrafast optics”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Adaptive noise canceling for transient absorption microscopy

Significance: Ultrafast fiber lasers are an attractive alternative to bulk lasers for nonlinear optical microscopy for their compactness and low cost. The high relative intensity noise (RIN) of these lasers poses a challenge for pump-probe measurements such as transient absorption and stimulated Raman scattering, along with modalities that provide label-free contrast from the vibrational and electronic structure of molecules. Aim: Digital adaptive filtering was applied to determine the applicability for canceling laser RIN in a transient absorption microscope with an ultrafast fiber laser source. Approach: Digitized signals from the transmitted probe and reference photodetectors were fed to an adaptive filter in MATLAB, running in a noise canceling configuration. This result was then fed to a software lock-in algorithm to demodulate the pump-probe signal. Images were built up one line scan at a time with a 3.5-kHz resonant scanner, with 100× averaging. The imaging target was Bi4Ge3O12, which exhibits nondegenerate two-photon absorption at the pump/probe wavelengths used (530-nm pump and 490-nm probe). Results: Without adaptive noise cancellation, the lock-in output primarily passes the laser RIN within its detection bandwidth, resulting in images that closely follow the linear transmissivity and lack sensitivity to pump-probe time delay. With adaptive noise cancellation in front of the lock-in, the RIN rejection is enough to restore the z-sectioning and sensitivity to pump-probe delay, as expected for transient absorption. Results were limited primarily by noise from the photodetector and analog-to-digital converter. Conclusions: Digital adaptive noise cancellation, even when limited by electronics noise, can recover pump-probe signals by removal of laser RIN, under conditions where averaging alone fails.

42 ENGINEERING↗
DOE OSTI2025

Magnetic field driven emergent phenomena: Insights from magneto-optics and nanoscopy

This review explores magnetic field-driven emergent phenomena across various material systems, emphasizing the pivotal roles of magneto-optical and nanoscopy techniques. We examine fundamental aspects of Landau electrodynamics in both 2D and 3D systems, including quantum Hall and topological magnetoelectric effects in graphene and topological insulators. Particularly attention is given to magnetic excitations and magnetopolaritons, such as surface magnon polaritons, magnetoplasmons, and magnetoexcitons in novel quantum materials, including quantum magnets and hybrid heterostructures. Advanced imaging techniques, such as scattering-type scanning near-field optical microscopy (SNOM) and microwave impedance microscopy, are showcased for their capability to resolve these phenomena with microscopic and nanoscopic resolution. These insights are complemented by discussions of advanced experimental approaches, including cryogenic environments, ultrafast pump-probe techniques, and the integration of magnetic fields into near-field optical methodologies. We further investigate the potential of these imaging techniques for unraveling complex magnetic orders, quantum phases, and correlated electronic behaviors. Finally, we offer perspectives on future research directions and highlight emerging opportunities in the evolving field of optical magneto-nanoscopy.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ultrafast pulse pumping of topological nanospaser

Here, we theoretically examine a topological nanospaser that is optically pumped using an ultra-fast circularly-polarized pulse. The spasing system consists of a silver nanospheroid, which supports surface plasmon (SP) excitations, and a transition metal dichalcogenide (TMDC) monolayer nanoflake. The silver nanospheroid screens the incoming pulse and creates a non-uniform spatial distribution of electron excitations in the TMDC nanoflake. These excitations decay into the localized SPs, which can be of two types with the corresponding magnetic quantum number ±1. The amount and the type of the generated SPs depend on the intensity of the optical pulse. For small pulse amplitude, only one plasmonic mode is predominantly generated, resulting in far-field elliptically polarized radiation. For large amplitude of the optical pulse, both plasmonic modes are generated in almost the same amount, resulting in linearly polarized far-field radiation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Method and apparatus for measuring optical pulses

A pulse analysis system or method includes a frequency filter that receives an ultrafast pulse under test and disperses the pulse under test over a frequency range. The frequency filter separates the pulse under test into component frequency slices and provides the frequency slices to a detector coupled to a digitizer, which processes the digitized signal and collects a sonogram characteristic of the pulse under test. The frequency slices are arranged to overlap. Ptychography is performed on the sonogram to obtain characteristics of the pulse under test.

Kane, Daniel J.↗
DOE OSTI2023

Method and apparatus for measuring optical pulses

A pulse analysis system or method includes a frequency filter that receives an ultrafast pulse under test and disperses the pulse under test over a frequency range. The frequency filter separates the pulse under test into component frequency slices and provides the frequency slices to a detector coupled to a digitizer, which processes the digitized signal and collects a sonogram characteristic of the pulse under test. The frequency slices are arranged to overlap. Ptychography is performed on the sonogram to obtain characteristics of the pulse under test.

Kane, Daniel J.↗
DOE OSTI2023

Exploring fingerprints of ultrafast structural dynamics in molecular solutions with an X-ray laser

We apply ultrashort x-ray laser pulses to track optically excited structural dynamics of [Ir 2 (dimen) 4 ] 2+ molecules in solution. In our exploratory study we determine angular correlations in the scattered x-rays, which comprise a complex fingerprint of the ultrafast dynamics. Model-assisted analysis of the experimental correlation data allows us to elucidate various aspects of the photoinduced changes in the excited molecular ensembles. We unambiguously identify that in our experiment the photoinduced transition dipole moments in [Ir 2 (dimen) 4 ] 2+ molecules are oriented perpendicular to the Ir-Ir bond. The analysis also shows that the ground state conformer of [Ir 2 (dimen) 4 ] 2+ with a larger Ir–Ir distance is mostly responsible for the formation of the excited state. We also reveal that the ensemble of solute molecules can be characterized with a substantial structural heterogeneity due to solvent influence. In conclusion, the proposed x-ray correlation approach offers an alternative path for studies of ultrafast structural dynamics of molecular ensembles in the liquid and gas phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Spin-mediated shear oscillators in a van der Waals antiferromagnet

Understanding how microscopic spin configuration gives rise to exotic properties at the macroscopic length scale has long been pursued in magnetic materials. One seminal example is the Einstein-de Haas effect in ferromagnets, in which angular momentum of spins can be converted into mechanical rotation of an entire object. However, for antiferromagnets without net magnetic moment, how spin ordering couples to macroscopic movement remains elusive. Here we observed a seesaw-like rotation of reciprocal lattice peaks of an antiferromagnetic nanolayer film, whose gigahertz structural resonance exhibits more than an order-of-magnitude amplification after cooling below the Neel temperature. Using a suite of ultrafast diffraction and microscopy techniques, we directly visualize this spin-driven rotation in reciprocal space at the nanoscale. This motion corresponds to interlayer shear in real space, in which individual micro-patches of the film behave as coherent oscillators that are phase-locked and shear along the same in-plane axis. Using time-resolved optical polarimetry, we further show that the enhanced mechanical response strongly correlates with ultrafast demagnetization, which releases elastic energy stored in local strain gradients to drive the oscillators. Finally, our work not only offers the first microscopic view of spin-mediated mechanical motion of an antiferromagnet but it also identifies a new route towards realizing high-frequency resonators up to the millimetre band, so the capability of controlling magnetic states on the ultrafast timescale can be readily transferred to engineering the mechanical properties of nanodevices.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Electrochemical Control of the Ultrafast Lattice Response of a Layered Semimetal

The unique layer-stacking in two-dimensional (2D) van der Waals materials facilitates the formation of nearly degenerate phases of matter and opens novel routes for the design of low-power, reconfigurable functional materials. Electrochemical ion intercalation between stacked layers offers a promising approach to stabilize bulk metastable phases and to explore the effects of extreme carrier doping and strain. However, in situ characterization methods to study the structural evolution and dynamical functional properties of these intercalated materials remains limited. Here a novel experimental platform is presented capable of simultaneously performing electrochemical lithium-ion intercalation and multimodal ultrafast characterization of the lattice using both electron diffraction and nonlinear optical techniques. Using the layered semimetal WTe 2 as a model system, the interlayer shear phonon mode that modulates stacking between 2Dlayers is probed, showing that small amounts of lithiation enhance the amplitude and lifetime of the phonon, contrary to expectations. This results from the dynamically fluctuating and anharmonic structure between nearly degenerate phases at room temperature, which can be stabilized by electronic carriers accompanying the inserted lithium ions. At high lithiation, the T d ’ structure emerges and quenches the phonon response. This work defines new approaches for using electrochemistry to engineer the dynamic structure of 2D materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Direct Observation of Coherent Longitudinal and Shear Acoustic Phonons in TaAs Using Ultrafast X-Ray Diffraction

Here, using femtosecond time-resolved x-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral line shape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acoustic deformations can transiently alter the electronic structure near the Weyl points and support this with model calculations. Our study underscores the benefit of using off-axis crystal orientations when optically exciting acoustic deformations in topological semimetals, allowing one to transiently change their crystal and electronic structures.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Field-resolved observation of exciton coherence in a van der Waals magnet

The emergence of coherence among electronic quasiparticles underlies collective quantum phenomena from superconductivity to superradiance. In semiconductors, exciton coherence is generally thought to decay rapidly due to scattering and dephasing, limiting its persistence on ultrafast timescales. Here, in this work, we demonstrate a light-field-driven mechanism that creates and stabilizes exciton coherence in the layered antiferromagnet CrSBr. We directly record the coherent optical field emitted by excitons and track in real time how a deterministic phase, imprinted by the excitation laser, drives incoherent excitons to synchronize into a collective state. This ensemble remains phase coherent for more than 2 ps, whereas its resonance energy undergoes an ultrafast modulation mediated by spin and lattice interactions. The time-resolved field evolution indicates that the multiple peaks seen in conventional spectra originate from a single excitonic resonance subject to dynamic energy modulation. Our findings establish optical phase imprinting as a mechanism to control and sustain collective order in semiconducting magnets, bridging light-driven dynamics with excitonic and magnetic correlations in layered quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

All-optical single-shot complete electric field measurement of extreme ultraviolet free electron laser pulses

Recent advances in ultrafast extreme ultraviolet (EUV) and x-ray light sources provide direct access to fundamental time and length scales for biology, chemistry, and materials physics. However, such light pulses are challenging to measure due to the need for femtosecond time resolution at difficult-to-detect wavelengths. Also, single-shot measurements are needed because severe pulse-to-pulse fluctuations are common. Here we demonstrate single-shot, complete field measurements by applying a novel version of frequency resolved optical gating. An EUV free electron laser beam creates a transient grating containing the pulse’s electric field information, which is read out with a 400 nm probe pulse. By varying the time delay between two copies of the EUV pump, rather than between the pump and the probe, we separate the needed coherent wave mixing from the slow incoherent response. Because this approach uses photoionization, it should be applicable from the vacuum ultraviolet to hard x rays.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ultrafast Carrier Drift Transport Dynamics in CsPbI3 Perovskite Nanocrystalline Thin Films

We study the early time carrier drift dynamics in CsPbI3 nanocrystal thin films with a sub 25 ps time resolution. Prior to trapping, carriers exhibit band-like transport characteristics, which is similar to those of traditional semiconductor solar absorbers including Si and GaAs due to optical phonon and carrier scattering at high temperatures. In contrast to the popular polaron scattering mechanism, the CsPbI3 nanocrystal thin film demonstrates the strongest optical phonon scattering mechanism among other inorganic-organic hybrid perovskites, Si, and GaAs. This ultrafast dynamics study establishes a foundation for understanding the fundamental carrier drift properties that drive perovskite nanocrystal optoelectronics.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS,S↗
DOE OSTI2020

Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using ultrafast transient polarization spectroscopy, extending the well-known technique of optical Kerr effect spectroscopy to excited electronic states. The third-order nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S 1 excited state. By measuring this response, which is highly sensitive to details of the excited state character and structure, as a function of time delays between the three pulses involved, we extract the dephasing time of the wave packet on the excited state. The dephasing time, measured as a function of time delay after pump excitation, shows oscillations indicating oscillatory wave packet dynamics on the excited state. Finally, from the experimental measurements and supporting theoretical calculations, we deduce that the wave packet completely leaves the S 1 state potential energy surface after three traversals of the intersystem crossing between the singlet S 1 and triplet T 2 states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Multichannel photodissociation dynamics in CS 2 studied by ultrafast electron diffraction

In this study, the structural dynamics of photoexcited gas-phase carbon disulfide (CS 2 ) molecules are investigated using ultrafast electron diffraction. The dynamics were triggered by excitation of the optically bright 1 B 2 ( 1 Σ u + ) state by an ultraviolet femtosecond laser pulse centred at 200 nm. In accordance with previous studies, rapid vibrational motion facilitates a combination of internal conversion and intersystem crossing to lower-lying electronic states. Photodissociation via these electronic manifolds results in the production of CS fragments in the electronic ground state and dissociated singlet and triplet sulphur atoms. The structural dynamics are extracted from the experiment using a trajectory-fitting filtering approach, revealing the main characteristics of the singlet and triplet dissociation pathways. Finally, the effect of the time-resolution on the experimental signal is considered and an outlook to future experiments provided.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Optical current generation in graphene: CEP control vs. ω + 2 ω control

The injection of directional currents in solids with strong optical fields has attracted tremendous attention as a route to realize ultrafast electronics based on the quantum-mechanical nature of electrons at femto- to attosecond timescales. Such currents are usually the result of an asymmetric population distribution imprinted by the temporal symmetry of the driving field. Here we compare two experimental schemes that allow control over the amplitude and direction of light-field-driven currents excited in graphene. Both schemes rely on shaping the incident laser field with one parameter only: either the carrier-envelope phase (CEP) of a single laser pulse or the relative phase between pulses oscillating at angular frequencies ω and 2ω, both for comparable laser parameters. We observe that the efficiency in generating a current via two-color-control exceeds that of CEP control by more than two orders of magnitude (7 nA vs. 18 pA), as the ω + 2ω field exhibits significantly more asymmetry in its temporal shape. We support this finding with numerical simulations that clearly show that two-color current control in graphene is superior, even down to single-cycle pulse durations. We expect our results to be relevant to experimentally access fundamental properties of any solid at ultrafast timescales, as well as for the emerging field of petahertz electronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Spatio-Kinetic Electronic Heterogeneity in MoS 2 Revealed by Ultrafast Electron Microscopy: Implications for Optoelectronics

There is broad interest in layered, two-dimensional (2D) semiconductors owing to their high optical absorption and ability to heterogeneously integrate with various substrates. In such layered semiconductors, mesoscopic imperfections, such as surface step edges, may affect charge carrier kinetics and device performance, but studying their effects on carrier transport with sufficient spatial and temporal resolution is a challenge. Using scanning ultrafast electron microscopy, we image the near-surface charge carrier kinetics with μm/ps spatiotemporal resolution in single-crystal MoS 2 samples with surface steps tens of nanometers in height. We find an approximately 3-fold increase in surface trap density near such surface steps compared to the uniform, flat surface regions. Despite the difference in trap state density, filling of the traps occurs over the same time scale (∼100 ps), but carrier recovery is much slower near the step compared to the uniform regions of the material. Furthermore, these results provide an approach to measure ultrafast dynamics and determine the required uniformity of layered materials depending on the speed limit constraints for specific applications.

SEM↗
DOE OSTI2022

Control of valley polarization in gapped graphene by linearly polarized ultrashort optical pulse

We present a versatile model of gapped graphene to manipulate valley polarization by using ultrafast linearly polarized pulses of zero areas. First, a circularly polarized pulse of a single oscillation produces a valley-selective population of the conduction band by means of topological resonance. Then we apply a linearly polarized femtosecond-long pulse that changes the valley polarization. The magnitude of such a change depends on the amplitude and the direction of polarization of the pulse. In conclusion, our protocol provides a favorable platform for applications in valleytronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗