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Results for “Ultrafast Photonics”

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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Room temperature persisting surface charge carriers driven by intense terahertz electric fields in a topological insulator Bi 2 Se 3

Topologically protected surface current is highly promising for next-generation low-dissipation and disorder-tolerant quantum electronics and computing. Yet, electric transport from the co-existing bulk state dominates the responses of the Dirac surface state, especially at elevated temperatures relevant to technological applications. Here, we present an approach that convincingly showcases the generation, disentanglement, and precise control of enduring surface charge carriers on a topological insulator, Bi 2 Se 3 , with high bulk conductivity, all achieved at room temperature. By using pump–probe modulation spectroscopy under ultrabroadband driving tunable from 4 meV to 1.55 eV, we show the terahertz (THz) field-induced surface carriers by discovering their initial temporal responses dominant over high density trivial bulk carriers. Strikingly, the response of the induced surface carrier responses persists for more than ~5 ps and is enhanced by reducing pump photon energy. The dynamics and lifetime of the distinct surface response manifest themselves as the enhanced THz pump-induced THz transmission, which directly correlates with the transient negative THz conductivity. Increasing the THz driving field reduces the induced surface carrier lifetime and identifies, particularly, an optimal pump field of E s ~ 224 kV cm -1 for generating the dominant surface response relative to the bulk. This surface carrier dominant regime is suppressed by a joint effect of enhanced surface-bulk scattering and a more rapid saturation of surface excitation compared to the bulk that sets in above E s . The controllability of room temperature topologically surface carriers through pump photon energy offer compelling possibilities for extending this approach to other topological complex materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Coherent light control of a metastable hidden state

Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS 2 upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Terahertz-field activation of polar skyrons

Unraveling collective modes arising from coupled degrees of freedom is crucial for understanding complex interactions in solids and developing new functionalities. Unique collective behaviors emerge when two degrees of freedom, ordered on distinct length scales, interact. Polar skyrmions, three-dimensional electric polarization textures in ferroelectric superlattices, disrupt the lattice continuity at the nanometer scale with nontrivial topology, leading to previously unexplored collective modes. Here, using terahertz-field excitation and femtosecond x-ray diffraction, we discover subterahertz collective modes, dubbed “skyrons”, which appear as swirling patterns of atomic displacements functioning as atomic-scale gearsets. The key to activating skyrons is the use of the THz field that couples primarily to skyrmion domain walls. Momentum-resolved time-domain measurements of diffuse scattering reveal an avoided crossing in the dispersion relation of skyrons. Atomistic simulations and dynamical phase-field modeling provide microscopic insights into the three-dimensional crystallographic and polarization dynamics. The amplitude and dispersion of skyrons are demonstrated to be controlled by sample temperature and electric-field bias. The discovery of skyrons and their coupling with terahertz fields opens avenues for ultrafast control of topological polar structures.

ferroelectrics↗
DOE OSTI2022

Attosecond coherent electron motion in Auger-Meitner decay

In quantum systems, coherent superpositions of electronic states evolve on ultrafast time scales (few femtoseconds to attoseconds; 1 attosecond = 0.001 femtoseconds = 10 -18 seconds), leading to a time-dependent charge density. Here we performed time-resolved measurements using attosecond soft x-ray pulses produced by a free-electron laser, to track the evolution of a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse, we created a clock to time-resolve the electron dynamics and demonstrated control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Broadband Ultrafast Dynamics of Refractory Metals: TiN and ZrN

Transition metal nitrides have recently gained attention in the fields of plasmonics, plasmon-enhanced photocatalysis, photothermal applications, and nonlinear optics because of their suitable optical properties, refractory nature, and large laser damage thresholds. Here we report comparative studies of the transient response of films of titanium nitride (TiN), zirconium nitride (ZrN), and gold (Au) under femtosecond excitation. Broadband transient optical characterization helps to adjudicate earlier, somewhat inconsistent reports regarding hot electron lifetimes based upon single wavelength measurements. These pump–probe experiments show sub-picosecond transient dynamics only within the epsilon-near-zero window of the refractory metals. The dynamics are dominated by photoinduced interband transitions resulting from ultrafast electron energy redistribution. The enhanced reflection modulation in the epsilon-near-zero window makes it possible to observe the ultrafast optical response of these films at low pump fluences. These results indicate that electron–phonon coupling in TiN and ZrN is 25–100 times greater than in Au. Strong electron–phonon coupling drives the sub-picosecond optical response and facilitates greater lattice heating compared to Au, making TiN and ZrN promising for photothermal applications. The spectral response and dynamics of TiN and ZrN are only weakly sensitive to pump fluence and pump excitation energy. However, the magnitude of the response is much greater at higher pump photon energies and higher fluences, reaching peak observed values of 15% in TiN and 50% in ZrN in the epsilon-near-zero window.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ultrafast Collective Excited-State Dynamics of a Virus-Supported Fluorophore Antenna

Radiation brightening was recently observed in a multifluorophore-conjugated brome mosaic virus (BMV) particle at room temperature under pulsed excitation. On the basis of its nonlinear dependence on the number of chromophores, the origins of the phenomenon were attributed to a collective relaxation. However, the mechanism remains unknown. Here, we present ultrafast transient absorption and fluorescence spectroscopic studies which shed new light on the collective nature of the relaxation dynamics in such radiation-brightened, multifluorophore particles. Our findings indicate that the emission dynamics is consistent with a superradiance mechanism. The ratio between the rates of competing radiative and nonradiative relaxation pathways depends on the number of chromophores per virus. The findings suggest that small icosahedral virus shells provide a unique biological scaffold for developing nonclassical, deep subwavelength light sources and may open new avenues for the development of photonic probes for medical imaging applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Pathways to excitation of atoms with bicircular laser pulses

We study the excitation of the hydrogen atom by bichromatic circularly polarized laser pulses using numerical solutions of the time-dependent Schrödinger equation. The results are in agreement with the selection rules for multiphoton processes in such fields, namely, excited states are populated in which orbital angular momentum and magnetic quantum numbers are either both odd or both even, independent of the relative helicity, peak intensity, and pulse duration of the pulses. For co-rotating pulses the results show that excitation predominantly proceeds to states with magnetic quantum number of the same helicity as the laser pulses. Besides pathways via direct photon absorption from the ground state our results indicate that a transfer of population among the Rydberg states occurs via Λ-type transitions. In the case of counter-rotating pulses the largest excitation probability is found for Rydberg states that differ in magnetic quantum number by Δm=±3. This pattern allows us to estimate how many photons from each of the two bichromatic fields have been absorbed. Finally, we confirm that a population in Rydberg states beyond a maximum orbital angular quantum number is unlikely.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Dynamical Nonlinear Inversion of the Surface Photovoltage at Si(100)

A surface photovoltage (SPV) is observed whenever a doped semiconductor with non-negligible band bending is illuminated by light and charge carriers are excited across the band gap. The sign of the SPV depends on the nature of the doping, the amplitude of the SPV increases with the fluence of the light illumination up to a saturation value, which is determined by the doping concentration. We have investigated Si(100) samples with well-characterized doping levels over a wide range of illumination fluences. Surprisingly, the sign of the SPV upon illumination with 532 nm photons reverses for some p-doping concentrations at high fluences. This is a new effect associated with a crossover between electronic excitations in the bulk and at the surface of the semiconductor.

14 SOLAR ENERGY↗
DOE OSTI2025

Soft x-ray high-harmonic generation in an anti-resonant hollow core fiber driven by a 3 μ m ultrafast laser

High-harmonic upconversion driven by a mid-infrared femtosecond laser can generate coherent soft x-ray beams in a tabletop-scale setup. Here, we report on a compact ytterbium-pumped optical parametric chirped pulse amplifier (OPCPA) laser system seeded by an all-fiber front-end and employing periodically poled lithium niobate (PPLN) nonlinear media operated near the pulse fluence limits of current commercially available PPLN crystals. The OPCPA delivers 3 µm wavelength pulses with 775 µJ energy at 1 kHz repetition rate, with transform-limited 120 fs pulse duration, diffraction-limited beam quality, and ultrahigh 0.33% rms energy stability over >18 h. Using this laser, we generate soft x-ray high harmonics (HHG) in argon gas by focusing into a low-loss, high-pressure gas-filled anti-resonant hollow core fiber (ARHCF), generating coherent light at photon energies up to the argon L-edge (250 eV) and carbon K-edge (284 eV), with high beam quality and ∼1% rms energy stability. This work demonstrates soft x-ray HHG in a high-efficiency guided-wave phase matched geometry, overcoming the high losses inherent to mid-IR propagation in unstructured waveguides, or the short interaction lengths of gas cells or jets. The ARHCF can operate in the long term without damage and with the repetition rate, stability, and robustness required for demanding applications in spectromicroscopy and imaging. Finally, we discuss routes for further optimizing the soft x-ray HHG flux by driving He at higher laser intensities using either the signal (1.5 μm) or idler wavelengths (3 μm).

Femtosecond lasers↗
DOE OSTI2025

Photoactivation Transition State and Dynamical Response of the Orange Carotenoid Protein

The orange carotenoid protein (OCP) regulates light harvesting in cyanobacteria by acting as a photoreceptor in its resting form, OCP O , and by effecting the quenching of bilin excitons upon binding to the core of the phycobilisome in its photoactivated red form, OCP R . We show herein using fluorescence anisotropy measurements and the action spectra for the rate constants of the two light-driven steps in the mechanism that the photoactivation of the OCP from Synechocystis sp. PCC 6803 is triggered by excited-state motions of the canthaxanthin chromophore that yield a twisted and bent conformation. Well-tempered metadynamics simulations reveal that a bicycle-pedal configuration, due to twisting of the two adjacent C=C bonds at the C13−C14 and C15−C15′ positions in the center of canthaxanthin’s π-conjugated isoprenoid backbone, can be accommodated by the binding site in the OCP, with the energy of a captured photon required to cross the local activation energy barriers from the dark equilibrium structure. The bicycle-pedal configuration breaks the conserved hydrogen-bonding interactions between the carbonyl substituent of the β-ionone end ring of canthaxanthin and the adjacent W288 and Y201 residues in the C-terminal domain. The action spectra are modulated by the vibronic excitation prepared by absorption transitions to the S 2 state, indicating that the photoactivation reactions are triggered by the canthaxanthin chromophore well prior to vibrational equilibration. These findings show that an ultrafast structural response of the OCP protein to the excited-state motions of the canthaxanthin chromophore controls the photoactivation yield and the sensing of blue light.

Fluorescence↗
DOE OSTI2024

Symmetry-Breaking Charge Transfer in Metal–Organic Frameworks

High quantum-yield charge carrier generation from the initially prepared excitons defines a key step in the light-harvesting and conversion scheme. Photoinduced charge transfer in molecular electron donor—acceptor assemblies is driven by a sizable ΔG 0 , which compromises the potential of the generated carriers. Reminiscent of the special pair at the reaction center of the natural light-harvesting complex, symmetry-breaking charge transfer (SBCT) within a pair of identical struts of metal-organic framework (MOF) will facilitate the efficient generation of long-lived charge carriers with maximized potentials without incorporating any foreign redox species. We report SBCT in pyrene-based zirconium metal–organic framework (MOF) NU-1000 that leads to efficient generation of radical ions in a polar solvent and bound CT states in a low-polar solvent. Further, the probe unveils the role of the low-lying non-Franck–Condon excitonic states as intermediates in the formation of the SBCT state from the initially prepared Franck–Condon S 1 states. Ultrafast and transient spectroscopy—probed over 200 fs-30 μs time scale-evinces a k SBCT = (110 ps) -1 in polar media (ε s = 37.5) forming solvated radical ions with recombination rate k CR = (~45 ns) -1 . A slower rate with k SBCT = (203 ps) -1 was recorded in low-polar (ε s = 7.0) solvent manifesting a bound [TBAPy •+ TBAPy •– ] state with k CR ≈ (17 μs) -1 . This discovery, along with other unique photophysical features relevant to light harvesting, should define a MOF-based platform for developing heterogeneous artificial photon energy conversion systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Ultrafast Production of NiCO and Ni Following 197 nm Photodissociation of Nickel Tetracarbonyl

Herein, we report on the ultrafast photodissociation of nickel tetracarbonyl—a prototypical metal–ligand model system—at 197 nm. Using mid-infrared transient absorption spectroscopy to probe the bound C≡O stretching modes, we find evidence for the picosecond time scale production of highly vibronically excited nickel dicarbonyl and nickel monocarbonyl, in marked contrast with a prior investigation at 193 nm. Further spectral evolution with a 50 ps time constant suggests an additional dissociation step; the absence of any corresponding growth in signal strongly indicates the production of bare Ni, a heretofore unreported product from single-photon excitation of nickel tetracarbonyl. Thus, by probing the deep UV-induced photodynamics of a prototypical metal carbonyl, this Letter adds time-resolved spectroscopic signatures of these dynamics to the sparse literature at high excitation energies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Multi-messenger dynamic imaging of laser-driven shocks in water using a plasma wakefield accelerator

Understanding dense matter hydrodynamics is critical for predicting plasma behavior in environments relevant to laser-driven inertial confinement fusion. Traditional diagnostic sources face limitations in brightness, spatiotemporal resolution, and in their ability to detect relevant electromagnetic fields. In this work, we present a dual-probe, multi-messenger laser wakefield accelerator platform combining ultrafast X-rays and relativistic electron beams at 1 Hz, to interrogate a free-flowing water target in vacuum, heated by an intense 200 ps laser pulse. This scheme enables high-repetition-rate tracking the evolution of the interaction using both particle types. Betatron X-rays reveal a cylindrically symmetric shock compression morphology assisted by low-density vapor, resembling foam-layer-assisted fusion targets. The synchronized electron beam detects time-evolving electromagnetic fields, uncovering charge separation and ion species differentiation during plasma expansion – phenomena not captured by photons or hydrodynamic simulations. We show that combining both probes provides complementary insights spanning kinetic to hydrodynamic regimes, highlighting the need for hybrid physics models to accurately predict fusion-relevant plasma behavior.

imaging techniques↗
DOE OSTI2023

Ultrafast time-resolved 2D imaging of laser-driven fast electron transport in solid density matter using an x-ray free electron laser

High-power, short-pulse laser-driven fast electrons can rapidly heat and ionize a high-density target before it hydrodynamically expands. The transport of such electrons within a solid target has been studied using two-dimensional (2D) imaging of electron-induced Kα radiation. However, it is currently limited to no or picosecond scale temporal resolutions. Here, we demonstrate femtosecond time-resolved 2D imaging of fast electron transport in a solid copper foil using the SACLA x-ray free electron laser (XFEL). An unfocused collimated x-ray beam produced transmission images with sub-micron and ~10 fs resolutions. The XFEL beam, tuned to its photon energy slightly above the Cu K-edge, enabled 2D imaging of transmission changes induced by electron isochoric heating. Time-resolved measurements obtained by varying the time delay between the x-ray probe and the optical laser show that the signature of the electron-heated region expands at ~25% of the speed of light in a picosecond duration. Time-integrated Cu Kα images support the electron energy and propagation distance observed with the transmission imaging. The x-ray near-edge transmission imaging with a tunable XFEL beam could be broadly applicable for imaging isochorically heated targets by laser-driven relativistic electrons, energetic protons, or an intense x-ray beam.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

A Flat Analyzer Polycapillary Spectrometer for X-ray Absorption Spectroscopy of Dilute Transition Metals at X-ray-Free Electron Lasers

X-ray absorption spectroscopy (XAS) coupled with highly intense pulses from an X-ray-free electron laser (XFEL) can be used to track ultrafast chemical dynamics. Nonetheless, measurements for dilute samples (≤1 mM) have been exceptionally challenging, as scattering background signals dominate over the sample’s X-ray fluorescence. We show that femtosecond time-resolved XAS measurements of sub-millimolar transition metal solutions are now possible at the Linac Coherent Light Source (LCLS) using a high-throughput polycapillary XAS spectrometer, designed, developed, and commissioned at LCLS and the Stanford Synchrotron Radiation Lightsource (SSRL). The instrument integrates three polycapillary optics that collect and collimate X-ray fluorescence emitted from the interaction point with a high solid angle. X-ray collimated fluorescence is then selectively diffracted by coupled graphite analyzer crystals. As a result, the contribution of scattered photons is suppressed. Experiments at the Pt L 3 -edge on 0.1 mM aqueous K 2 PtCl 6 (delivered via a 100 μm liquid jet) were successfully performed in the laser pump X-ray probe configuration at the LCLS XCS and XPP instruments. We report the transient spectra of hexachloroplatinate within the first 10 ps after a 266 nm photoexcitation. We observed a short-lived reduced intermediate (≈2 ps). The polycapillary X-ray spectrometer at LCLS now enables the efficient study of the dynamics of ultradilute transition metals in solution. This capability opens the door to investigating plasmonic systems, photocatalysts, enzymes, and other scarce and dilute samples.

LCLS↗
DOE OSTI2025

Stimulated Emission from Below the Bandgap in Giant Quantum Shells

Colloidal semiconductor nanocrystals (NCs) have emerged as promising candidates for developing solution-processable optical gain media, with potential applications in integrated photonic circuits and lasers. However, the deployment of NCs in these technologies has been hindered by nonradiative Auger recombination of multiexciton states, which shortens the optical gain lifetime and reduces its spectral range. Here, we demonstrate that these limitations can be overcome by using giant colloidal quantum shells (g-QSs), comprising a quantum-confined CdSe shell grown over a large (~14 nm) CdS bulk core. Such bulk-nanoscale architecture minimizes exciton–exciton interactions, leading to suppressed Auger recombination and one of the broadest gain bandwidths reported for colloidal nanomaterials, spanning energies both above and, remarkably, below the bandgap. Ultrafast transient absorption and photoluminescence measurements demonstrate that the high-energy portion of optical gain arises from states containing more than 15 excitons per particle while the unusual sub-bandgap gain behaviour results from an Auger-assisted radiative recombination, a mechanism that has traditionally been viewed as a loss pathway. Altogether, these results reveal a unique gain regime associated with bulk-nanocrystal hybrid systems, which offers a promising path toward solution-processable light sources.

Absorption↗
DOE OSTI2020

Speckle correlation as a monitor of X-ray free-electron laser induced crystal lattice deformation

X-ray free-electron lasers (X-FELs) present new opportunities to study ultrafast lattice dynamics in complex materials. While the unprecedented source brilliance enables high fidelity measurement of structural dynamics, it also raises experimental challenges related to the understanding and control of beam-induced irreversible structural changes in samples that can ultimately impact the interpretation of experimental results. This is also important for designing reliable high performance X-ray optical components. In this work, X-FEL beam-induced lattice alterations are investigated by measuring the shot-to-shot evolution of near-Bragg coherent scattering from a single crystalline germanium sample. It is shown that X-ray photon correlation analysis of sequential speckle patterns measurements can be used to monitor the nature and extent of lattice rearrangements. Additionally, abrupt, irreversible changes are observed following intermittent high-fluence monochromatic X-ray pulses, thus revealing the existence of a threshold response to X-FEL pulse intensity.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Harmonic generation predominantly from a single spin channel in a half metal

Harmonic generation in atoms and molecules has reshaped our understanding of ultrafast phenomena beyond the traditional nonlinear optics and has launched attosecond physics. Harmonics from solids represent a new frontier, where both majority and minority spin channels contribute to harmonics. This is true even in a ferromagnet whose electronic states are equally available to optical excitation. In this work, we demonstrate that harmonics can be generated {mostly} from a single spin channel in half metallic chromium dioxide. An energy gap in the minority channel greatly reduces the harmonic generation, so harmonics predominantly emit from the majority channel, with a small contribution from the minority channel. However, this is only possible when the incident photon energy is well below the energy gap in the minority channel, so all the transitions in the minority channel are virtual. The onset of the photon energy is determined by the transition energy between the dipole-allowed transition between the O-$2p$ and Cr-$3d$ states. Harmonics mainly from a single spin channel can be detected, regardless of laser field strength, as far as the photon energy is below the minority band energy gap. This prediction should be tested experimentally

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗