Search NASA⌕ Search

SEARCH · Search NASA

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Inverse design for waveguide dispersion with a differentiable mode solver

Inverse design of optical components based on adjoint sensitivity analysis has the potential to address the most challenging photonic engineering problems. However, existing inverse design tools based on finite-difference-time-domain (FDTD) models are poorly suited for optimizing waveguide modes for adiabatic transformation or perturbative coupling, which lies at the heart of many important photonic devices. Among these, dispersion engineering of optical waveguides is especially challenging in ultrafast and nonlinear optical applications involving broad optical bandwidths and frequency-dependent anisotropic dielectric material response. In this work, we develop gradient back-propagation through a general-purpose electromagnetic eigenmode solver and use it to demonstrate waveguide dispersion optimization for second harmonic generation with maximized phase-matching bandwidth. This optimization of three design parameters converges in eight steps, reducing the computational cost of optimization by ∼100x compared to exhaustive search and identifying new designs for broadband optical frequency doubling of laser sources in the 1.3–1.4 µm wavelength range. Furthermore, we demonstrate that the computational cost of gradient back-propagation is independent of the number of parameters, as required for optimization of complex geometries. This technique enables practical inverse design for a broad range of previously intractable photonic devices.

Gray, Dodd (ORCID:000000030469599X)↗
DOE OSTI2021

Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast $\mathrm{XUV}$-$\mathrm{IR}$ regime

Polycyclic aromatic hydrocarbons (PAHs) play an important role in interstellar chemistry and are subject to high energy photons that can induce excitation, ionization, and fragmentation. Previous studies have demonstrated electronic relaxation of parent PAH monocations over 10–100 femtoseconds as a result of beyond-Born-Oppenheimer coupling between the electronic and nuclear dynamics. Here, we investigate three PAH molecules: fluorene, phenanthrene, and pyrene, using ultrafast XUV and IR laser pulses. Simultaneous measurements of the ion yields, ion momenta, and electron momenta as a function of laser pulse delay allow a detailed insight into the various molecular processes. We report relaxation times for the electronically excited PAH * , PAH +* and PAH 2+* states, and show the time-dependent conversion between fragmentation pathways. Additionally, using recoil-frame covariance analysis between ion images, we demonstrate that the dissociation of the PAH 2+ ions favors reaction pathways involving two-body breakup and/or loss of neutral fragments totaling an even number of carbon atoms.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Nonlinear optics in 2D materials: From classical to quantum

Nonlinear optics has long been a cornerstone of modern photonics, enabling a wide array of technologies, from frequency conversion to the generation of ultrafast light pulses. Recent breakthroughs in two-dimensional (2D) materials have opened a frontier in this field, offering new opportunities for both classical and quantum nonlinear optics. These atomically thin materials exhibit strong light–matter interactions and large nonlinear responses, thanks to their tunable lattice symmetries, strong resonance effects, and highly engineerable band structures. In this paper, we explore the potential that 2D materials bring to nonlinear optics, covering topics from classical nonlinear optics to nonlinearities at the few-photon level. We delve into how these materials enable possibilities, such as symmetry control, phase matching, and integration into photonic circuits. The fusion of 2D materials with nonlinear optics provides insights into the fundamental behaviors of elementary excitations—such as electrons, excitons, and photons—in low-dimensional systems and has the potential to transform the landscape of next-generation photonic and quantum technologies.

2D materials↗
DOE OSTI2022

Ultrafast infrared plasmon switching in aligned carbon-nanotube optical resonators

Reconfigurable plasmonic materials are crucial components in active photonic devices for optical communication, signal processing, and sensing applications. Certain candidates including transparent conducting oxides, small-bandgap semiconductors (i.e. Ge, InSb), and conducting polymers can exhibit switchable free carrier concentrations triggered by optical, electrical or thermal excitations. Here, we show that aligned films of single-walled carbon nanotubes (SWCNTs) can serve as all-optically tunable plasmonic material in the mid-infrared range, thereby adding them to the library of switchable plasmonic materials. Interband optical pumping with femtosecond laser pulses results in the photoexcitation of free charge carriers, which transiently blueshifts the plasmon resonances of patterned, periodic SWCNT nano-resonators spanning the mid-infrared spectral range from 1700 to 2700 cm -1 . Furthermore. the ultrafast plasmon modulation exhibits a nearly single-picosecond decay time, attributed to interband carrier relaxation and inter-tube charge transfer. Given that aligned films of SWCNTs have high thermal stability, excellent photostability, epsilon-near-zero property, and extremely large optical anisotropy, their dynamic tunability represents a promising pathway towards active optical devices in the technologically important mid-infrared range.

single-walled carbon nanotubes↗
DOE OSTI2021

Autoionizing Polaritons in Attosecond Atomic Ionization

Light-induced states and Autler-Townes splitting of laser-coupled states are common features in the photoionization spectra of laser-dressed atoms. The entangled light-matter character of metastable Autler-Townes multiplets, which makes them autoionizing polaritons, however, is still largely unexplored. We employ attosecond transient-absorption spectroscopy in argon to study the formation of polariton multiplets between the 3s –1 4p and several light-induced states. We measure a controllable stabilization of the polaritons against ionization, in excellent agreement with ab initio theory. Using an extension of the Jaynes-Cummings model to autoionizing states, we show that this stabilization is due to the destructive interference between the Auger decay and the radiative ionization of the polaritonic components. Furthermore, these results give new insights into the optical control of electronic structure in the continuum and unlock the door to applications of radiative stabilization in metastable polyelectronic systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

The DREAM Endstation at the Linac Coherent Light Source

Free-electron lasers (FEL), with their ultrashort pulses, ultrahigh intensities, and high repetition rates at short wavelength, have provided new approaches to Atomic and Molecular Optical Science. One such approach is following the birth of a photo electron to observe ion dynamics on an ultrafast timescale. Such an approach presents the opportunity to decipher the photon-initiated structural dynamics of an isolated atomic and molecular species. It is a fundamental step towards understanding single- and non-linear multi-photon processes and coherent electron dynamics in atoms and molecules, ultimately leading to coherent control following FEL research breakthroughs in pulse shaping and polarization control. A key aspect for exploring photoinduced quantum phenomena is visualizing the collective motion of electrons and nuclei in a single reaction process, as dynamics in atoms/ions proceed at femtosecond (10 –15 s) timescales while electronic dynamics take place in the attosecond timescale (10 –18 s). Here, we report on the design of a Dynamic Reaction Microscope (DREAM) endstation located at the second interaction point of the Time-Resolved Molecular and Optical (TMO) instrument at the Linac Coherent Light Source (LCLS) capable of following the photon–matter interactions by detecting ions and electrons in coincidence. The DREAM endstation takes advantage of the pulse properties and high repetition rate of LCLS-II to perform gas-phase soft X-ray experiments in a wide spectrum of scientific domains. With its design ability to detect multi-ions and electrons in coincidence while operating in step with the high repetition rate of LCLS-II, the DREAM endstation takes advantage of the inherent momentum conservation of reaction product ions with participating electrons to reconstruct the original X-ray photon–matter interactions. In this report, we outline in detail the design of the DREAM endstation and its functionality, with scientific opportunities enabled by this state-of-the-art instrument.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Ultrafast structural changes direct the first molecular events of vision

Vision is initiated by the rhodopsin family of light-sensitive G protein-coupled receptors (GPCRs). A photon is absorbed by the 11-cis retinal chromophore of rhodopsin, which isomerizes within 200 femtoseconds to the all-transconformation, thereby initiating the cellular signal transduction processes that ultimately lead to vision. However, the intramolecular mechanism by which the photoactivated retinal induces the activation events inside rhodopsin remains experimentally unclear. Here we use ultrafast time-resolved crystallography at room temperature to determine how an isomerized twisted all-trans retinal stores the photon energy that is required to initiate the protein conformational changes associated with the formation of the G protein-binding signalling state. The distorted retinal at a 1-ps time delay after photoactivation has pulled away from half of its numerous interactions with its binding pocket, and the excess of the photon energy is released through an anisotropic protein breathing motion in the direction of the extracellular space. Notably, the very early structural motions in the protein side chains of rhodopsin appear in regions that are involved in later stages of the conserved class A GPCR activation mechanism. Our study sheds light on the earliest stages of vision in vertebrates and points to fundamental aspects of the molecular mechanisms of agonist-mediated GPCR activation.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Side-chain ionization enables ultrafast intramolecular singlet fission in the azaquinodimethane skeleton

Singlet fission (SF) could significantly alleviate thermalization losses of high-energy photons, thus holding great potential for improving the power conversion efficiency of solar cells. Conventional SF materials require an intricate control of molecular packing motifs in the solid state to achieve efficient multiexciton generation. Small molecule intramolecular singlet fission (iSF) materials have emerged as promising alternatives and show great potential for practical device applications. However, the scope of such iSF materials remains rather limited, necessitating innovative molecular design strategies. Herein, we present how a side-chain ionization strategy leads to an iSF chromophore based on the azaquinodimethane (AQM) ring system. Systematic theoretical and spectroscopic analyses reveal that the direct attachment of electron-withdrawing ionic groups to the conjugated AQM core renders the originally fluorescent AQM nonemissive, leading to ionic AQM (iAQM) derivatives capable of ultrafast iSF to populate triplet-like species. Further fine-tuning of the iAQM skeleton imparts subtle intermolecular interactions that are indispensable for the efficient separation of triplet pairs following iSF in the aggregated state. Our findings offer unprecedented insights into molecular design and triplet exciton dynamics, laying the foundation for the discovery of rare molecular iSF materials.

Wu, Zixiang↗
DOE OSTI2025

Interligand Coupling Drives Fast Triplet Energy Transfer Routes in PbS/Tetracene Quantum Dot Hybrids

The binding of photoactive organic ligands to inorganic quantum dots (QDs) creates a versatile hybrid architecture that allows access to photophysical processes such as efficient triplet exciton generation with near-infrared radiation. Here we report the subnanosecond generation of a hybrid triplet state with mixed ligand-QD character by replacing native oleate ligands on small PbS QDs with 5,12-tetracenepropiolic acid, a bifunctional ligand with two carboxylic acids that tends to lie face-on with the QD surface at low loadings. The face-on geometry engenders a regime of strong electronic coupling that is evident in steady-state absorption and hastens triplet energy flow by several orders of magnitude compared with more typical tetracene-based ligands exhibiting weak coupling. We further determined via Fourier transform infrared (FTIR) and supported by density functional theory (DFT)-based geometry optimizations that high ligand loading causes a shift in QD-ligand mutual disposition toward an edge-on geometry that instigates the formation of intermolecular excited states characterized by triplet excimer-like features in photoluminescence and transient absorption. Our results demonstrate the ability to control strongly coupled ligand-QD systems toward ultrafast generation of photophysically relevant species such as triplets that are valuable for photon upconversion and catalysis.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Imaging Wavepackets in Real-Space & Disentangling Ultrafast Solvation Dynamics with High-Energy Ultrafast X-ray Scattering

The microscopic information of solute and solute-solvent motions can be measured using ultrafast diffuse x-ray scattering, and compared to molecular dynamics simulations, as demonstrated in studies of solvated molecular systems done in X-ray free-electron lasers. However, for the typical photon energies used in these experiments, the photon momentum transfer range was limited to lower Q values where the signals arising from different parts of the studied system overlap significantly. Recently, this limitation was greatly alleviated by extending the photon energy at the Linac Coherent Light-Source (LCLS), significantly increasing the accessible momentum transfer range. This improvement is transformative for ultrafast diffuse x-ray scattering measurements, enabling for the first time to disentangle the solute scattering difference signal, that persists to higher Q values, from the bulk solvent and solute-solvent cross-terms difference signals. In addition, it enhances the prediction ability of modeling and simulation methods such as the hybrid QM/MM approach. The extended Q range also opens the way to resolve in real-space details regarding coherent wavepackets motions beyond their center-of-mass positions. Here, we present the first results on high-energy (18keV) diffuse x-ray scattering in solution, demonstrating high fidelity time-resolved scattering and analysis of the photoexcited model photocatalysts PtPOP ([Pt2(POP)4]4-), and IrDimen ([Ir2(dimen)4]2+) in several solvents. These complexes provide ideal systems for demonstrating the ability of high-Q ultrafast scattering and QM/MM simulations to decompose ultrafast solvation dynamics into specific changes in the solute-solvent pair distribution function with a particular focus on how electronically excited states change the interaction between the solvent and photo-catalytically active metal sites. We introduce an approach to further utilize the high-energy capability and demonstrate a single-shot ultra-wide-angle X-ray Scattering modality using two perpendicular detectors, spanning a scattering angle range of more than 100 degrees, allowing to extend the accessible momentum transfer range up to Q~14 Å-1. We develop a model-free method to invert the x-ray scattering signals and enable the recovery of multiple pair-density motions that happen simultaneously, allowing us to directly measure in real-space nuclear wavepacket motions. . [1] Natan, Adi. "Real-Space Inversion and Super-Resolution of Ultrafast X-ray Scattering using Natural Scattering Kernels." arXiv preprint arXiv:2107.05576 (2021)

Natan, Adi↗
DOE OSTI2022

Ultrafast Triplet Generation at the Lead Halide Perovskite/Rubrene Interface

Triplet sensitization of rubrene by bulk lead halide perovskites has recently resulted in efficient infrared-to-visible photon upconversion via triplet-triplet annihilation. Notably, this process can occur under solar relevant fluxes, potentially paving the way toward integration with photovoltaic devices. In order to further improve the upconversion efficiency, the fundamental photophysical pathways at the perovskite/rubrene interface must be clearly understood to maximize charge extraction. Here, we utilize ultrafast transient absorption spectroscopy to elucidate the processes underlying triplet generation at the perovskite/rubrene interface. In this work, our results point to a triplet generation mechanism based on hot carriers; thermally excited charge carriers in the perovskite cool more rapidly in the presence of rubrene, suggesting rapid extraction of these thermally excited carriers on the picosecond time scale. Subsequent triplet formation in rubrene is observed on a subnanosecond time scale.

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

Tuning the Quantum Dot (QD)/Mediator Interface for Optimal Efficiency of QD-Sensitized Near-Infrared-to-Visible Photon Upconversion Systems

Lead sulfide (PbS) quantum dots (QDs) have shown promising performance as a sensitizer in infrared-to-visible photon upconversion systems. To investigate the key design rules, we compare three PbS-sensitized upconversion systems using three mediator molecules with the same tetracene triplet acceptor at different distances from the QD. Using transient absorption spectroscopy, we directly measure the triplet energy-transfer rates and efficiencies from the QD to the mediator and from the mediator to the emitter. With increasing distance between the mediator and PbS QD, the efficiency of the first triplet energy transfer from the QD to the mediator decreases because of a decrease in the rate of this triplet energy-transfer step, while the efficiency of the second triplet energy transfer from the mediator to the emitter increases because of a reduction in the QD-induced mediator triplet state decay. The latter effect is a result of the slow rate constant of the second triplet energy-transfer process, which is 3 orders of magnitude slower than the diffusion-limited value. The combined results lead to a net decrease of the steady-state upconversion quantum yield with distance, which could be predicted by our kinetic model. Our result shows that the QD/mediator interface affects both the first and second triplet energy transfer processes in the photon upconversion system, and the QD/mediator distance has an opposite effect on the efficiencies of the first and second triplet energy transfer. Lastly, these findings provide important insight for the further rational improvement of the overall efficiency of QD-based upconversion systems.

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

Optics-on-a-chip for ultrafast manipulation of 350-MHz hard x-ray pulses

Microelectromechanical systems (MEMS) are miniature devices integrated into a vast range of industrial and consumer applications. Optical MEMS are developed for dynamic spatiotemporal control in lightwave manipulation and communication as modulators, switches, multiplexers, spectrometer, etc. However, they have not been shown to function similarly in sub-nm wavelength regimes, namely, with hard x-rays, as high-brilliance pulsed x-rays have proven powerful for addressing challenges in time-domain science, from energy conversion to neurobiological control. While desirable temporal properties of x-ray pulses can be enhanced by optics, conventional x-ray optics are inherently massive in size, hence, never dynamic. We demonstrate highly ultrafast x-ray optics-on-a-chip based on MEMS capable of modulating hard x-ray pulses exceeding 350 MHz, 10 3 × higher than any other mechanical modulator, with a pulse purity >10 6 without compromising the spectral brilliance. Moreover, the timing characteristics of the devices can be tuned on-the-fly to deliver optimal pulse properties to create a host of dynamic x-ray instruments and applications, impossible with traditional optics of 10 9 × bulkier and more massive. The advent of the ultrafast optics-on-a-chip heralds a new paradigm of x-ray photonics, time-domain science, and accelerator diagnostics, especially at not only the future-generation light sources that offer coherent and high-frequency pulses but also lab-based facilities that normally do not offer timing structures.

42 ENGINEERING↗
DOE OSTI2024

Ultrafast Symmetry Control in Photoexcited Quantum Dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2022

A Monte Carlo technique to model performance of streak camera-based time-resolving x-ray spectrometers

A Monte Carlo technique has been developed to simulate the expected signal and the statistical noise of x-ray spectrometers that use streak cameras to achieve the time resolution required for ultrafast diagnostics of laser-generated plasmas. The technique accounts for statistics from both the photons incident on the streak camera’s photocathode and the electrons emitted by the photocathode travelling through the camera’s electron optics to the sensor. We use the technique to optimize the design of a spectrometer, which deduces the temporal history of electron temperature of the hotspot in an inertial confinement fusion implosion from its hard x-ray continuum emission spectra. The technique is general enough to be applied to any instrument using an x-ray streak camera.

Stoupin, S. (ORCID:0000000226225270)↗
DOE OSTI2025

Spatio-spectral optical fission in time-varying subwavelength layers

Transparent conducting oxides are highly doped semiconductors that exhibit favourable optical features compared with metals, including reduced material losses, tuneable electronic and optical properties, and enhanced damage thresholds. Recently, the photonic community has renewed its attention towards these materials, recognizing their remarkable nonlinear optical properties in the near-infrared spectrum. The exceptionally large and ultrafast change in the refractive index, which can be optically induced in these compounds, extends beyond the boundaries of conventional perturbative analysis and makes this class of materials the closest approximation to a time-varying system. Here we report the spatio-spectral fission of an ultrafast pulse trespassing a thin film of aluminium zinc oxide with a non-stationary refractive index. By applying phase conservation to this time-varying layer, our model can account for both space and time refraction and explain, in quantitative terms, the spatial separation of both spectrum and energy. Our findings represent an example of extreme nonlinear phenomena on subwavelength propagation distances, which provides new insights into transparent conducting oxides’ transient optical properties. This can be critical for the ongoing research on photonic time crystals, on-chip generation of non-classical states of light, integrated optical neural networks, ultrafast beam steering and frequency-division multiplexing.

integrated optics↗
DOE OSTI2026

Ultrafast Dynamics of Excitonic Complexes in Electrolyte-Gated Monolayer MoS 2

Understanding and controlling ultrafast excitons and trion dynamics in monolayer transition metal dichalcogenides (TMDs) is critical for optoelectronic and photonic applications. These dynamics depend strongly on carrier density, but most studies use fluence-dependence to modulate electron-hole populations rather than direct electrostatic gating that is more relevant to optoelectronic devices. We utilize electrolyte gating to tune the ground-state carrier density of monolayer MoS 2 and probe excitonic dynamics using transient absorption spectroscopy, thereby modifying absorption through bandgap renormalization, screening, phase-space filling, and exciton-trion crossover. Spectral deconvolution reveals distinct but coupled exciton and trion dynamics. Excitons form independently of voltage but relax faster with increasing carrier density, consistent with Auger-like processes, while trions decay more rapidly through multiple channels. At higher voltages, trion relaxation shifts from a sub-picosecond cooling to slower trapping-assisted processes. Furthermore, our results provide missing insights into the interplay between excitons and trions in monolayer MoS 2 , relevant for TMD-based optoelectronics.

chalcogenides↗
DOE OSTI2023

Ultrafast Optical Nanoscopy of Carrier Dynamics in Silicon Nanowires

Carrier distribution and dynamics in semiconductor materials often govern their physical properties that are critical to functionalities and performance in industrial applications. The continued miniaturization of electronic and photonic devices calls for tools to probe carrier behavior in semiconductors simultaneously at the picosecond time and nanometer length scales. Here, in this paper, we report pump–probe optical nanoscopy in the visible-near-infrared spectral region to characterize the carrier dynamics in silicon nanostructures. By coupling experiments with the point-dipole model, we resolve the size-dependent photoexcited carrier lifetime in individual silicon nanowires. We further demonstrate local carrier decay time mapping in silicon nanostructures with a sub-50 nm spatial resolution. Our study enables the nanoimaging of ultrafast carrier kinetics, which will find promising applications in the future design of a broad range of electronic, photonic, and optoelectronic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗