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Results for “Harmonic generation”

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 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Full characterization of ultrathin 5-nm low-k dielectric bilayers: Influence of dopants and surfaces on the mechanical properties

Ultrathin films and multilayers, with controlled thickness down to single atomic layers, are critical for advanced technologies ranging from nanoelectronics to spintronics to quantum devices. However, for thicknesses less than 10 nm, surfaces and dopants contribute significantly to the film properties, which can differ dramatically from that of bulk materials. Therefore, for amorphous films being developed as low dielectric constant interfaces for nanoelectronics, the presence of surfaces or dopants can soften films and degrade their mechanical performance. Here we use coherent short-wavelength light to fully and nondestructively characterize the mechanical properties of individual films as thin as 5 nm within a bilayer. In general, we find that the mechanical properties depend both on the amount of doping and the presence of surfaces. In very thin (5-nm) silicon carbide bilayers with low hydrogen doping, surface effects induce a substantial softening - by almost an order of magnitude - compared with the same doping in thicker (46-nm) bilayers. These findings are important for informed design of ultrathin films for a host of nano- and quantum technologies, and for improving the switching speed and efficiency of next-generation electronics.

36 MATERIALS SCIENCE↗
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 OSTI2023

Reinvented: An Attosecond Chemist

Attosecond science requires a substantial rethinking of how to make measurements on very short timescales; how to acquire the necessary equipment, technology, and personnel; and how to build a set of laboratories for such experiments. This entails a rejuvenation of the author in many respects, in the laboratory itself, with regard to students and postdocs, and in generating funding for research. It also brings up questions of what it means to do attosecond science, and the discovery of the power of X-ray spectroscopy itself, which complements the short timescales addressed. The lessons learned, expressed in the meanderings of this autobiographical article, may be of benefit to others who try to reinvent themselves.

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

Electro-optic characterization of synthesized infrared-visible light fields

The measurement and control of light field oscillations enable the study of ultrafast phenomena on sub-cycle time scales. Electro-optic sampling (EOS) is a powerful field characterization approach, in terms of both sensitivity and dynamic range, but it has not reached beyond infrared frequencies. Here, we show the synthesis of a sub-cycle infrared-visible pulse and subsequent complete electric field characterization using EOS. The sampled bandwidth spans from 700 nm to 2700 nm (428 to 110 THz). Tailored electric-field waveforms are generated with a two-channel field synthesizer in the infrared-visible range, with a full-width at half-maximum duration as short as 3.8 fs at a central wavelength of 1.7 µm (176 THz). EOS detection of the complete bandwidth of these waveforms extends it into the visible spectral range. To demonstrate the power of our approach, we use the sub-cycle transients to inject carriers in a thin quartz sample for nonlinear photoconductive field sampling with sub-femtosecond resolution.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Challenges in the study of chemistry and photochemistry at air–water interfaces: Toward in situ monitoring of reaction kinetics with spectroscopic techniques

Air–water interfaces, including those on droplet surfaces, have been the subject of many recent experiments due to their propensity for unique chemistry. Here, in this study, an overview of some recent advancements in understanding interfacial reaction kinetics is provided, highlighting non-surface-specific methods—such as mass spectrometry—compared with the advantages of surface-specific techniques—such as reflection–absorption spectroscopy, sum frequency generation, and photoelectron spectroscopy. This Perspective discusses the information depth and time constraints of common surface-specific spectroscopic methods that need to be addressed to monitor interfacial chemistry in situ and uses a few key examples from the literature as case studies. It concludes by advocating for the continued development of advanced spectroscopic methods to further investigate interfacial chemistry, underscoring the need for interdisciplinary collaboration to bridge the gap between molecular-level insights and macroscopic observations in future research.

Air-water interface↗
DOE OSTI2020

Tuning time and energy resolution in time-resolved photoemission spectroscopy with nonlinear crystals

Time- and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. In this work, we demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear β-BaB 2 O 4 crystals for frequency upconversion, providing a flexible experiment design. We achieve time resolutions of 58–103 fs and corresponding energy resolutions of 55–27 meV. We propose a method to select crystal thickness based on desired experimental resolutions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Considerations in upconversion: A practical guide to sum-frequency generation spectrometer design and implementation

Here, in this tutorial review, we discuss how the choice of upconversion pulse shape in broadband vibrational sum-frequency generation (SFG) spectrometer design impacts the chemical or physical insights one can obtain from a set of measurements. A time-domain picture of a vibrational coherence being mapped by a second optical field is described and the implications of how this mapping, or upconversion process, takes place are given in the context of several popular and emerging approaches found in the literature. Emphasis is placed on broadband frequency-domain measurements, where the choice of upconversion pulse enhances or limits the information contained in the SFG spectrum. We conclude with an outline for a flexible approach to SFG upconversion using pulse-shaping methods and a simple guide to design and optimize the associated instrumentation.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Towards critical and supercritical electromagnetic fields

Abstract The availability of ever stronger, laser-generated electromagnetic fields underpins continuing progress in the study and application of nonlinear phenomena in basic physical systems, ranging from molecules and atoms to relativistic plasmas and quantum electrodynamics. This raises the question: how far will we be able to go with future lasers? One exciting prospect is the attainment of field strengths approaching the Schwinger critical field ${E}_{\mathrm{cr}}$ in the laboratory frame, such that the field invariant ${E}^2-{c}^2{B}^2>{E}_{\mathrm{cr}}^2$ is reached. The feasibility of doing so has been questioned, on the basis that cascade generation of dense electron–positron plasma would inevitably lead to absorption or screening of the incident light. Here we discuss the potential for future lasers to overcome such obstacles, by combining the concept of multiple colliding laser pulses with that of frequency upshifting via a tailored laser–plasma interaction. This compresses the electromagnetic field energy into a region of nanometre size and attosecond duration, which increases the field magnitude at fixed power but also suppresses pair cascades. Our results indicate that laser facilities with peak power of tens of PW could be capable of reaching ${E}_{\mathrm{cr}}$ . Such a scenario opens up prospects for the experimental investigation of phenomena previously considered to occur only in the most extreme environments in the universe.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Deep learning-assisted modeling for χ (2) nonlinear optics

Modeling second-order (χ(2)) nonlinear optical processes remains computationally expensive due to the need to resolve fast field oscillations and simulate wave propagation using methods such as the split-step Fourier method (SSFM). This can become a bottleneck in real-time applications, such as high-repetition-rate laser systems requiring rapid feedback and control. We present a long short-term memory-based surrogate model trained on SSFM simulations generated from a start-to-end model of the photocathode drive laser at SLAC National Accelerator Laboratory’s Linac Coherent Light Source II. The model achieves over 250× speedup while maintaining high fidelity, enabling future real-time optimization and laying the foundation for data-integrated modeling frameworks and digital twins of laser systems.

Accelerator Physics (physics.acc-ph)↗
DOE OSTI2022

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

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

Perovskite-Derivative Valleytronics

Halide perovskites are revolutionizing the renewable energy sector owing to their high photovoltaic efficiency, low manufacturing cost, and flexibility. Their remarkable mobility and long carrier lifetime are also valuable for information technology, but fundamental challenges like poor stability under an electric field prevent realistic applications of halide perovskites in electronics. Here, it is discovered that valleytronics is a promising route to leverage the advantages of halide perovskites and derivatives for information storage and processing. The synthesized all-inorganic lead-free perovskite derivative, Cs 3 Bi 2 I 9 , exhibits strong light-matter interaction and parity-dependent optically addressable valley degree of freedom. In this work, robust optical helicity in all odd-layer-number crystals with inversion symmetry breaking is observed, indicating excitonic coherence extending well beyond 11 layers. The excellent optical and valley properties of Cs 3 Bi 2 I 9 arise from the unique parallel bands, according to first principles calculations. This discovery points to new materials design principles for scalable valleytronic devices and demonstrates the promise of perovskite derivatives beyond energy applications.

2D materials↗
DOE OSTI2023

Molybdenum Disulfide Nanoribbons with Enhanced Edge Nonlinear Response and Photoresponsivity

MoS 2 nanoribbons have attracted increased interest due to their properties, which can be tailored by tuning their dimensions. Herein, the growth of MoS 2 nanoribbons and triangular crystals formed by the reaction between films of MoOx (2 2 nanoribbons arising from distinct contributions from the single–layer edges and multilayer core. Nanoscale imaging reveals a blue-shifted exciton emission of the monolayer edge compared to the isolated MoS 2 monolayers due to built-in local strain and disorder. We further report on an ultrasensitive photodetector made of a single MoS 2 nanoribbon with a responsivity of 8.72 × 10 2 A W –1 at 532 nm, among the highest reported up-to-date for single-nanoribbon photodetectors. These findings can inspire the design of MoS 2 semiconductors with tunable geometries for efficient optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Chemistry, Structure, and Function of Lone Pairs in Extended Solids

The lone pair has been a known feature of the electronic structure of molecules for over 100 years. Beginning with the pioneering work of Lewis and others that was later developed into useful guidelines for predicting molecular structure, lone pairs and their steric consequences are now taught at the very earliest stages of a chemistry education. In the crystalline solid state, lone pairs have perhaps had a less visible yet equally consequential role, with a significant impact on a range of properties and functionalities. Important properties associated with s 2 electron-derived lone pairs include their role in creating conditions favorable for ion transport, in the formation and correlation of local dipoles and the resulting polar behavior leading to ferroics and multiferroics, in increasing the refractive index of glass, in reducing the thermal conductivity of thermoelectric materials, and in breaking local symmetry permitting second-harmonic light generation.. In recent years, the role of the lone pair in developing the electronic structure of some topological quantum materials has also been recognized. While structural distortions due to lone pairs have traditionally been characterized through their crystallography, recent advances in scattering and spectroscopy have revealed the presence of local lone pair-driven distortions that do not correlate over long length scales. The role of these crystallographically “hidden” lone pairs, their detection, and their impact on properties have become a growing body of work in the literature. Hidden lone pairs are an effective argument for considering a role for lone pairs that goes beyond their being objects that occupy space in the coordination polyhedra of cations. This Account introduces the chemistry of lone pairs in extended crystalline solids, including a discussion of when they are stereochemically active, how they manifest in the structure, and how their chemistry can be tuned by the chemical environment around them. Eventually, all of these factors work in unison to help develop and tune properties of interest. Certain specific examples of structure–property relationships in materials that are driven by lone pair behavior are described here, including the potential impact of lone pairs on the optical and electronic properties of hybrid halide perovskite compounds that are relevant to their photovoltaic applications. Here, we highlight the role of lone pairs in the dielectric behavior of geometrically frustrated pyrochlores, the temperature-dependent optoelectronic behavior of halide perovskites, the polar phase transitions in lead-free ferroelectric perovskites, and the compositional insulator-to-metal transition in ruthenium pyrochlores. The theme underpinning this Account is that the lone pair can be considered to be a powerful design element for a broad range of material function.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Observation of light-driven band structure via multiband high-harmonic spectroscopy

Intense light–matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond timescales, opening routes to the all-optical control of electronic currents in solids at petahertz rates. Such control typically requires electric-field amplitudes in the range of almost volts per angstrom, when the voltage drop across a lattice site becomes comparable to the characteristic bandgap energies. In this regime, intense light–matter interaction induces notable modifications to the electronic and optical properties, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remain an outstanding problem. As the oscillating electric field changes within the driving field’s cycle, does the band structure follow and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe the laser-induced closing of the bandgap between adjacent conduction bands. Our work reveals the link between nonlinear light–matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗