Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “nonlinear optical response”

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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Polar coupling enabled nonlinear optical filtering at MoS 2 /ferroelectric heterointerfaces

Complex oxide heterointerfaces and van der Waals heterostructures present two versatile but intrinsically different platforms for exploring emergent quantum phenomena and designing new functionalities. The rich opportunity offered by the synergy between these two classes of materials, however, is yet to be charted. Here, we report an unconventional nonlinear optical filtering effect resulting from the interfacial polar alignment between monolayer MoS 2 and a neighboring ferroelectric oxide thin film. The second harmonic generation response at the heterointerface is either substantially enhanced or almost entirely quenched by an underlying ferroelectric domain wall depending on its chirality, and can be further tailored by the polar domains. Unlike the extensively studied coupling mechanisms driven by charge, spin, and lattice, the interfacial tailoring effect is solely mediated by the polar symmetry, as well explained via our density functional theory calculations, pointing to a new material strategy for the functional design of nanoscale reconfigurable optical applications.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Interplay between Ultrafast Electronic and Librational Dynamics in Liquid Nitrobenzene Probed with Two-Color Four-Wave Mixing

Here, we present an experimental and theoretical study of the interplay between ultrafast electron dynamics and librational dynamics in liquid nitrobenzene. A femtosecond ultraviolet pulse and two femtosecond near-infrared pulses interact with nitrobenzene molecules, generating a four-wave mixing nonlinear signal measured in the Optical Kerr Effect geometry. The signal is measured to be nonzero only at negative time delays, corresponding to the near-infrared pulses arriving before the ultraviolet pulse. We perform time-dependent Quantum Master Equation calculations with classical libration to simulate the experiment. The simulations support the conclusion that the near-infrared pulses launch librational motion while creating electronic coherences resulting in a libration-modulated electronic nonlinear response. The analysis of the phase-matched four-wave mixing signals suggests a nonparametric process leaving the molecules in an excited electronic state, providing new insight into ultrafast nonlinear optical interactions in liquids and advancing toward probing ultrafast electronic coherences in complex molecular liquids.

Shivaram, Niranjan [Lawrence Berkeley National Lab↗
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 OSTI2024

Enhancement of terahertz fields in LiTaO 3 waveguides using a conical pulse front

The development of methods for the generation of strong ultrafast electromagnetic pulses in the terahertz (THz) spectral range has led to a surge of progress in nonlinear THz spectroscopy and THz control of molecular and collective responses. For spectroscopy in the 1-THz range, the submillimeter wavelengths and associated large spot sizes, large optical elements, and short distances between final focusing elements and samples can lead to cumbersome experimental setups that are incompatible with some sample environments. Here, we introduce a novel terahertz ring excitation (TREx) optical pumping geometry to generate superposing, focusing fields in planar THz waveguides made out of the electro-optic material lithium tantalate. High THz fields, >175 kV/cm, are generated and measured optically with no free-space THz propagation. The field level achieved by pumping with a sequence of concentric rings of excitation light exceeds by about 20× the result of a single cylindrically focused line of pump light that has been used routinely in previous work. The technique opens new prospects for compact waveguide-based linear and nonlinear THz spectroscopy and signal processing.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Light-induced electronic polarization in antiferromagnetic Cr 2 O 3

In a solid, the electronic subsystem can exhibit incipient order with lower point group symmetry than the crystal lattice. Ultrafast external fields that couple exclusively to electronic order parameters have rarely been investigated, however, despite their potential importance in inducing exotic effects. Here we show that when inversion symmetry is broken by the antiferromagnetic order in Cr 2 O 3 , transmitting a linearly polarized light pulse through the crystal gives rise to an in-plane rotational symmetry-breaking (from C 3 to C 1 ) via optical rectification. Using interferometric time-resolved second harmonic generation, we show that the ultrafast timescale of the symmetry reduction is indicative of a purely electronic response; the underlying spin and crystal structures remain unaffected. The symmetry-broken state exhibits a dipole moment, and its polar axis can be controlled with the incident light. Furthermore, our results establish a coherent nonlinear optical protocol by which to break electronic symmetries and produce unconventional electronic effects in solids.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Giant Modulation of Refractive Index from Picoscale Atomic Displacements

Abstract It is shown that structural disorder—in the form of anisotropic, picoscale atomic displacements—modulates the refractive index tensor and results in the giant optical anisotropy observed in BaTiS 3 , a quasi‐1D hexagonal chalcogenide. Single‐crystal X‐ray diffraction studies reveal the presence of antipolar displacements of Ti atoms within adjacent TiS 6 chains along the c ‐axis, and threefold degenerate Ti displacements in the a – b plane. 47/49 Ti solid‐state NMR provides additional evidence for those Ti displacements in the form of a three‐horned NMR lineshape resulting from a low symmetry local environment around Ti atoms. Scanning transmission electron microscopy is used to directly observe the globally disordered Ti a–b plane displacements and find them to be ordered locally over a few unit cells. First‐principles calculations show that the Ti a – b plane displacements selectively reduce the refractive index along the ab ‐plane, while having minimal impact on the refractive index along the chain direction, thus resulting in a giant enhancement in the optical anisotropy. By showing a strong connection between structural disorder with picoscale displacements and the optical response in BaTiS 3 , this study opens a pathway for designing optical materials with high refractive index and functionalities such as large optical anisotropy and nonlinearity.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Direct Measurement of Helicoid Surface States in RhSi Using Nonlinear Optics

Despite the fundamental nature of the edge state in topological physics, direct measurement of electronic and optical properties of the Fermi arcs of topological semimetals has posed a significant experimental challenge, as their response is often overwhelmed by the metallic bulk. However, laser-driven currents carried by surface and bulk states can propagate in different directions in nonsymmorphic crystals, allowing for the two components to be easily separated. Motivated by a recent theoretical prediction G. Chang et al., Phys. Rev. Lett. 124, 166404 (2020), we have measured the linear and circular photogalvanic effect currents deriving from the Fermi arcs of the nonsymmorphic, chiral Weyl semimetal RhSi over the 0.45-1.1 eV incident photon energy range. Our data are in good agreement with the predicted spectral shape of the circular photogalvanic effect as a function of photon energy, although the direction of the surface photocurrent departed from the theoretical expectation over the energy range studied. In conclusion, surface currents arising from the linear photogalvanic effect were observed as well, with the unexpected result that only two of the six allowed tensor element were required to describe the measurements, suggesting an approximate emergent mirror symmetry inconsistent with the space group of the crystal.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Above-threshold multiphoton photoemission from noble metal surfaces

Exciting solids with intense femtosecond laser pulses prompts electrons of the interrogated material to respond in a highly nonlinear manner, as is evident in the emission of high-order harmonic radiation and photoelectrons with kinetic energies well above that of the driving photons. Such high-field interactions can be resolved, for example, in above-threshold multiphoton photoemission (ATP) spectroscopy. In this work, we interrogate the nonlinear photoelectric responses of the pristine copper, silver, and gold noble metal surfaces in (111) and (100) crystal orientations in the perturbative regime. Using multiphoton photoemission spectroscopy (mPP) excited by finely tuned optical fields, we characterize enhancement of the mPP and ATP yields from (111) surfaces in selected k||-momentum ranges when the occupied Shockley surface (SS) states are (near-)resonantly coupled by multiphoton transitions to image potential (IP) intermediate states in the excitation process. The ATP signal from the IP states of (111) surfaces is largely defined by their formation through polarization of SS electrons; this observation is contrasted with ATP experiments from the Ag(100) surface, for which the SS becomes an unoccupied resonance and the IP states can only be excited from bands with significantly more bulk character. In addition, based on the optical power and nonlinear order-dependent mPP spectra, we provide evidence for ATP being a one-step, rather than a sequential process, as previously postulated.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Transparent conducting oxides: from all-dielectric plasmonics to a new paradigm in integrated photonics

During the past few years, the optics and photonics communities have renewed their attention toward transparent conducting oxides (TCOs), which for over two decades have been broadly employed for the fabrication of transparent electrodes in photovoltaic and communication technologies. This reinvigorated research curiosity is twofold: on the one hand, TCOs, with their metal-like properties, low optical absorption, and fabrication flexibility, represent an appealing alternative to noble metals for designing ultra-compact plasmonic devices. On the other hand, this class of hybrid compounds has been proved to possess exceptionally high optical nonlinearities when operating on a frequency window centered around their crossover point, the wavelength point at which the real part of the dielectric permittivity switches sign. Because TCOs are wide-bandgap materials with the Fermi level located in the conduction band, they are hybrid in nature, thus presenting both interband and intraband nonlinearities. This is the cause of a very rich nonlinear physics that is yet to be fully understood and explored. In addition to this, TCOs are epsilon-near-zero (ENZ) materials within a broad near-infrared spectral range, including the entire telecom bandwidth. In this operational window a myriad of novel electromagnetic phenomena have been demonstrated experimentally such as supercoupling, wavefront freezing, and photon doping. Furthermore, TCOs stand out among all other ENZ systems due to one fundamental characteristic, which is hardly attainable even by using structured materials. In fact, around their ENZ wavelength and for a quite generous operational range, these materials can be engineered to have an extremely small real index. This peculiarity leads to a slow-light effect that is ultimately responsible for a significant enhancement of the material nonlinear properties and is the cornerstone of the emerging field of near-zero-index photonics. In this regard, the recent history of nonlinear optics in conductive oxides is growing extremely fast due to a great number of experiments reporting unprecedentedly remarkable effects, including unitary index change, bandwidth-large frequency shift, efficient ultra-low-power frequency conversion, and many others. This review is meant to guide the reader through the exciting journey of TCOs, starting as an industrial material for transparent electrodes, then becoming a new alternative for low-loss plasmonics, and recently opening up new frontiers in integrated nonlinear optics. The present review is mainly focused on experimental observations.

42 ENGINEERING↗
DOE OSTI2021

Vibronic and Environmental Effects in Simulations of Optical Spectroscopy

Including both environmental and vibronic effects is important for accurate simulation of optical spectra, but combining these effects remains computationally challenging. We outline two approaches that consider both the explicit atomistic environment and the vibronic transitions. Both phenomena are responsible for spectral shapes in linear spectroscopy and the electronic evolution measured in nonlinear spectroscopy. The first approach utilizes snapshots of chromophore-environment configurations for which chromophore normal modes are determined. We outline various approximations for this static approach that assumes harmonic potentials and ignores dynamic system-environment coupling. The second approach obtains excitation energies for a series of time-correlated snapshots. This dynamic approach relies on the accurate truncation of the cumulant expansion but treats the dynamics of the chromophore and the environment on equal footing. Both approaches show significant potential for making strides toward more accurate optical spectroscopy simulations of complex condensed phase systems.

Chemistry↗
DOE OSTI2024

High Field Transport in (Ultra) Wide Bandgap Semiconductors: Diamond Versus Cubic GaN

We provide an analysis of nonlinear transport in diamond and cubic GaN (c-GaN) with emphasis on the different types of optical phonon scattering [i.e., optical deformation potential (ODP) scattering versus polar optic phonon (POP) scattering] limiting the carrier velocity. Both types of carrier mobilities and carrier saturation (peak) velocities in diamond and c-GaN as functions of different doping types and concentrations are obtained by directly solving the Boltzmann equation. Our model indicates that the nonrandomizing nature of POP scattering causes carrier temperature cooling, resulting in higher carrier drift velocity than with ODP scattering. This effect, in addition to the small carrier effective masses and large optical phonon energies, is responsible for the higher peak velocities in c-GaN, compared to carrier drift velocity in diamond.

42 ENGINEERING↗
DOE OSTI2024

TRUST Sensors in Environments: Fiber Optic Displacement (SE-FOD) Report, Release FY24

The objective of the Delivery Environments (DE) Testbeds to Reduce Uncertainty in Simulations and Tests (TRUST) project is to quantify and help increase confidence in specific areas of computational and experimental capabilities that are applicable to the development, on-target assessment, and qualification of current and future delivery environments. More complete quantification of confidence in experimental and computational capabilities and the sufficient increase of confidence in those capabilities is critical to improving weapons engineering design, qualification, and assessment efforts that are critical to the current and future stockpile. This work uses and provides feedback on analysis tools and experimental results databases for efficient and responsive engineering which are currently under development. Under the TRUST work package, there are five testbeds and their associated engineering analysis baseline models (EABMs): 1. Contact Thermal Conductivity (CTC), 2. Nonlinear Dynamics (ND), 3. Sensors in Environments: Accelerometers (SE-A), 4. Sensors in Environments: Fiber Optic Displacement Gauges (SE-FOD), and 5. Sensors in Environments: Thermocouples (SE-TC). The TRUST project uses single-feature testbeds to quantify uncertainties in specific models and experiments and to identify capability development needs that can help to reduce these uncertainties. Each testbed is designed, configured, and tested in collaboration with groups with design and experimental capability: E-14 and MPA-CINT. The complementary simulations are conducted using W-13 analysis tools and stored in model repositories with plans for incremental progress toward EABM requirements. W-13 extends and exercises the testbed simulations in collaboration with experimentalists for uncertainty quantification of current and future materials, geometries, and environments. Additionally, TRUST is intended to provide engineers in W-13 and E-14 with experience in both numerical simulations and experimental methods through cross-discipline collaborations. Following the introduction to the TRUST project, the remainder of this report focuses on experimental, modeling and simulation, and analysis efforts conducted in FY24 relevant to the TRUST Sensors in Environments: Fiber Optic Displacement (SE-FOD) testbed.

42 ENGINEERING↗
DOE OSTI2021

Plasmonically assisted channels of photoemission from metals

We analyze recently measured nonlinear photoemission spectra from Ag surfaces that reveal resonances whose energies do not scale with the applied photon energy but stay pinned to multiples of bulk plasmon energy $\hbar$ω p above the Fermi level. To elucidate these unexpected and peculiar features we investigate the spectra of plasmons generated in a solid by the optically pumped electronic polarization and their effect on photoemission. By combining quadratic response formalism for calculations of photoemission yield, a nonperturbative approach to inelastic electron scattering, and first-principles calculations for the electronic structure, we demonstrate the dependence of probability amplitude for single- and multiplasmon excitations on the basic parameters characterizing the photon pulse and the system. The resulting multiexcitation spectrum evolves towards a truncated plasmonic coherent state. Analogous concept is extrapolated to interpret plasmon generation by multiphoton excited electronic polarization. Based on this we elaborate a scenario that the thus created real plasmons act as supplementary frequency-locked pump field for non-Einsteinian plasmonically assisted channels of photoemission from metals. The established paradigm enables assignment and assessment of the observed linear $\hbar$ω p and nonlinear 2$\hbar$ω p electron yields from Ag. Such effects may be exploited for selective filtering of optical energy conversion in electronic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Nonlinear Optical Microscopy with Ultralow Quantum Light

Nonlinear optical (NLO) microscopy relies on multiple light–matter interactions to provide unique contrast mechanisms and imaging capabilities that are inaccessible to traditional linear optical imaging approaches, making them versatile tools to understand a wide range of complex systems. However, the strong excitation fields that are necessary to drive higher-order optical processes efficiently are often responsible for photobleaching, photodegradation, and interruption in many systems of interest. This is especially true for imaging living biological samples over prolonged periods of time or in accessing intrinsic dynamics of electronic excited-state processes in spatially heterogeneous materials. This perspective outlines some of the key limitations of two NLO imaging modalities implemented in our lab and highlights the unique potential afforded by the quantum properties of light, especially entangled two-photon absorption based NLO spectroscopy and microscopy. Here, we further review some of the recent exciting advances in this emerging filed and highlight some major challenges facing the realization of quantum-light-enabled NLO imaging modalities.

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

Birefringence axis rotation and nonlinear response of a side-hole fiber pressure sensor

The pressure-induced birefringence of side-hole fibers has been widely explored for hydrostatic pressure measurement. Here, this paper studies the effects of the initial birefringence of a side-hole fiber on the pressure response of polarimetric sensors based on side-hole fibers. A mathematical model, where the stress field induced by the pressure is assumed to be uniform in the core region of the fiber, was established to calculate the birefringence and optical axis rotation as a function of the differences between the two principal stress components of the stress field in the core region. Simulation results show that when there is misalignment between the initial birefringence axes and the principal axes of the stress field, pressure changes cause rotations of the birefringence axis, leading to complicated and nonlinear changes of birefringence as a function of pressure. Experiments were conducted using fiber-Bragg-grating-based resonators on side-hole fibers with different initial birefringence, and the results agree well with the simulation. The results underscore the importance of the control of magnitude and direction of the initial birefringence of the side-hole fiber and provide guidelines for the design and fabrication of side-hole fiber pressure sensors.

42 ENGINEERING↗
DOE OSTI2025

Optomechanical Tuning of Second Harmonic Generation Anisotropy in Janus MoSSe/MoS 2 Heterostructures

Symmetry breaking in van der Waals materials enables the realization of quantum states and advanced device functionalities. Janus transition-metal dichalcogenides (TMDs) exhibit distinctive nonlinear optical properties due to their broken out-of-plane mirror symmetry. However, the dynamic control of second harmonic generation (SHG) anisotropy and resonance behavior via optical excitation remains elusive. Here, in this work, we investigate the SHG response of Janus MoSSe/MoS 2 heterostructures with 2H and 3R stackings. We can tune the SHG response by varying the incident photon wavelength from 800 to 1000 nm, which shows a resonance-dependent enhancement in intensity and a deviation from 6-fold symmetry, indicating wavelength-dependent anisotropy. The ratio between maximum and minimum intensity in the armchair directions, associated with the SHG anisotropy, reaches a value of 1.73 at the excitation wavelength of 1000 nm. Group theory analysis and first-principles calculations reveal that the observed anisotropy arises from optically induced strain. Our findings highlight the role of symmetry breaking and optical resonance contributing to the optomechanical tuning of SHG anisotropy, offering opportunities for developing Janus TMD-based photonic devices for frequency conversion, light generation, and optical switching.

Janus transition metal dichalcogenides↗
DOE OSTI2025

Simulating quantum-classical interfaces via the Lindblad master equation

In hybrid quantum systems, the interface between quantum and classical domains is essential for the generation, control, and measurement of quantum states. Quantum-classical interfaces (QCIs) are ubiquitous in devices such as optical modulators, quantum sensors, and signal processors, where classical signals influence quantum dynamics. In this paper, we employ the Lindblad master equation to simulate the evolution of a quantum system interacting with a classical control system. Our model captures both linear and nonlinear interactions by incorporating first- and second-order susceptibilities, and it quantifies the influence of externally applied control parameters on decoherence and state evolution. As an illustrative example, we analyze an optical modulator and demonstrate how variations in material response and drive conditions affect photon statistics, coherence, and phase-space distributions. In conclusion, the findings offer a path to an all-encompassing model for understanding and optimizing QCIs, with wide-ranging implications for the performance, design, and robustness of next-generation quantum devices.

Quantum engineering↗
DOE OSTI2022

Multifunctional Cu 2 TSiS 4 (T = Mn and Fe): Polar Semiconducting Antiferromagnets with Nonlinear Optical Properties

In this work, Cu 2 TSiS 4 (T = Mn and Fe) polycrystalline and single-crystal materials were prepared with high-temperature solid-state and chemical vapor transport methods, respectively. The polar crystal structure (space group Pmn2 1 ) consists of chains of corner-sharing and distorted CuS 4 , Mn/FeS 4 , and SiS 4 tetrahedra, which is confirmed by Rietveld refinement using neutron powder diffraction data, X-ray single-crystal refinement, electron diffraction, energy-dispersive X-ray spectroscopy, and second harmonic generation (SHG) techniques. Magnetic measurements indicate that both compounds order antiferromagnetically at 8 and 14 K, respectively, which is supported by the temperature-dependent (100–2 K) neutron powder diffraction data. Additional magnetic reflections observed at 2 K can be modeled by magnetic propagation vectors k = (1/2,0,1/2) and k = (1/2,1/2,1/2) for Cu 2 MnSiS 4 and Cu 2 FeSiS 4 , respectively. The refined antiferromagnetic structure reveals that the Mn/Fe spins are canted away from the ac plane by about 14°, with the total magnetic moments of Mn and Fe being 4.1(1) and 2.9(1) μ B , respectively. Both compounds exhibit an SHG response with relatively modest second-order nonlinear susceptibilities. Density functional theory calculations are used to describe the electronic band structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗