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At least 397 records · Page 22

All sources NASA NTRS DOE OSTI

DOE OSTI2023

Intrinsic 1${T}^{{\prime} }$ phase induced in atomically thin 2 H -MoTe 2 by a single terahertz pulse

The polymorphic transition from 2H to 1${T}^{{\prime} }$-MoTe 2 , which was thought to be induced by high-energy photon irradiation among many other means, has been intensely studied for its technological relevance in nanoscale transistors due to the remarkable improvement in electrical performance. However, it remains controversial whether a crystalline 1${T}^{{\prime} }$ phase is produced because optical signatures of this putative transition are found to be associated with the formation of tellurium clusters instead. Here we demonstrate the creation of an intrinsic 1${T}^{{\prime} }$ lattice after irradiating a mono- or few-layer 2H-MoTe 2 with a single field-enhanced terahertz pulse. Unlike optical pulses, the low terahertz photon energy limits possible structural damages. We further develop a single-shot terahertz-pump-second-harmonic-probe technique and reveal a transition out of the 2H-phase within 10 ns after photoexcitation. Our results not only provide important insights to resolve the long-standing debate over the light-induced polymorphic transition in MoTe 2 but also highlight the unique capability of strong-field terahertz pulses in manipulating quantum materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Nonlinear quantum behavior of ultrashort-pulse optical parametric oscillators

The quantum features of ultrashort-pulse optical parametric oscillators (OPOs) are investigated theoretically in the nonlinear regime near and above threshold. Viewing the pulsed OPO as a multimode open quantum system, we rigorously derive a general input-output model that features nonlinear coupling among many cavity (i.e., system) signal modes and a broadband single-pass (i.e., reservoir) pump field. Under appropriate assumptions, our model produces a Lindblad master equation with multimode nonlinear Lindblad operators describing two-photon dissipation and a multimode four-wave-mixing Hamiltonian describing a broadband, dispersive optical cascade, which we show is required to preserve causality. To simplify the multimode complexity of the model, we employ a supermode decomposition to perform numerical simulations in the regime where the pulsed supermodes experience strong single-photon nonlinearity. We find that the quantum nonlinear dynamics induces pump depletion as well as corrections to the below-threshold squeezing spectrum predicted by linearized models. We also observe the formation of non-Gaussian states with Wigner-function negativity and show that the multimode interactions with the pump, both dissipative and dispersive, can act as effective decoherence channels. Finally, we briefly discuss some experimental considerations for potentially observing such quantum nonlinear phenomena with ultrashort-pulse OPOs on nonlinear nanophotonic platforms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Optically and thermally driven huge lattice orbital and spin angular momenta from spinning fullerenes

Lattice vibration in solids may carry angular momentum. But unlike the intrinsic spin of electrons, the lattice vibration is rarely rotational. To induce angular momentum, one needs to find a material that can accommodate a twisted normal mode, two orthogonal modes, or excitation of magnons. If excitation is too strong, one may exceed the Lindemann limit, so the material melts. Therefore these methods are not ideal. Here, we theoretically propose a route to phonon angular momentum in a molecular crystal C 60 . We find that a single laser pulse is able to inject a significant amount of angular momentum to C 60 , and the momentum transfer is helicity dependent. Changing from right-circularly polarized light to left-circularly polarized light switches the direction of phonon angular momentum. On the ultrafast timescale, the orbital angular momentum change closely resembles the displacive excitation of coherent phonons, with a cosine-function dependence on time, different from the spin counterpart. Atomic displacements, even under strong laser excitation, remain far below the Lindemann criterion. Under thermal excitation, spinning C 60 even at room temperature generates a huge angular momentum close to several hundred hÂ¯. Our finding opens the door to a large group of fullerenes, from C 60 , C 70 to their endohedral derivatives, where angular momentum can be generated through light or temperature. Furthermore, this paves the way to the phononic control electronic spin and harvesting thermal energy through phonon angular momentum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Coherent Combining for High‐Power Kerr Combs

Abstract Kerr frequency combs enable the miniaturization of comb sources for applications such as data communications and spectroscopy. However, due to the high field confinement and effective nonlinearity, Kerr combs typically operate with low output comb powers. While nonsolitonic Kerr combs operating in the normal group velocity dispersion (GVD) regime can access high pump‐to‐comb conversion efficiencies and relatively flat spectral profiles, many frequency comb applications require even higher comb‐line powers that are otherwise fundamentally unattainable without the use of optical amplifiers. A high efficient coherent beam combining of Kerr combs is demonstrated via on‐chip synchronization to greatly enhanced comb‐line powers. Two normal GVD Kerr combs are coherently combined for a 2.9 dB increase in comb power compared to a single comb while maintaining a high total pump‐to‐comb conversion efficiency of 26%. Lastly, it is shown that via spectral engineering of two normal GVD combs, it should be possible to significantly increase the spectral flatness of a combined comb. This platform enables fully integrated systems with powers that can readily exceed that of an individual comb system by more than an order of magnitude.

Kim, Bok Young↗

DOE OSTI2025

Resolving the phase of Fano resonance wave packets with photoelectron frequency-resolved optical gating

The creation of structured electronic wave packets (EWPs) energetically close to Fano resonances has been achieved with ultrafast extreme ultraviolet coherent light sources. However, direct real-time observations of EWP evolution and full reconstructions of the quantum properties of EWPs, including both amplitude and phase, are lacking. Here we introduce and demonstrate a comprehensive approach for the direct measurement and complete characterization of structured EWPs created within a prototypical Fano resonance. Because of its analogy with frequency-resolved optical gating (FROG), we named the method photoelectron FROG. The correlated EWP is initiated by a carefully engineered extreme UV pump pulse. A weak near-infrared laser field, serving as a probe pulse, samples the evolution of the EWPs in the time domain, as well as in the frequency domain. The amplitude and phase of the EWPs are obtained via a time-dependent reconstruction algorithm based on a short-time Fourier transformation. Given the excellent agreement between our experimental results and time-dependent reconstructions, we expect this method to be broadly applicable to the study of ultrafast processes, especially electronic ones, in complex systems, as well as the coherent control of such systems on their fundamental timescales.

quantum optics↗

DOE OSTI2020

Gain balanced nonlinear optical interferometer

A nonlinear fiber interferometer is disclosed suitable for fiber sensor and other applications. A first nonlinear fiber section amplifies probe and conjugate sidebands of a pump through four-wave mixing. A second section introduces a phase shift to be measured, for example from a sensor. A third nonlinear fiber section amplifies with phase-sensitive gain to increase signal-to-noise ratio. Based on phase-sensitive output power of probe and/or conjugate components, the phase shift can be measured. Superior performance can be obtained by balancing gain between the (first and third) nonlinear sections. Non-fiber, for example photonic integrated circuit, embodiments are disclosed. Differential sensing, alternative detection schemes, sensing applications, associated methods, and other variations are disclosed.

42 ENGINEERING↗

DOE OSTI2022

Gain balanced nonlinear optical interferometer

Lukens, Joseph M.↗

DOE OSTI2023

Gain balanced nonlinear optical interferometer

Lukens, Joseph M.↗

DOE OSTI2024

Spatiotemporal dispersion compensation for a 200-THz noncollinear optical parametric amplifier

A noncollinear optical parametric amplifier (NOPA) can produce few-cycle femtosecond laser pulses that are ideally suited for time-resolved optical spectroscopy measurements. However, the nonlinear-optical process giving rise to ultrabroadband pulses is susceptible to spatiotemporal dispersion problems. Here, we detail refinements, including chirped-pulse amplification (CPA) and pulse-front matching (PFM), that minimize spatiotemporal dispersion and thereby improve the properties of ultrabroadband pulses produced by a NOPA. Here, the description includes a rationale behind the choices of optical and optomechanical components, as well as assessment protocols. We demonstrate these techniques using a 1 kHz, second-harmonic Ti:sapphire pump configuration, which produces ~5-fs duration pulses that span from about 500 to 800 nm with a bandwidth of about 200 THz. To demonstrate the utility of the CPA-PFM-NOPA, we measure vibrational quantum beats in the transient–absorption spectrum of methylene blue, a dye molecule that serves as a reference standard.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Toward quantum networking with frequency-bin qudits

Quantum networking holds tremendous promise in transforming computation and communication. Entangled-photon sources are critical for quantum repeaters and networking, while photonic integrated circuits are vital for miniaturization and scalability. In this talk, we focus on generating and manipulating frequency-bin entangled states within integrated platforms. We encode quantum information as a coherent superposition of multiple optical frequencies; this approach is favorable due to its amenability to high-dimensional entanglement and compatibility with fiber transmission. We successfully generate and measure the density matrix of biphoton frequency combs from integrated silicon nitride microrings, fully reconstructing the state in an 8 × 8 two-qudit Hilbert space, the highest so far for frequency bins. Moreover, we employ Vernier electro-optic phase modulation methods to perform time-resolved measurements of biphoton correlation functions. Currently, we are exploring bidirectional pumping of microrings to generate indistinguishable entangled pairs in both directions, aiming to demonstrate key networking operations such as entanglement swapping and Greenberger–Horne–Zeilinger state generation in the frequency domain.

Myilswamy, Karthik V.↗

DOE OSTI2021

Radiative Heat Transport and Optical Characterization of High Temperature Molten Salts

The goal of this project was to advance the field of molten fluoride radiative heat transfer (RHT), through optical property measurements, heat transfer loop construction and operation, and computational fluid dynamics simulations. The following outcomes have been accomplished. A comprehensive review has been conducted to compile all available RHT-relevant optical absorption data for molten fluorides. The various measurement methods have also been compiled and critiqued. Thermal emission measurement methods have been refined and documented. A unique thermal emissivity measurement facility has been constructed and used to measure the emissivity of flowing FLiBe-exposed SS316 samples. A slight increase has been observed in the emissivity compared to unexposed SS316. A dual reflectance-emission setup was partially demonstrated for the purpose of molten fluoride absorption measurement. Preliminary infrared edge data for FLiNaK was obtained. A visible near-infrared (NIR) measurement setup has been constructed and will be used to measure absorption of corrosion products in FLiBe. A new multi-band thermal radiation method using blackbody-weighted spectral bands for the absorption-coefficient was deployed to investigate the thermal performance of the UW Natural Circulation FLiBe Loop under various power levels and operating conditions. The results showed an increasing and decreasing trend in the overall heat transfer with optical thickness with a maximum at optical thickness τ D ≈Ο(1). A forced convection FLiBe loop was constructed for the purpose of studying corrosion and thermal hydraulic phenomena. A vertical cantilever pump is used to achieve up to 5 gpm and 5 m/s flow velocity in hot and cold test sections. A methodology has been established for modeling radiative heat transfer (RHT) in molten salt coolants for the purpose of quantifying the contribution of thermal radiation in conditions relevant to FHR or MSR systems. The comparison between the results obtained for forced and mixed convection showed that in the studied ranges of optical thickness, the maximum effect of RHT on overall heat transfer was 60% improvement observed at z/D = 250 for forced convection; whereas for mixed convection, that value was higher at 170% observed at z/D = 30. The highest effect of RHT on the overall energy distribution was observed at τ D ≈3.4. Negligible effect (<20%) was observed above τ D =18 and below τ D ≈0.002. A CFD code-to-code comparison was conducted using COMSOL Multiphysics at UW-Madison and STAR-CCM at MIT, for a forced and mixed convection laminar flow for a grey medium in a vertical heated using both COMSOL Multiphysics at UW-Madison and STAR-CCM at MIT. The relative error was the largest at τ D =40 for the radiative heat flux, bulk temperature, and Nusselt number. On the other hand, the relative error was the least at τ D =0.002 for the conductive heat flux, bulk temperature, and Nusselt number.

Anderson, Mark↗

DOE OSTI2025

Predictable third harmonic generation in GaAs metasurfaces through group theory inverse design of meta-atoms

Here we report the group theory-based inverse design of meta-atoms for a dielectric metasurface in GaAs with predictable optical linear response and third harmonic generation (THG). Six sharp Fano resonances have been observed with a corresponding polarization dependence as predicted by group theory and the meta-atom’s symmetry in the D2h point group. THG has been observed for two modes under x-polarization excitation and one mode for y-polarization, in agreement with theoretical symmetry predictions. The polarization-dependent THG aspect ratio was observed to reach as high as 108. Through strategic structural or symmetry-preserving perturbations, it was shown that the THG can be enhanced or reduced by a factor of 7. The highest THG conversion efficiency was estimated to be 3.1×10-7 at the pump intensity of 1.51 MW/cm2. This high THG conversion efficiency indicates that our group theory approach to modal engineering opens a new path towards optical nonlinearity tuning in dielectric metasurfaces.

Aoueille, Andrew↗

DOE OSTI2021

Adaptive four-level modeling of laser cooling of solids

Laser cooling of rare-earth doped solids has been demonstrated across a wide range of material platforms, inspiring the development of simple phenomenological models such as the four-level model to elucidate the universal properties of laser cooling under various operating conditions. However, these models usually require the input of full absorption spectra that must be provided experimentally or by additional complicated atomic modeling. In this Letter, we propose that a four-level model, when extended to admit effective energy levels adaptive to the pumping photon energy, can accurately predict the cooling efficiency as a function of temperature and pumping frequency using only few inputs such as the absorption coefficient measured at a single frequency and temperature. Our model exploits the quasi-equilibrium properties of the excitation of rare-earth ions for the determination of the effective four energy levels. The model is validated against published experimental results for a span of materials including ytterbium/thulium-doped glass and crystals. With the verified model, we derive explicit expressions for the optimal frequency and the operating bandwidth of pumping lasers. Our model significantly simplifies the modeling process of laser cooling and is expected to stimulate further development of optical refrigeration.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

The Recent Improvements of the SNS Extraction Kicker Power Supplies

A total of 14 extraction kickers., with one as the hot spare., are in service to extract protons out of the storage ring at the SNS. The jitter issue and the short lifetime of the switches were resolved after the thyratrons were replaced with solid state switches in 2018. This paper discusses the recent improvements. Two thyristor switches suffered overheating damage in separate incidents. One was due to the oil pump failure and the other was the result of a disconnected oil hose. An ultrasonic flow meter and a fiber optic temperature monitoring system have been installed for each extraction kicker power supply. The flow meter continuously monitors the entire tank oil flow. The temperature monitor detects the thyristor switch real-time temperatures in three locations. Fault thresholds are selected so that the thyristor switches are protected from overheating damage. Alarms are configured to alert staff to take actions before faults occur. In addition., the cause of an intermittent misfire issue was identified, and the solution was implemented. Lastly., a future oscilloscope upgrade and an oil level sensor are discussed.

Tan, Yugang↗

DOE OSTI2020

Broad Frequency Shift of Parametric Processes in Epsilon-Near-Zero Time-Varying Media

The ultrafast changes of material properties induced by short laser pulses can lead to a frequency shift of reflected and transmitted radiation. Recent reports highlight how such a frequency shift is enhanced in spectral regions where the material features a near-zero real part of the permittivity. Here, we investigate the frequency shift for fields generated by four-wave mixing. In our experiment, we observed a frequency shift of more than 60 nm (compared to the pulse width of ~40 nm) in the phase conjugated radiation generated by a 500 nm aluminium-doped zinc oxide (AZO) film pumped close to the epsilon-near-zero wavelength. Our results indicate applications of time-varying media for nonlinear optics and frequency conversion.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Optical control of ultrafast structural dynamics in a fluorescent protein

The photoisomerization reaction of a fluorescent protein chromophore occurs on the ultrafast timescale. The structural dynamics that result from femtosecond optical excitation have contributions from vibrational and electronic processes and from reaction dynamics that involve the crossing through a conical intersection. The creation and progression of the ultrafast structural dynamics strongly depends on optical and molecular parameters. When using X-ray crystallography as a probe of ultrafast dynamics, the origin of the observed nuclear motions is not known. Now, high-resolution pump–probe X-ray crystallography reveals complex sub-ångström, ultrafast motions and hydrogen-bonding rearrangements in the active site of a fluorescent protein. However, we demonstrate that the measured motions are not part of the photoisomerization reaction but instead arise from impulsively driven coherent vibrational processes in the electronic ground state. A coherent-control experiment using a two-colour and two-pulse optical excitation strongly amplifies the X-ray crystallographic difference density, while it fully depletes the photoisomerization process. A coherent control mechanism was tested and confirmed the wave packets assignment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Long-Lived Population Inversion in Resonantly Driven Excitonic Antiferromagnet

Van der Waals magnets are an emerging material family for investigating light-matter interactions and spin-correlated excitations. Here, we report the discovery of a photo-induced state with a lifetime of 17 ps in the van der Waals antiferromagnet NiPS 3 , which appears exclusively with resonant pumping at 1.476 eV in the antiferromagnetic state. Furthermore, the long-lived state comes with a negative photoconductivity, a characteristic optical response of population inversion. Our findings demonstrate a promising pathway to potentially achieve long-lived lasing at terahertz frequencies in reduced dimensions.

36 MATERIALS SCIENCE↗

DOE OSTI2021

On-chip non-Hermitian optical parametric amplifiers with a large bandwidth

Recently, our groups have introduced the notion of optical parametric amplification based on non-Hermitian phase matching wherein the incorporation of loss can lead to gain in this nonlinear optical process. Previous simulation results using second-order nonlinear optical coupled-mode theory have demonstrated the potential of this technique as an alternative to the stringent phase-matching condition, which is often difficult to achieve in semiconductor platforms. Here we fortify this notion for the case of third-order nonlinearity by considering parametric amplification in silicon nanowires and illustrate the feasibility of these devices by employing rigorous finite-difference time-domain analysis using realistic materials and geometric parameters. Particularly, we demonstrate that by systematic control of the optical loss of the idler in a four-wave mixing process, we can achieve efficient unidirectional energy conversion from the pump to the signal component even when the typical phase-matching condition is violated. Importantly, our simulations show that a signal gain of ∼ <#comment/> 9 d B for a waveguide length of a few millimeters is possible over a large bandwidth of several hundreds of nanometers ( ∼ <#comment/> 600 n m ). This bandwidth is nearly 2 orders of magnitude larger than what can be achieved in the conventional silicon-photonics-based four-wave mixing process.

Ahmed, Asif (ORCID:0000000152234392)↗