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At least 73 records · Page 4

Spectroscopy of Degenerate One-Dimensional Electrons in Carbon Nanotubes (Final Report)

The goal of this research program was to understand the fundamental properties of degenerate one-dimensional (1-D) electrons in single-wall carbon nanotubes (SWCNTs). SWCNTs provide an ideal 1-D environment in which to study many-body physics. Semiconducting SWCNTs exhibit rich optical spectra dominated by extremely stable 1-D excitons, whereas metallic SWCNTs contain massless 1-D carriers with ultralong mean-free paths. Despite the large number of electrical, optical, and magnetic studies of SWCNTs during the last two decades, most of the predicted exotic properties of interacting 1-D electrons have yet to be observed, and some reported experimental results remain highly controversial. Here, we report on our research projects for the last 16 years summarizing spectroscopy on SWCNTs using an arsenal of spectroscopic methods from the terahertz to the visible spectral range, including ultrafast optical spectroscopy and ultrahigh magnetic fields. These studies provided a wealth of new insights into the nature of strongly correlated carriers in the ultimate 1-D limit that will lead to novel nanodevice concepts and implementations. Particular emphasis was placed on dynamical 1-D phenomena in the terahertz, infrared, and optical frequency ranges. Because SWCNTs are direct-band-gap materials, they are one of the leading candidates to unify electronic and optical functions in nanoscale circuits and elucidate how electron correlations can affect and control finite-frequency phenomena in 1-D systems. As a result, we have published 78 research articles (Web of Science), including ten reviews and book volumes/chapters. Below, we highlight and summarize several accomplishments that provided new insights into the fundamental properties of1-D carriers, excitons, and phonons of SWCNTs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Light-induced microwave noise in superconducting microwave-optical transducers

Microwave-to-optical transducers are integral to the future of superconducting quantum computing, as they would enable scaling and long-distance communication of superconducting quantum processors through optical-fiber links. However, optically induced microwave noise poses a significant challenge in achieving quantum transduction between microwave and optical frequencies. In this work, we study light-induced microwave noise in an integrated electro-optical transducer harnessing the Pockels effect of thin-film lithium niobate. We reveal three sources of added noise with distinctive time constants ranging from sub-100 ns to milliseconds. Furthermore, our results provide insights into the mechanisms and corresponding mitigation strategies for light-induced microwave noise in superconducting microwave-optical transducers and pave the way toward realizing the ultimate goal of quantum transduction.

42 ENGINEERING↗

Design and Optimization of a Hybrid Design for Quantum Transduction

This study presents the mechanical design and analysis of a quantum electro-optical transducer engineered to operate at millikelvin temperatures within a dilution refrigerator. The transducer enables bidirectional microwave-optical frequency conversion through a hybrid architecture that integrates a superconducting radiofrequency (SRF) cavity with an electro-optic optical cavity. Among several design options investigated, the configuration offering the best thermal and mechanical performance was selected, yielding a robust solution with reduced sensitivity to fabrication tolerances, improved heat dissipation, as well as alignment precision. The design ensures uniform temperature distribution, enabling higher laser pump powers and, thus, increased conversion efficiency, while maintaining mechanical stresses safely below the material yield strength. Electromagnetic simulations further validate the design, demonstrating enhanced coupling between the optical and microwave modes, as well as a broader tuning range achieved with smaller tuner displacements.

quantum computing↗

Distributed Fiber Optic Sensing to Identify Locations of Resistive Transitions in REBCO Conductors and Magnets

High-temperature superconductors such as REBa 2 Cu 3 O 7-x (REBCO, RE = rare earth) can generate strong magnetic fields that are promising for applications in particle accelerators and compact fusion reactors. Traditionally, voltage taps are installed in superconducting magnets to measure the voltage signals due to resistive transitions. The voltage-tap-based diagnostics is important for the development of magnet technology as it can help pinpoint the locations in the magnet windings that limit the magnet performance. The architecture of the multi-tape REBCO cable such as CORC wires, however, makes it difficult to apply the voltage-tap-based diagnostics to identify the locations of resistive transitions. Distributed fiber optic sensing (DFOS) has the potential to address this issue. In this paper, we report the measurements of thermal strain along a CORC wire based on optical frequency domain reflectometry with a maximum spatial resolution of 0.65 mm and a temporal resolution of 10 Hz. The optical fiber is co-wound with the CORC wire that is epoxy impregnated. During the test, current was increased until a resistive transition occurred in the conductor. The spectrum shift of the reflected light along the fiber was recorded. The results suggested that with proper thermal isolation from the cryogen, DFOS can be used to identify the locations of resistive transitions in CORC wires and magnets. In conclusion, the results will allow a better understanding of the causes of resistive transitions in REBCO conductors and magnets, which will help improve the REBCO magnet technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Optical and transport properties of plasma mixtures from ab initio molecular dynamics

Predicting the charged particle transport properties of warm dense matter/hot dense plasma mixtures is a challenge for analytical models. High accuracy ab initio methods are more computationally expensive, but can provide critical insight by explicitly simulating mixtures. In this work, we investigate the transport properties and optical response of warm dense carbon–hydrogen mixtures at varying concentrations under either conserved electronic pressure or mass density at a constant temperature. We compare options for mixing the calculated pure species properties to estimate the results of the mixtures. We find that a combination of the Drude model with the Matthiessen's rule works well for DC electron transport and low-frequency optical response. This breaks down at higher frequencies, where a volumetric mix of pure-species AC conductivities works better.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Distributed fiber optic strain sensing of bending deformation of a well mockup in the laboratory

Well integrity is critical to the safety and success of subsurface energy exploration and management, as leakage of fluids from subsurface reservoirs is often induced by compromised wells. This study investigates bending deformation of a mockup of an oil/gas well that is subjected to loads expected in deviated wells under reservoir compaction and assesses the feasibility of utilizing distributed fiber optic strain sensing to monitor the deformation. Here, a well mockup, which consists of outer and inner steel pipes with a cemented annulus, is tested under three-point bending loading and its strain and curvature development is monitored by Brillouin optical time domain reflectometry/analysis (BOTDR/A) as well as optical frequency domain reflectometry (OFDR). The primary objective of this research is to assess the strain sensing performance of newly fabricated fiber optic cables and to identify key cable characteristics which could improve the quality of distributed strain measurements with BOTDR/A. Results show that the tight-buffered cable is best suited for strain sensing as its maximum errors in the strain measurement were -36% and -24% against conventional sensors at the maximum elastic and plastic bending loads, respectively, whereas those of the non-tight-buffered cable were -45% and -71%, respectively. Similar trends were obtained in the bending curvature measurement. The detailed design of the tight-buffered cable is presented to elucidate key characteristics of such a cable, which will facilitate accurate distributed strain sensing in oil and gas wells.

42 ENGINEERING↗

Cascaded Optical Nonlinearities in Dielectric Metasurfaces

Since the discovery of the laser, optical nonlinearities have been at the core of efficient light conversion sources. Typically, thick transparent crystals or quasi-phase matched waveguides are utilized in conjunction with phase-matching techniques to select a single parametric process. In recent years, due to the rapid developments in artificially structured materials, optical frequency mixing has been achieved at the nanoscale in subwavelength resonators arrayed as metasurfaces. Phase matching becomes relaxed for these wavelength-scale structures, and all allowed nonlinear processes can, in principle, occur on an equal footing. This could promote harmonic generation via a cascaded (consisting of several frequency mixing steps) process. However, so far, all reported work on dielectric metasurfaces have assumed frequency mixing from a direct (single step) nonlinear process. In this work, we prove the existence of cascaded second-order optical nonlinearities by analyzing the second- and third-wave mixing from a highly nonlinear metasurface in conjunction with polarization selection rules and crystal symmetries. We find that the third-wave mixing signal from a cascaded process can be of comparable strength to that from conventional third-harmonic generation and that surface nonlinearities are the dominant mechanism that contributes to cascaded second-order nonlinearities in our metasurface.

36 MATERIALS SCIENCE↗

Experimental investigation on the coolability of nuclear reactor debris beds using seawater

During the Fukushima nuclear reactor accident, seawater was injected into the reactor core to cool the decay heat from the heat generating porous debris bed. However, the impact of dissolved salts in water on the coolability of a debris bed is not well understood. This paper is one of the first works to investigate the cooling mechanisms for debris bed using seawater. An experimental system was built where the packed bed test section was volumetrically heated via a high frequency induction heater. The temperature along the axis of the test section was measured using a high resolution temperature sensor based on Optical Frequency Domain Reflectometry. Experimental results show that the dryout heat flux increases with an increase in concentration, with pure water having a dryout volumetric heat flux of 1.8 MW/m and salt water of concentration 7% having a dryout volumetric heat flux of 2.8 MW/m. However, this enhanced coolability using salt water is short term, as the crystallization fouling mechanism becomes significant over time and leads to gradual temperature excursion in the bed. The fouling mechanism eventually leads to a cross section of the debris bed to plug with the deposited salts, and this leads to a pressure build up in the lower regions of the debris bed.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Wavelength conversion through plasmon-coupled surface states

Surface states generally degrade semiconductor device performance by raising the charge injection barrier height, introducing localized trap states, inducing surface leakage current, and altering the electric potential. We show that the giant built-in electric field created by the surface states can be harnessed to enable passive wavelength conversion without utilizing any nonlinear optical phenomena. Photo-excited surface plasmons are coupled to the surface states to generate an electron gas, which is routed to a nanoantenna array through the giant electric field created by the surface states. The induced current on the nanoantennas, which contains mixing product of different optical frequency components, generates radiation at the beat frequencies of the incident photons. We utilize the functionalities of plasmon-coupled surface states to demonstrate passive wavelength conversion of nanojoule optical pulses at a 1550 nm center wavelength to terahertz regime with efficiencies that exceed nonlinear optical methods by 4-orders of magnitude.

42 ENGINEERING↗

Status Update on the Development of Transducers and Bonding Techniques for Enabling Acoustic Measurements of Damage in Microreactor Components

This report provides an overview of potential sensors and sensor-bonding techniques to enable the online acoustic interrogation of microreactor components and enhance structural health monitoring capabilities. The report focuses primarily on optical fiber–based acoustic sensors and describes initial experimental progress toward the deployment of these sensors for microreactor applications. The general approach is to monitor the resonant frequencies of microreactor components and search for evidence of structural defects that could indicate imminent failure. If properly identified, then the components could be repaired during the next reactor outage to prevent costly unplanned shutdowns. The ability to monitor the structural health of components could also reduce the need for time-consuming visual inspections and reduce staffing to improve microreactor economic viability. Increased sensor density is also one of the first steps to moving toward eventual semiautonomous operation. The expected microreactor conditions in which acoustic sensors must survive are characterized, including temperatures, neutron fluences, thermomechanical strains, and vibrational frequencies. Optical fiber–based acoustic sensors are identified as an attractive candidate for acoustic monitoring because of their high accuracy, immunity to electromagnetic interference, and resiliency in high-temperature, high-radiation environments. Optical fiber–based intrinsic sensors, such as type-II fiber-Bragg gratings and Fabry-Pérot Cavities (FPCs), are particularly attractive for a microreactor environment because of their high temperature stability, and FPCs also enable higher frequency interrogation with a lower sensitivity to radiation-induced drift. This report describes multiple interrogation systems, but the best interrogation system for a given situation will depend on the specific microreactor application, including the desired acoustic vibrational amplitudes, modes, and resonant frequencies. Initial experiments included fabricating three FPCs, tack-welding these FPCs to stainless-steel pipes or rods and performing room-temperature acoustic sensing tests to capture the vibrational frequency content. Peaks were identified in the measured frequency spectra and compared with the theoretical fundamental frequencies obtained from Euler-Bernoulli beam theory. Two of the three FPCs measured vibrational frequencies that generally matched those obtained from theory. Future work will include similar testing on pipes or other microreactor components with intentional flaws to evaluate the ability to determine changes in resonant frequencies. Finally, these tests will be repeated at high temperatures, potentially with an applied thermomechanical stress, to include environmental conditions similar to those for a microreactor application.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Strong-Field Control of Plasmonic Properties in Core–Shell Nanoparticles

Utilization of the plasmonic response in nanosystems is a key component of nanophotonics that is typically altered by varying the incident optical frequency or the material configuration. However, in this work we demonstrate that employing intense, femtosecond laser fields unlock nonlinear light–matter interactions such that precise control of the optical response is achieved solely by adjusting the incident intensity. The plasmonic properties of Au/SiO 2 nanoshells are manipulated by exploiting the nonlinear index of refraction of gold and experimentally observed by employing photoelectrons emitted during the interaction as a sensitive, sub-wavelength probe. A striking transition seen in the photoelectron energy spectrum between the weak and strong-field regime is verified by a modified Mie theory simulation that incorporates the nonlinear dielectric nanoshell response. The exhibited intensity-dependent optical control of the plasmonic response in prototypical core–shell nanoparticles paves the way toward ultrafast switching and opto-electronic signal modulation with more complex nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Large negative thermal expansion in GdFe(CN) 6 driven by unusual low-frequency modes

Understanding the negative thermal expansion (NTE) mechanism is of great importance. In this work, we consider the new NTE compound GdFe(CN) 6 (αv = -34.2×10 -6 K -1 ) as a case study to investigate the NTE mechanism from the perspective of the lattice vibrational dynamics. The atomic mean-square displacements suggest that the NTE of GdFe(CN) 6 comes from the strong tension effect induced by the transverse vibrations of the atomic –Fe–Ctriple bondN–Gd– linkages, with the largest contribution given by N atoms. Lattice dynamics calculations show that three low-frequency optical modes at about 50 cm -1 show the largest negative Grüneisen parameters thus providing the largest contribution to the NTE. In conclusion, the existence of these unusual low-frequency vibrational modes can be ascribed to the presence of GdN 6 trigonal prisms in the framework structure of GdFe(CN) 6 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Expanding the range of the resolvable strain from distributed fiber optic sensors using a local adaptive reference approach

Optical frequency domain reflectometry (OFDR) is a spectral measurement technique in which shifts in the local Rayleigh backscatter spectra can be used to perform distributed temperature or strain measurements relative to a reference measurement using ordinary single-mode optical fibers. Here, we demonstrate a data processing methodology for improving the resolvable range of temperature and strain by adaptively varying the reference measurement position by position, based on the time evolution of the local optical intensities and the correlation between the reference and active measurements. These methods nearly double the resolvable range of temperature and strain compared with that achieved using the traditional static reference approach.

47 OTHER INSTRUMENTATION↗

Monolithic Kerr and electro-optic hybrid microcombs

Microresonator-based soliton generation promises chip-scale integration of optical frequency combs for applications spanning from time keeping to frequency synthesis. Access to the soliton repetition rate is a prerequisite for those applications. While miniaturized cavities harness Kerr nonlinearity and enable terahertz soliton repetition rates, such high rates are not amenable to direct electronic detection. Here, we demonstrate hybrid Kerr and electro-optic microcombs using a lithium niobate thin film that exhibits both Kerr and Pockels nonlinearities. By interleaving the high-repetition-rate Kerr soliton comb with the low-repetition-rate electro-optic comb on the same waveguide, wide Kerr soliton mode spacing is divided within a single chip, allowing for direct electronic detection and feedback control of the soliton repetition rate. Our work establishes an integrated approach to electronically access terahertz solitons, paving the way for building chip-scale referenced comb sources.

42 ENGINEERING↗

Methods for microwave characterization of electro-optic crystals for quantum transduction

Microwave-optic quantum transducers are essential devices to develop distributed quantum networks and implement related quantum communication protocols. Three dimensional high-coherence time microwave cavities embedded with electro-optic nonlinear dielectric materials provide promising platforms to boost the efficiency of the microwave-optic frequency conversion. However, so far, the properties for such dielectric crystals operating at milli-Kelvin cryogenic temperatures have not been well understood. Here, we propose a scheme to precisely measure and benchmark the dielectric constant and analyze the dissipation mechanisms of electro-optic materials, such as Lithium Niobate, at the quantum threshold. We will use Fermilab’s three dimensional superconducting cavities with long coherence time. The proposed method of microwave characterization lays the foundations for engineering quantum transduction devices and quantum sensors with high conversion efficiency and fidelity.

Zorzetti, Silvia↗

Observation of a highly conductive warm dense state of water with ultrafast pump–probe free-electron-laser measurements

The electrical conductivity of water under extreme temperatures and densities plays a central role in modeling planetary magnetic fields. Experimental data are vital to test theories of high-energy-density water and assess the possible development and presence of extraterrestrial life. These states are also important in biology and chemistry studies when specimens in water are confined and excited using ultrafast optical or free-electron lasers (FELs). Here we utilize femtosecond optical lasers to measure the transient reflection and transmission of ultrathin water sheet samples uniformly heated by a 13.6 nm FEL approaching a highly conducting state at electron temperatures exceeding 20 000 K. The experiment probes the trajectory of water through the high-energy-density phase space and provides insights into changes in the index of refraction, charge carrier densities, and AC electrical conductivity at optical frequencies. At excitation energy densities exceeding 10 MJ/kg, the index of refraction falls to n = 0.7, and the thermally excited free-carrier density reaches ne = 5 × 1027 m−3, which is over an order of magnitude higher than that of the electron carriers produced by direct photoionization. Significant specular reflection is observed owing to critical electron density shielding of electromagnetic waves. The measured optical conductivity reaches 2 × 104 S/m, a value that is one to two orders of magnitude lower than those of simple metals in a liquid state. At electron temperatures below 15 000 K, the experimental results agree well with the theoretical calculations using density-functional theory/molecular-dynamics simulations. With increasing temperature, the electron density increases and the system approaches a Fermi distribution. In this regime, the conductivities agree better with predictions from the Ziman theory of liquid metals.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

MgSiP 2 : An Infrared Nonlinear Optical Crystal with a Large Non‐Resonant Phase‐Matchable Second Harmonic Coefficient and High Laser Damage Threshold

Superior infrared nonlinear optical (NLO) crystals are in urgent demand in the development of lasers and optical technologies for communications and computing. The critical challenge is to find a crystal with large non‐resonant phase‐matchable NLO coefficients and high laser damage threshold (LDTs) simultaneously, which however scale inversely. This work reports such a material, MgSiP 2, that exhibits a large second harmonic generation (SHG) coefficient of d 14 ≈ d 36 = 89 ± 5 pm V −1 at 1550 nm fundamental wavelength, surpassing the commercial NLO crystals AgGaS 2 , AgGaSe 2 , and ZnGeP 2 . First principles theory reveals the polarizability and geometric arrangement of the [SiP 4 ] tetrahedral units as the origin of this large nonlinear response. Remarkably, it also exhibits a high LDT value of 684 GW cm −2 , which is six times larger than ZnGeP 2 and three times larger than CdSiP 2 . It has a wide transparency window of 0.53–10.35 µm, allowing broadband tunability. Further, it is Type I and Type II phase‐matchable with large effective SHG coefficients of d eff,I ≈80.2 pm V −1 and d eff,II ≈73.4 pm V −1 . The outstanding properties of MgSiP 2 make it a highly attractive candidate for optical frequency conversion in the infrared.

36 MATERIALS SCIENCE↗

Broadband Stability of the Habitable Zone Planet Finder Fabry–Pérot Etalon Calibration System: Evidence for Chromatic Variation

The comblike spectrum of a white light–illuminated Fabry–Pérot etalon can serve as a cost-effective and stable reference for precise Doppler measurements. Understanding the stability of these devices across their broad (hundreds of nanometers) spectral bandwidths is essential to realizing their full potential as Doppler calibrators. However, published descriptions remain limited to small bandwidths or short time spans. We present an ∼6 month broadband stability monitoring campaign of the Fabry–Pérot etalon system deployed with the near-infrared Habitable Zone Planet Finder (HPF) spectrograph. We monitor the wavelengths of each of ∼3500 resonant modes measured in HPF spectra of this Fabry–Pérot etalon (free spectral range = 30 GHz, bandwidth = 820–1280 nm), leveraging the accuracy and precision of an electro-optic frequency comb reference. These results reveal chromatic structure in the Fabry–Pérot mode locations and their evolution with time. We measure an average drift on the order of 2 cm s{sup –1} day{sup −1}, with local departures up to ±5 cm s{sup –1} day{sup −1}. We discuss these behaviors in the context of the Fabry–Pérot etalon mirror dispersion and other optical properties of the system and the implications for the use of similar systems for precise Doppler measurements. Our results show that this system supports the wavelength calibration of HPF at the ≲10 cm s{sup −1} level over a night and the ≲30 cm s{sup −1} level over ∼10 days. Our results also highlight the need for long-term and spectrally resolved study of similar systems that will be deployed to support Doppler measurement precision approaching ∼10 cm s{sup −1}.

42 ENGINEERING↗