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DOE OSTI2025

Optical 14 C Tracing for Biological and Pharmaceutical Applications Using Two-Color Cavity Ringdown Spectroscopy

Laser-based 14 C quantitation has been proposed as a more affordable, higher-throughput, table-top alternative to accelerator mass spectrometry (AMS). Here, we demonstrate the feasibility of a mid-IR 14 C detector based on two-color cavity ringdown spectroscopy (2C-CRDS) for low-level 14 C isotope tracing in biological studies. The 2C-CRDS technique quantifies the sample 14 C content by measuring the 14 CO 2 absorption signals from the combusted samples with mid-IR lasers. With 2C-CRDS, we previously demonstrated the most sensitive and accurate optical measurements of 14 CO 2 . The current detection sensitivity and quantitation accuracy of the instrument, at a few parts per quadrillion (where a quadrillion = 10 15 ) 14 C/C mole fraction, is competitive against AMS. Here, by applying the 2C-CRDS 14 C sensor to two applications relevant to 14 C-labeled biochemical analysis and pharmaceutical studies, we demonstrate sub-fCi level (where 1 fCi = 10 –15 Ci) quantitation of sample 14 C activity, with a minimum sample-size requirement of 3 mg of carbon. The current measurement throughput, ~25 min/sample, is largely limited by the sampling efficiency of the online combustion and CO 2 processing interface to the 2C-CRDS instrument. The possibility of a significantly improved measurement throughput of a few minutes per sample is suggested by the results of a flow-through 14 CO 2 sampling scheme. In conclusion, this improved measurement efficiency, combined with the relatively low cost and compact size of a 2C-CRDS sensor, could potentially revolutionize high-sensitivity 14 C tracing in biological, pharmaceutical, and clinical studies.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

Silicon nitride stress-optic microresonator modulator for optical control applications

Modulation-based control and locking of lasers, filters and other photonic components is a ubiquitous function across many applications that span the visible to infrared (IR), including atomic, molecular and optical (AMO), quantum sciences, fiber communications, metrology, and microwave photonics. Today, modulators used to realize these control functions consist of high-power bulk-optic components for tuning, sideband modulation, and phase and frequency shifting, while providing low optical insertion loss and operation from DC to 10s of MHz. In order to reduce the size, weight and cost of these applications and improve their scalability and reliability, modulation control functions need to be implemented in a low loss, wafer-scale CMOS-compatible photonic integration platform. The silicon nitride integration platform has been successful at realizing extremely low waveguide losses across the visible to infrared and components including high performance lasers, filters, resonators, stabilization cavities, and optical frequency combs. Yet, progress towards implementing low loss, low power modulators in the silicon nitride platform, while maintaining wafer-scale process compatibility has been limited. Here we report a significant advance in integration of a piezo-electric (PZT, lead zirconate titanate) actuated micro-ring modulation in a fully-planar, wafer-scale silicon nitride platform, that maintains low optical loss (0.03 dB/cm in a 625 µm resonator) at 1550 nm, with an order of magnitude increase in bandwidth (DC - 15 MHz 3-dB and DC - 25 MHz 6-dB) and order of magnitude lower power consumption of 20 nW improvement over prior PZT modulators. The modulator provides a >14 dB extinction ratio (ER) and 7.1 million quality-factor (Q) over the entire 4 GHz tuning range, a tuning efficiency of 162 MHz/V, and delivers the linearity required for control applications with 65.1 dB·Hz 2/3 and 73.8 dB·Hz 2/3 third-order intermodulation distortion (IMD3) spurious free dynamic range (SFDR) at 1 MHz and 10 MHz respectively. We demonstrate two control applications, laser stabilization in a Pound-Drever Hall (PDH) lock loop, reducing laser frequency noise by 40 dB, and as a laser carrier tracking filter. This PZT modulator design can be extended to the visible in the ultra-low loss silicon nitride platform with minor waveguide design changes. This integration of PZT modulation in the ultra-low loss silicon nitride waveguide platform enables modulator control functions in a wide range of visible to IR applications such as atomic and molecular transition locking for cooling, trapping and probing, controllable optical frequency combs, low-power external cavity tunable lasers, quantum computers, sensors and communications, atomic clocks, and tunable ultra-low linewidth lasers and ultra-low phase noise microwave synthesizers.

Wang, Jiawei (ORCID:0000000257965220)↗

DOE OSTI2024

X-ray diagnostics for the cavity-based x-ray free-electron laser project

The success of x-ray free-electron lasers (XFELs) in recent years has greatly advanced many scientific fields. However, most of these XFELs suffer from a low longitudinal coherence and instabilities due to the stochastic start-up process. A cavity-based x-ray free-electron laser (CBXFEL) is a possible future direction in the development of fully coherent and stable x-ray sources. One of the challenges of a CBXFEL is the requirement for the μ⁢m−sized electron bunches to fully overlap in three dimensions with the circulating μ⁢m−sized x-ray pulses in an x-ray cavity tens or hundreds of meters long. We present here the development of an x-ray diagnostics system for accurate alignment of x-ray beams in the CBXFEL cavity. The system was developed within the framework of a CBXFEL research and development collaboration among Argonne National Laboratory, SLAC National Accelerator Laboratory, and Spring-8. All the designed diagnostic components have been fully characterized at the Advanced Photon Source to demonstrate a capability for sub-μ⁢rad angular and μ⁢m spatial alignment of the CBXFEL cavity.

Free-electron lasers↗

DOE OSTI2021

A 10-Gb/s Driver/Receiver ASIC and Optical Modules for Particle Physics Experiments

We present the design and test results of a Drivers and Limiting AmplifierS ASIC operating at 10 Gbps (DLAS10) and three Miniature Optical Transmitter/Receiver/Transceiver modules (MTx+, MRx+, and MTRx+) based on DLAS10. DLAS10 can drive two Transmitter Optical Sub-Assemblies (TOSAs) of Vertical Cavity Surface Emitting Lasers (VCSELs), receive the signals from two Receiver Optical Sub-Assemblies (ROSAs) that have no embedded limiting amplifiers, or drive a VCSEL TOSA and receive the signal from a ROSA, respectively. Each channel of DLAS10 consists of an input Continuous Time Linear Equalizer (CTLE), a four-stage limiting amplifier (LA), and an output driver. The LA amplifies the signals of variable levels to a stable swing. The output driver drives VCSELs or impedance-controlled traces. DLAS10 is fabricated in a 65 nm CMOS technology. The die is 1 mm x 1 mm. DLAS10 is packaged in a 4 mm x 4 mm 24-pin quad-flat no-leads (QFN) package. DLAS10 has been tested in MTx+, MRx+, and MTRx+ modules. Both measured optical and electrical eye diagrams pass the 10 Gbps eye mask test. Furthermore, the input electrical sensitivity is 40 mVp-p, while the input optical sensitivity is -12 dBm. The total jitter of MRx+ is 29 ps (P-P) with a random jitter of 1.6 ps (RMS) and a deterministic jitter of 9.9 ps. Each MTx+/MTRx+ module consumes 82 mW/ch and 174 mW/ch, respectively.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

On-chip spectroscopic sensors with optical fringe suppression

An on-chip spectroscopic sensor includes a tunable diode laser. A laser driver for drives the tunable diode laser. An analyte test cavity receives a chemical sample and exposes the received chemical sample to light from the tunable diode laser. An optical detector detects light emerging from the analyte test cavity as a result of the laser exposure. A spectral analyzer determines a spectrum of the emerging light, matches and removes one or more known optical fringe patterns from the determined spectrum, and determines a composition or concentration of the chemical sample from the optical fringe pattern-removed spectrum.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

On-chip spectroscopic sensors with optical fringe suppression

Green, William↗

DOE OSTI2022

Coaxial laser absorption and optical emission spectroscopy of high-pressure aluminum monoxide

This work advances laser absorption spectroscopy with measurements of aluminum monoxide (AlO) temperature and column density in extreme pressure ( P > 60 bar) and temperature ( T > 4000 K) environments. Measurements of the AlO A 2 Π i – X 2 Σ + transition are made using a microelectromechanical system, tunable vertical cavity surface emitting laser (MEMS-VCSEL). Simultaneous emission measurements of the AlO B 2 Σ + – X 2 Σ + transition are made along a line of sight that is coaxial with the laser absorption. Absorption temperature fits agree with emission spectra for a T = 3200 K, P = 9 bar case. In cases with T > 4000 K, P > 60 bar, absorption fits match the ambient temperature while emission fits over-estimate it, owing to high optical depths. These data juxtapose passive and active spectroscopic methods and demonstrate the versatility of AlO laser absorption in high-pressure and high-temperature environments where experimental data remain scarce, and engineering models will benefit from refined measurements.

Daniel, K. A.↗

DOE OSTI2021

Using Disorder to Overcome Disorder: A Mechanism for Frequency and Phase Synchronization of Diode Laser Arrays

Noise and disorder are known, in certain circumstances and for certain systems, to improve the level of coherence over that of the noise-free system. Examples include cases in which disorder enhances response to periodic signals, and those where it suppresses chaotic behavior. We report a new type of disorder-enhancing mechanism, observed in a model that describes the dynamics of external cavity-coupled semiconductor laser arrays, where disorder of one type mitigates (and overcomes) the desynchronization effects due to a different disorder source. Here, we demonstrate stabilization of dynamical states due to frequency locking and subsequently frequency locking-induced phase locking. Here, we have reduced the equations to a potential model that illustrates the mechanism behind the misalignment-induced frequency and phase synchronization.

42 ENGINEERING↗

DOE OSTI2025

Bi-stability and period-doubling cascade of frequency combs in exceptional-point lasers

Abstract Recent studies have demonstrated that a laser can self-generate frequency combs when tuned near an exceptional point (EP), where two cavity modes coalesce. These EP combs induce periodic modulation of the population inversion in the gain medium, and their repetition rate is independent of the laser cavity’s free spectral range. In this work, we perform a stability analysis that reveals two notable properties of EP combs, bi-stability and a period-doubling cascade. The period-doubling cascade enables halving of the repetition rate while maintaining the comb’s total bandwidth, presenting opportunities for the design of highly compact frequency comb generators.

exceptional points↗

DOE OSTI2020

1.5 – 1.6 μm semiconductor lasers with an asymmetric periodic optically coupled waveguide

High-power 1.5 – 1.6-μm semiconductor lasers with an asymmetric periodic optically coupled waveguide are developed and their current – voltage, light – current, and spectral characteristics are experimentally studied. The characteristics of these lasers are compared with the characteristics of traditional lasers based on double separate-confinement heterostructures. It is shown that the developed lasers have lower divergence and almost the same threshold and power characteristics as conventional lasers with Fabry – Perot resonators. The developed lasers with a cavity length of 1.6 mm and a mesa-stripe contact width of 3 μm mounted in a housing 11 mm in diameter have a power no lower than 200 mW at a pump current not exceeding 700 mA with a divergence of 25 – 35° versus 45° typical for conventional lasers. (lasers)

36 MATERIALS SCIENCE↗

DOE OSTI2022

Design of inertial fusion implosions reaching the burning plasma regime

One of the last remaining milestones in fusion research before reaching ignition is creating a burning plasma state, where alpha particles from deuterium-tritium (DT) fusion reactions redeposit their energy as the dominant source of heating in the plasma. The indirect-drive inertial confinement fusion approach at the National Ignition Facility (NIF) uses a laser-generated radiation cavity (hohlraum) to spherically implode DT fuel to high temperatures and densities in a central ”hot spot”. Here, we deliver more energy to the hot spot than ever before, while maintaining the extreme pressures required for inertial confinement, by increasing the size of the implosion compared to previous experiments. We develop more efficient hohlraums, to drive these larger implosions within NIF’s current laser energy and power capability and control symmetry by moving energy between laser beams and by changing the shape of the hohlraum. These designs resulted in record fusion powers of 1.5 petawatts, greater than the input power of the laser, and 170 kJ of fusion energy. Radiation hydrodynamics simulations show alpha particle heating as the dominant term in the hot spot energy balance, e.g. a burning plasma state. This work is expected to motivate future studies of burning plasmas and improve predictive capability by providing a benchmark for modeling used to understand the proximity to ignition.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Standoff Infrared Measurements of Chemical Plume Dynamics in Complex Terrain Using a Combination of Active Swept-ECQCL Laser Spectroscopy with Passive Hyperspectral Imaging

Chemical plume detection and modeling in complex terrain present numerous challenges. We present experimental results from outdoor releases of two chemical tracers (sulfur hexafluoride and Freon-152a) from different locations in mountainous terrain. Chemical plumes were detected using two standoff instruments collocated at a distance of 1.5 km from the plume releases. A passive long-wave infrared hyperspectral imaging system was used to show time- and space-resolved plume transport in regions near the source. An active infrared swept-wavelength external cavity quantum cascade laser system was used in a standoff configuration to measure quantitative chemical column densities with high time resolution and high sensitivity along a single measurement path. Both instruments provided chemical-specific detection of the plumes and provided complementary information over different temporal and spatial scales. The results show highly variable plume propagation dynamics near the release points, strongly dependent on the local topography and winds. Effects of plume stagnation, plume splitting, and plume mixing were all observed and are explained based on local topographic and wind conditions. Measured plume column densities at distances ~100 m from the release point show temporal fluctuations over ~1 s time scales and spatial variations over ~1 m length scales. The results highlight the need for high-speed and spatially resolved measurement techniques to provide validation data at the relevant spatial and temporal scales required for high-fidelity terrain-aware microscale plume propagation models.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Radiation-hard miniature optical engine with high bandwidth

Future silicon trackers will be operated in an intense radiation environment and require large volumes of data to be transmitted off detector. In addition, the optical modules must be of low mass in order to limit multiple scattering and nuclear interactions that would degrade the overall performance of the detector. Here, we present a miniature optical engine that satisfies these constraints. The optical engine consists of an ASIC driving a VCSEL (Vertical Cavity Surface Emitting Laser) array in an optical package. Two ASICs are designed to operate a 12-channel VCSEL array at 1.28 or 5.12 Gb/s per channel, which yields a total data rate of up to 60 Gb/s. The core transistors are fabricated in a 65 nm CMOS process which enhance the radiation-hardness. Each channel contains equalizer (CTLE) and clock-data recovery circuits (CDR) so that the ASIC can restore the highly distorted electrical signal after propagating through several meters of cables of small diameter. The equalizer, CDR, and VCSEL driver are configured via a digital I 2 C chip interface with triple redundant memory to mitigate single event upset (SEU) effects. The bias and modulation currents are controlled by a digital-to-analog converter (DAC). We present the design of the circuit together with the results of the simulations and preliminary measurements.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

A 20 Gbps PAM4 data transmitter ASIC for particle physics experiments

We present the design and test results of a novel data transmitter ASIC operating up to 20.48 Gbps with 4-level Pulse-Amplitude-Modulation (PAM4) for particle physics experiments. This ASIC, named GBS20, is fabricated in a 65 nm CMOS technology. Two serializers share a 5.12 GHz Phase Locked Loop (PLL) clock. The outputs from the serializers are combined into a PAM4 signal that directly drives a Vertical-Cavity-Surface-Emitting-Laser (VCSEL). The input data channels, each at 1.28 Gbps, are scrambled with an internal 2$^{7}$-1 Pseudo-Random Binary Sequence (PRBS), which also serves as a frame aligner. GBS20 is tested to work at 10.24 and 20.48 Gbps with a VCSEL-based Transmitter-Optical-Subassembly (TOSA). The power consumption of GBS20 is below 238 mW and reduced to 164 mW in the low-power mode.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Infrared Absorption Spectra of H2SO4, SO3, SO2, and H2O at 300C and 350C

Mid infrared absorption spectra of sulfuric acid (H2SO4), sulfur trioxide (SO3), sulfur dioxide (SO2), and water (H2O) were collected in a high temperature gas cell operating at either 300C or 350C. The spectra were collected using tunable external cavity quantum cascade lasers (ECQCLs) tuning, which were capable of operating over the wavelength range from approximately 7 microns to 9 microns, where H2SO4 and SO3 have their strongest absorption features. The spectra can be used as a library for developing gas sensors.

infrared absorption↗

DOE OSTI2020

Standoff Detection of Chemical Plumes Using Swept-ECQCL Remote Detection Technology: Results from EMRTC Complex Terrain Dual Tracer Experiment

As part of the Complex Terrain Dual Tracer Experiments performed in support of the LYNM program, a swept-wavelength external cavity quantum cascade laser (swept-ECQCL) remote detection system was deployed to measure chemical plume propagation with high temporal resolution. The swept-ECQCL remote detection technology was initially developed at PNNL, and is now under further development at Opticslah, LLC under SBIR funding from DOE (DOE SBIR Phase I Project DE-SC0019855, Remote Detection Technologies, Program Manager Chris Ramos). The swept-ECQCL technology provides a single-frequency infrared laser source which is rapidly scanned over a large wavelength range to measure the infrared absorption of gases, liquids, or solids. Analysis of the measured infrared absorption spectrum is used to detect, identify, and quantify the chemical species which are present. While most previous laser-based techniques used small wavelength tuning ranges to measure only a few isolated spectral lines of a few species, the swept-ECQCL provides the large tuning range needed to measure multiple species simultaneously, and to detect broad absorption features from large molecules or condensed phase materials. In addition, the swept-ECQCL systems have high enough spectral resolution and sensitivity to measure narrow lines of small molecules and determine isotope ratios. The remote detection system for gas plumes is based on the swept-ECQCL technology, and consists of a swept-ECQCL source, infrared detector, control electronics, and beam transmitting and alignment optics. The remote detection system directs the infrared output of the swept-ECQCL to a target retro reflector typically located at ~10-10,000 m distance. The swept-ECQCL wavelength is varied continuously over a large wavelength range (>1000 nm) at rates up to 1000 Hz. The swept ECQCL light reflected from the remote target is collected and focused onto an infrared photodetector. By measuring the detector signal continuously as the swept-ECQCL wavelength is varied, a time-series of absorption spectra are measured for the gases along the beam line of-sight. Based on analysis and fitting of the measured absorption spectra, the time-dependent chemical concentrations of species are determined. Multiple species and mixtures can be detected simultaneously, for all species with absorption features above the sensor noise floor. The sensor output is thus a continuous, high-speed record of identified chemicals along with their concentrations and isotope ratios of interest. The high-speed operation enables low-noise operation in conditions of atmospheric turbulence and allows tracking of fluctuating concentrations in transient chemical plumes as needed for reliable remote detection applications. All components operate with minimal cooling requirements and no cryogens are needed. In addition, the output infrared light is invisible with an intensity below the maximum permissible exposure (MPE) threshold of 100 mW/cm2 for these infrared wavelengths and thus eye safe. The measurement concept for plume detection using the swept-ECQCL remote detection system is as follows. The ECQCL beam is directed toward a remote retro-reflector, which reflects the beam back to the ECQCL system where it is focused onto an infrared photodetector. The line-of-sight from the ECQCL system to the retro-reflector defines the measurement path. The detected infrared signal is recorded continuously and detects the absorption of molecular species along the measurement path. Before a plume release, the system measures absorption from atmospheric constituents, which in this LWIR band consist primarily of lines from H 2 O and CO 2 , with additional weaker absorption from N 2 O, NH 3 , and O 3 possibly contributing. The system then measures any changes in absorption due to the tracer compounds when they enter the measurement path. The shape of absorption features is used to distinguish and identify the different tracer compounds, and the strength of the absorption is used to determine the path-integrated concentration – also called the column density.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Fundamental bandwidth limits and shaping of frequency-modulated combs

Frequency-modulated (FM) combs based on active cavities like quantum cascade lasers have recently emerged as promising light sources in many spectral regions. Unlike passive modelocking, which generates amplitude modulation using the field’s amplitude, FM comb formation relies on the generation of phase modulation from the field’s phase. They can therefore be regarded as a phase-domain version of passive modelocking. However, while the ultimate scaling laws of passive modelocking have long been known—Haus showed in 1975 that pulses modelocked by a fast saturable absorber have a bandwidth proportional to effective gain bandwidth—the limits of FM combs have been much less clear. Here, we show that FM combs based on fast gain media are governed by the same fundamental limits, producing combs whose bandwidths are linear in the effective gain bandwidth. Not only do we show theoretically that the diffusive effect of gain curvature limits comb bandwidth, but we also show experimentally how this limit can be increased. By adding carefully designed resonant-loss structures that are evanescently coupled to the cavity of a terahertz laser, we reduce the curvature and increase the effective gain bandwidth of the laser, demonstrating bandwidth enhancement. Our results can better enable the creation of active chip-scale combs and be applied to a wide array of cavity geometries.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Low-loss stable storage of 1.2 Å X-ray pulses in a 14 m Bragg cavity

Here, we present an experimental demonstration of a stable, low-loss, large X-ray cavity operating at 1.2 Å wavelength. The cavity consists of four separate high-reflectivity single crystal diamond Bragg mirrors arranged in a rectangular configuration with a round-trip distance of 14.2 m. Femtosecond X-ray pulses from an X-ray free-electron laser were coupled into the cavity via a transmission phase grating. We show that a stable mode can be maintained with the introduction of cavity focusing and measure round-trip efficiencies approaching 88%, or >96% when excluding grating and lens losses, close to the Bragg mirror theoretical performance limit. The direct observation of sustained stable X-ray circulation provides the most direct evidence to date that cavity-based X-ray free-electron lasers and other cavity-based hard X-ray systems are feasible.

47 OTHER INSTRUMENTATION↗