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DOE OSTI2022

Controlling Structural, Electronic, and Energy Flow Dynamics of Catalytic Processes through Tailored Nanostructures

MoS 2 (molybdenum disulfide) is a highly-versatile catalyst material for support of numerous reactions from hydrodesulfurization and denitrogenation to the focus of this renewal proposal: hydrogenation of CO/CO 2 towards (higher) alcohols. At the same time, MoS 2 is a non-toxic, environmentally-benign and rather inert material- which under ambient conditions for some time has served as a lubricant and, more recently, as next-generation electronic material. The apparent contrast between inertness and stability in ambient, and catalytic activity under reactive conditions is puzzling and calls for a synergistic theoretical and experimental investigation with the long-term objective of enabling the rational design of MoS 2 -based catalysts for alcohol-formation reactions by providing a microscopic understanding of the environmental factors that determines site activity and selectivity. Our research project seeks answers to the questions (a) what conformation does MoS 2 adopt under reaction conditions (as opposed to that under ultrahigh vacuum and low temperatures)?; (b) what reaction pathways exist on such a material?; (c) how can the local environment of the active sites be manipulated so as to make MoS 2 an efficient catalyst for production of higher alcohol from syngas? In particular, research strategies will explore how the basal plane composed of sulfur atoms can be activated so as to exhibit a reactivity of its own, by addressing three research targets and building on extensive preliminary and enabling work: (1) vacancies and vacancy aggregates on the basal plane; (2) non-local catalyst transformation through alkali doping, hydrogenation and phase transition; (3) fabrication of a metal-nanoparticle-activated MoS 2 system, in which particle anchoring, reactive sites and pathways as well as selectivity are controlled by design, as an example of predictive development of a catalyst material,. All strategies are directed to improve the efficacy of the key reactive sites and selectivity of chemical pathways by design, to replace the inefficient methodology of trial and error in catalyst development. This research project represents a synergistic combination of computational guidance, foundational surface-science-based experiments and validation under reactive conditions that aims at transformative new insights into the working of MoS 2 -based hydrogenation-catalysts, a topic squarely at the center of the interest of DOE BES. Guided and led by Talat Rahman, a computational physicist, this project will apply density functional theory to understand structure, reaction pathways and chemical potentials associated with MoS 2 -based CO/CO 2 hydrogenation, augmented by kinetic Monte Carlo methods for reaction rates and prefactors as well as ab-initio molecular dynamics for evaluation of thermal stability. Complementary experimental input and validation will originate from co-PI Ludwig Bartels, a physical chemist and materials scientist, whose group focuses on local imaging and preparation of MoS 2 materials, from co-PI Peter Dowben, an experimental physicist, whose group is expert in the spectroscopy of occupied and unoccupied electronic states, and from senior collaborator Michael White of Brookhaven National Laboratory, whose group generates high-resolution electronic and activity information on size-selected well-defined metal chalcogenide clusters. This collaborative effort will enable a comprehensive understanding of the correlation of structural integrity and catalytic activity of MoS 2 in forms ranging from extended films to individual particles with known geometries and binding sites. Alcohol formation from syngas is a rapidly emerging application that has great potential through facile, economic, and decentralized biomass gasification. CO 2 activation is one of the most pressing concerns of our time: increasing CO 2 levels in the atmosphere change the climate and expose the globe to environmental transformations with the potential for enormous economic and societal impact. We will investigate CO/CO 2 hydrogenation via an interdisciplinary research collaboration with established synergy – one that, in accordance with the mission of the DOE, involves accredited Hispanic-Serving Institutions and that, through student exchange with international collaborators and National Labs, will directly benefit a broad spectrum of communities and generate human resources in sciences essential to their future.

2D materials↗
DOE OSTI2022

Atomic-Scale Surface Studies of Bulk Metallic Glasses. Final Report

Bulk metallic glasses (BMGs) are of both scientific and technological interest because the absence of periodic atomic arrangements provides them with unique physical, chemical, and mechanical properties. Their high strength, superior elasticity, and an ability to be easily formed into virtually unlimited shapes with feature sizes from centimeters to Angstroms by blow molding and thermoplastic forming makes them an attractive choice for more and more practical applications and products. Due to their complex internal structure, however, experiments that yield insight into their exact atomic arrangements have been scarce. As a result, glass physics is one of the last remaining unexplored fields of materials science despite the scientific and technological importance of glasses in our daily lives, and the question how to characterize and control matter away from equilibrium, as glasses are, was listed as one of five Grand Challenges in a recent DoE report. The main reason for the slow progress in glass physics is the lack of experimental tools that enable access to atomic-scale structural and behavioral information for disordered materials. Such atomic-scale knowledge is mandatory to establish structure-property relationships that ultimately could allow to custom-design alloys featuring specific desired characteristics. With no such relationships available, theory development in glass remains basic and the few that exist are often untested. The aim of this research was to enable progress in our understanding of BMGs by developing a new approach that will allow a meaningful application of local surface science methods to specially prepared BMG samples to obtain a wealth of quantitative information on their atomic arrangements. Key was the availability of specially prepared samples whose surfaces feature large atomically flat terraces despite being entirely amorphous, which we have produced from a Pt 57.5 Cu 14.7 Ni 5.3 P 22.5 alloy (‘Pt-BMG’) both under ambient conditions as well as in ultrahigh vacuum using a unique setup that has been specially developed within this grant. Our approach starts with the in-situ preparation of oxide crystals that are terminated by large terraces, from which exact mirror images out of BMG will be produced using thermoplastic forming (TPF); for the research within this grant, we have successfully used (001)-oriented SrTiO 3 single crystal surfaces as well as (100)-, (110)-, and (111)-oriented single crystals made from LaAlO 3 . Since the resulting BMG replicas display all features of the original crystal with sub-Angstrom fidelity, thereby mimicking the original crystal’s termination by atomically flat terraces without being crystalline themselves, they are ideally suited for further investigation. The following atomic-scale local studies were then carried within this proposal: (i) high-resolution surface imaging and local spectroscopy using scanning probe microscopy, which showed disordered atom-like features and revealed changes in the gradient of the local surface potential on a 1-2 nm length scale; (ii) characterization of atomic-scale plastic flow with affected volumes as low as 1000 atoms, which showed local hardness near or above the theoretically predicted maximum and, once plastic deformation was initiated, homogeneous flow of the atoms involved; (iii) characterization of surface relaxation processes and the onset of crystallization induced by annealing, which showed that upon heating over the material’s glass transition temperature, the surface rearranges and relaxes towards a more stable, denser packed glass, which increases on-terrace surface roughness, while surface tension smoothens step edges; and (iv) studies that investigate the dependence of the material’s mechanical properties and structure on processing parameters, revealing that relaxed glasses get denser, harder, and more elastic. In combination, this information allows to combine structural models with mechanical properties and preparation history, thereby facilitating the development of preparation-structure-property relationships for metallic glasses. With the availability of such information, bulk metallic glasses can be further optimized to be used in more and more applications in industry.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Surface Science Studies of Selective Fischer-Tropsch Chemistry on Cobalt Carbide Surfaces

Advances in catalysis science are critical to the progress of the United States. Catalysis is employed, in one way or another, in the production of almost every chemical and product manufactured. The catalysis research that we undertook here, regarding the role of specific facets of cobalt carbide in the Fischer-Tropsch production of low molecular weight olefins (FTO), is motivated by the work of many previous investigators. In particular two research groups from China had discovered FTO catalysts that work very selectively for low molecular weight olefins coupled with low production of methane. These are potentially very important findings that could find significant industrial utility if improvements can be discovered. With the research undertaken here we chose to focus on one of these studies and especially the Co 2 C surfaces that they implicate as being responsible for this exciting FTO catalysis with low production of methane. In this study, Zhong and co-workers investigated cobalt-manganese oxide catalysts for the Fischer-Tropsch to Olefins process. After reaching steady-state their catalyst showed a good selectivity to light olefins and low selectivity to methane with a carbon monoxide conversion of 31.8% at one atmosphere (with a H 2 /CO ratio of two and a temperature of 250°C). Lower H 2 /CO ratios and lower pressures increased the olefin production. Their catalyst characterization studies indicated that cobalt carbide quadrangular nanoprisms with preferentially exposed (101) and (020) facets were important in favoring lower olefin production and inhibiting methane formation. The authors stated that these cobalt carbide nanoprisms are a promising new catalyst system for directly converting synthesis gas to lower olefins. Motivated by the studies of Zhong and co-workers, our goal with the research here was to contribute to a better understanding of catalysis science through the study of surface chemical reactions related to the Fischer-Tropsch to Olefins reaction on specific facets of planar model cobalt carbide catalysts in ultrahigh vacuum.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Growth of Well-Defined Model Catalysts for Electrochemistry: From Surface Science Studies to Electrocatalytic CO2 Conversion

We combined ultrahigh vacuum (UHV) surface science techniques, electrochemical measurements, and computational modeling to investigate electrocatalytic systems that are crucial components of the carbon management effort, including oxygen evolution reactions (OER) and CO2 reduction reactions (CO2RR). Well-defined Model catalysts were grown on substrates in the UHV chamber and characterized with X-ray photoelectron spectroscopy (XPS) and scanning tunneling microscopy (STM). Selected model electrocatalysts were then tested in electrochemical cells to establish the structure-property relationships in OER and CO2RR. Our results showed that the edge sites of Fe2O3 grown on Au(111) were the most active toward OER and incorporation of Ni at the edge sites (NiFeOx) further boosted their OER activity. We also resolved the size-dependent electrocatalytic CO2-to-CO conversion of the Ag nanoparticle electrocatalysts with average particle diameter between 2 to 6 nm: smaller diameter (< 3 nm) particles favored H2 evolution reaction (HER) due to a high population of Ag edge sites, whereas larger diameter particles favored CO2RR as the population of Ag(100) surface sites grew. We further discovered that electronic interactions between small diameter Ag particles and highly defective carbon supports could break the size-dependent CO2RR selectivity, resulting in highly selective (CO Faradaic Efficiency > 90%) and active Ag nanoparticle electrocatalysts with sizes < 2 nm diameter.

Deng, Xingyi↗
DOE OSTI2025

Understanding of Ag Nanocatalysts for Electrocatalytic CO2 Conversion: Effects of Particle Size and Carbon Support

In this talk, we combined ultrahigh vacuum (UHV) surface science techniques, electrochemical measurements, and computational modeling to investigate Ag based electrocatalysts for CO2 reduction reaction (CO2RR). Our goal is to understand the critical characteristics governing the activity and selectivity of Ag electrocatalysts. Ag electrocatalysts were grown on highly oriented pyrolytic graphite (HOPG) in the UHV chamber, characterized with X-ray photoelectron spectroscopy (XPS) and scanning tunneling microscopy (STM), and then tested in a custom-built gastight H-cell. Supported by computational modeling based on density functional theory (DFT) calculations and microkinetic modeling (MKM), our studies revealed a strong size-dependent electrocatalytic CO2-to-CO conversion of the Ag nanoparticle electrocatalysts with average particle diameter between 2 to 6 nm. Smaller diameter (< 3 nm) particles favored H2 evolution reaction (HER) due to a high population of Ag edge sites, whereas larger diameter particles favored CO2RR as the population of Ag(100) surface sites grew. We further discovered that electronic interactions between small diameter Ag particles and highly defective carbon supports could break the size-dependent CO2RR reactivity, resulting in highly selective (CO Faradaic Efficiency > 90%) and active Ag nanoparticle electrocatalysts with sizes < 2 nm diameter. This knowledge is key to understand electrocatalysts performance and to ultimately guide electrocatalyst design

Ag nanoparticles↗
DOE OSTI2025

Robotic Assembly of SRF Cavity Pair

Superconducting Radio Frequency (SRF) cavities for particle accelerators require tight tolerances, ultrahigh vacuum, and strict cleanliness during assembly. As in the semiconductor industry, defects such as particles and residues are deleterious to performance, possibly rendering a cavity unfit for use. This problem is addressed primarily through cleanroom assembly during sensitive steps and rigorous chemical processing to prevent and remove such defects. Human workers are often the largest source of contamination, even with proper gowning and practices. The semiconductor industry has long integrated robots in cleanroom operation, but this has not occurred for SRF cavity production; SRF cavities, unlike wafers, are complex shapes, require more hands-on mechanical assembly, and are low-volume production items. At Jefferson Laboratory, a co-operative robot (cobot) has been setup to overcome these problems. Cobots are safe for use alongside human workers and can integrate new tools such as a 3D camera part detection and gripper for item manipulation. Therefore, cobots represent a promising avenue for reducing particulate generated during a variety of assembly tasks. A mockup of a cavity pair and coupler was setup and the cobot programmed to automatically pick up the coupler and place on the mating cavity flange. Particle counting methods were setup to measure human vs cobot assembly particulate generation inside a cavity mockup. Other potential uses will be discussed for further improving SRF cavity assembly steps, where a cobot can replace or assist a human operator, and what potential gains are expected.

Duzik, Adam [Thomas Jefferson National Accelerator↗
DOE OSTI2020

Carbide-Modified Pd on ZrO2 as Active Phase for CO2-Reforming of Methane—A Model Phase Boundary Approach

Starting from subsurface Zr0-doped “inverse” Pd and bulk-intermetallic Pd0Zr0 model catalyst precursors, we investigated the dry reforming reaction of methane (DRM) using synchrotron-based near ambient pressure in-situ X-ray photoelectron spectroscopy (NAP-XPS), in-situ X-ray diffraction and catalytic testing in an ultrahigh-vacuum-compatible recirculating batch reactor cell. Both intermetallic precursors develop a Pd0–ZrO2 phase boundary under realistic DRM conditions, whereby the oxidative segregation of ZrO2 from bulk intermetallic PdxZry leads to a highly active composite layer of carbide-modified Pd0 metal nanoparticles in contact with tetragonal ZrO2. This active state exhibits reaction rates exceeding those of a conventional supported Pd–ZrO2 reference catalyst and its high activity is unambiguously linked to the fast conversion of the highly reactive carbidic/dissolved C-species inside Pd0 toward CO at the Pd/ZrO2 phase boundary, which serves the role of providing efficient CO2 activation sites. In contrast, the near-surface intermetallic precursor decomposes toward ZrO2 islands at the surface of a quasi-infinite Pd0 metal bulk. Strongly delayed Pd carbide accumulation and thus carbon resegregation under reaction conditions leads to a much less active interfacial ZrO2–Pd0 state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

In Situ High-Temperature Ultrafast Electron Diffraction through Integrated Furnace and MEMS Platforms

Temperature fundamentally governs phase stability, defect evolution, and transport behavior in materials. Despite its central role, direct measurements of structural evolution at elevated temperatures on ultrafast timescales have remained limited. Here, we report the design, integration, and validation of 2 complementary in situ heating platforms that substantially extend the thermal operating range of ultrafast electron diffraction (UED). A compact furnace-type heating stage enables stable diffraction measurements from room temperature to 800 K with ±0.1 K stability under ultrahigh vacuum, achieved through multi-sensor feedback control, dual air-cooling channels, and a thermally isolated motion stage. In parallel, a microelectromechanical system (MEMS)-based heating platform provides rapid thermal response and access to extreme temperatures ≥1,373 K with ±0.1 K stability over hundreds-micrometer regions while supporting simultaneous electrical biasing for electrothermal coupling studies. Absolute temperature calibration is established using diffraction-based thermometry via aluminum lattice expansion and independently validated through in situ melting of bismuth thin films. UED measurements further reveal pronounced temperature-dependent nonequilibrium lattice dynamics in bismuth, including modifications to electron–phonon coupling and Debye–Waller behavior, as well as enhanced ultrafast diffuse scattering in aluminum at elevated temperatures. Together, these developments establish a practical framework for quantitative, time-resolved studies of temperature-driven kinetics and nonequilibrium structural dynamics under extreme thermal environments.

Bai, Qianqian [Chinese Academy of Sciences (CAS), ↗
DOE OSTI2021

Methods and devices configured to operated scanning tunneling microscopes using out-of-bandwidth frequency components added to bias voltage and related software

In the system and method disclosed, an ultrahigh vacuum (UHV) scanning tunneling microscope (STM) tip is used to selectively desorb hydrogen atoms from the Si(100)-2X1:H surface by injecting electrons at a negative sample bias voltage. A new lithography method is disclosed that allows the STM to operate under imaging conditions and simultaneously desorb H atoms as required. A high frequency signal is added to the negative sample bias voltage to deliver the required energy for hydrogen removal. The resulted current at this frequency and its harmonics are filtered to minimize their effect on the operation of the STM's feedback loop. This approach offers a significant potential for controlled and precise removal of hydrogen atoms from a hydrogen-terminated silicon surface and thus may be used for the fabrication of practical silicon-based atomic-scale devices.

Moheimani, Seyed Omid Reza↗
DOE OSTI2023

Methods and devices configured to operated scanning tunneling microscopes using out-of-bandwidth frequency components added to bias voltage and related software

In the system and method disclosed, an ultrahigh vacuum (UHV) scanning tunneling microscope (STM) tip is used to selectively desorb hydrogen atoms from the Si(100)-2X1:H surface by injecting electrons at a negative sample bias voltage. A new lithography method is disclosed that allows the STM to operate under imaging conditions and simultaneously desorb H atoms as required. A high frequency signal is added to the negative sample bias voltage to deliver the required energy for hydrogen removal. The resulted current at this frequency and its harmonics are filtered to minimize their effect on the operation of the STM's feedback loop. This approach offers a significant potential for controlled and precise removal of hydrogen atoms from a hydrogen-terminated silicon surface and thus may be used for the fabrication of practical silicon-based atomic-scale devices.

Moheimani, Seyed Omid Reza↗
DOE OSTI2020

Surface Reactivity of Ag-Modified Ceria to Hydrogen: A Combined Experimental and Theoretical Investigation

We investigate the mechanism of H 2 activation on Ag-modified cerium oxide surfaces, of interest for different catalytic applications. The study is performed on thin epitaxial cerium oxide films, investigated by X-ray photoemission spectroscopy to assess the changes of both the Ag oxidation state and the concentration of Ce 3+ ions, O vacancies, and hydroxyl groups on the surface during thermal reduction cycles in vacuum and under hydrogen exposure. The results are interpreted using density functional theory calculations to model pristine and Ag-modified ceria surfaces. Although the reactivity of ceria toward H 2 oxidation improves when a fraction of Ce cations is substituted with Ag, the concentration of reduced Ce 3+ ions in Ag-modified ceria is found to be lower than in pure ceria under the same conditions. This behavior is observed even though the number of surface oxygen vacancies caused by the thermal treatment under hydrogen exposure is larger for the Ag-modified surface. These results are explained in terms of a change of the oxidation state of the surface Ag, which is able to acquire some of the extra surface electrons created by the oxygen vacancies and the adsorbed hydrogen atoms. Our findings provide new insights into the reactivity of Ag-modified ceria, which has been proposed as a promising alternative to platinum electrodes in electrochemical devices.

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

Investigating the Elusive Nature of Atomic O from CO 2 Dissociation on Pd(111): The Role of Surface Hydrogen

CO 2 dissociation is a key step in CO 2 conversion reactions to produce value-added chemicals typically through hydrogenation. In many cases, the atomic O produced from CO 2 dissociation can potentially block adsorption sites or change the oxidation state of the catalyst. Here, we used ambient pressure X-ray photoelectron spectroscopy (AP-XPS) and density functional theory (DFT) calculations to investigate the presence of surface species from the dissociation of CO 2 on Pd(111). AP-XPS results show that CO 2 was dissociated to produce adsorbed CO, but dissociated atomic O was not observed at room temperature. We were only able to observe atomic O when CO 2 was introduced at 500 K. Further investigations of O-covered Pd(111) revealed that chemisorbed O could be easily removed by low pressures of CO and H 2 . Notably, the effect of H 2 is quite prominent since it could react with chemisorbed O at a pressure as low as 2 × 10 -9 Torr, and the presence of H2 at ambient pressure prevented CO 2 dissociation. DFT calculations showed that in the presence of background H 2 , facile CO 2 dissociation took place via the reverse water–gas shift (rWGS) reaction, which resulted in the formation of adsorbed CO and removal of O by H 2 . DFT also identified the possible variation of surface species on simultaneous exposure of CO 2 and H 2 over Pd(111) depending on temperature and pressure, which opens alternative opportunities to tune the CO 2 hydrogenation catalysis by controlling the reaction conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Tuning Strong Metal–Support Interaction Kinetics on Pt-Loaded TiO 2 (110) by Choosing the Pressure: A Combined Ultrahigh Vacuum/Near-Ambient Pressure XPS Study

Pt catalyst particles on reducible oxide supports often change their activity significantly at elevated temperatures due to the strong metal–support interaction (SMSI), which induces the formation of an encapsulation layer around the noble metal particles. However, the impact of oxidizing and reducing treatments at elevated pressures on this encapsulation layer remains controversial, partly due to the “pressure gap” between surface science studies and applied catalysis. In the present work, we employ synchrotron-based near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) to study the effect of O 2 and H 2 on the SMSI-state of well-defined Pt/TiO 2 (110) catalysts at pressures of up to 0.1 Torr. Further, by tuning the O 2 pressure, we can either selectively oxidize the TiO 2 support or both the support and the Pt particles. Catalyzed by metallic Pt, the encapsulating oxide overlayer grows rapidly in 1 × 10 –5 Torr O 2 , but orders of magnitude less effectively at higher O 2 pressures, where Pt is in an oxidic state. While the oxidation/reduction of Pt particles is reversible, they remain embedded in the support once encapsulation has occurred.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Strain-Modified Raman Responses in Monolayer MoS 2 Nanobubbles Resolved at 5 nm

The formation of nanoscale bubbles is an unavoidable consequence during the transfer of two-dimensional materials onto target substrates, driven by van der Waals interactions at the interface. While often viewed as imperfections, these nanoscale bubbles have garnered considerable scientific interest due to the substantial in-plane strain gradients they induce, which in turn give rise to a variety of intriguing optoelectronic effects, particularly in semiconducting transition metal dichalcogenides. Determining and analyzing the strain distribution within nanobubbles at the nanoscale is crucial for advancing our understanding of these underlying strain-induced effects. Here, we present a high-resolution scanning tunneling microscopy-based tip-enhanced Raman spectroscopic investigation of localized nanoscale strain distribution within the nanobubbles formed between monolayer MoS 2 and Au interface. By employing cryogenic temperature (78 K), we successfully differentiate the nanoscale Raman signatures between nanobubble edge and pristine MoS 2 . We verify a maximum tensile strain of ∽1.15–1.34% at the nanobubble edge, which gradually diminishes toward the center, yielding a cross-sectional strain profile consistent with a doughnut-shaped distribution. Furthermore, we report to achieve ∽5 nm spatial resolution in probing such edge-localized strain within the nanobubble. In addition, comparative average strain analysis of such MoS 2 nanobubbles is conducted via geometric mechanistic analysis such as membrane and nonlinear plate theories, providing key insight into the geometric nature near the bubble edge. Our work provide fundamental information about strain-induced nanoscale chemical understanding of 2D materials on the nanometer scale, paving the way for practical applications of nanobubbles in strain-engineered optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Controlled Experiments and Optimized Theory of Absorption Spectra of Li Metal and Salts

Investigation of Li metal and ionic compounds through experimental and theoretical spectroscopy has been of tremendous interest due to their prospective applications in Li-metal and Li-ion batteries. Li K-edge soft X-ray absorption spectroscopy (sXAS) provides the most direct spectroscopic characterization; unfortunately, due to the low core-level energy and the highly reactive surface, Li-K sXAS of Li metal has been extremely challenging, as evidenced by many controversial reports. Here, through controlled and ultra-high energy resolution experiments of two kinds of in situ prepared samples, we report the intrinsic Li-K sXAS of Li-metal that displays a prominent leading peak that has not been revealed before. Furthermore, theoretical simulations show that, due to the low number of valence electrons in Li, the Li-K sXAS is strongly affected by the response of the valence electrons to the core hole. We successfully reproduce the Li-K sXAS by state-of-the-art calculations with considerations of a number of relevant parameters such as temperature, energy resolution, and, especially, contributions from transitions which are forbidden in the single-particle treatment. Such a comparative experimental and theoretical investigation is further extended to a series of Li ionic compounds, which highlight the importance of considering the total and single-particle energies for obtaining an accurate alignment of the spectra. Furthermore, our work provides the first reliable Li-K sXAS of the Li metal surface with advanced theoretical calculations. The experimental and theoretical results provide a critical benchmark for studying Li chemistry in both metallic and ionic states.

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

36 Hz integral linewidth laser based on a photonic integrated 4.0 m coil resonator

Laser stabilization sits at the heart of many precision scientific experiments and applications, including quantum information science, metrology, and atomic timekeeping. Many of these systems narrow the laser linewidth and stabilize the carrier by use of Pound–Drever–Hall (PDH) locking to a table-scale, ultrahigh quality factor (Q), vacuum spaced Fabry–Perot reference cavity. Integrating these cavities to bring characteristics of PDH stabilization to the chip scale is critical to reducing their size, cost, and weight, and enabling a wide range of portable and system-on-chip applications. We report a significant advance in integrated laser linewidth narrowing, stabilization, and noise reduction by use of a photonic integrated 4.0 m long coil resonator to stabilize a semiconductor laser. We achieve a 36 Hz 1 / π <#comment/> -integral linewidth, Allan deviation of 1.8 × <#comment/> 10 − <#comment/> 13 at 10 ms measurement time, and a 2.3 kHz/s drift—to the best of our knowledge, the lowest integral linewidth and highest stability demonstrated for an integrated waveguide reference cavity. This performance represents over an order of magnitude improvement in integral linewidth and frequency noise over previous integrated waveguide PDH stabilized reference cavities and bulk-optic and integrated injection locked approaches, and over two orders of magnitude improvement in frequency and phase noise than integrated injection locked approaches. Two different wavelength coil designs are demonstrated, stabilizing lasers at 1550 nm and 1319 nm. The resonator is bus-coupled to a 4.0 m long coil, with a 49 MHz free spectral range, mode volume of 1.0 × <#comment/> 10 10 µ <#comment/> m 3 , and 142 million intrinsic Q , fabricated in a CMOS compatible, ultralow loss silicon nitride waveguide platform. Our measurements and simulations show that the thermorefractive noise floor for this particular cavity is reached for frequencies down to 20 Hz in an ambient environment with simple passive vibration isolation and without vacuum or thermal isolation. The thermorefractive noise limited performance is estimated to yield an 8 Hz 1 / π <#comment/> -integral linewidth and Allan deviation of 5 × <#comment/> 10 − <#comment/> 14 at 10 ms, opening a stability regime that heretofore has been available only in fundamentally non-integrated systems. These results demonstrate the potential to bring the characteristics of laboratory-scale stabilized lasers to the integrated, wafer-scale compatible chip scale, and are of interest for a number of applications in quantum technologies and atomic, molecular, and optical physics, and with further developments below 10 Hz linewidth, can be highly relevant to ultralow noise microwave generation.

Liu, Kaikai (ORCID:0000000213609646)↗