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DOE OSTI2024

Determination of the mean energy of fast electron losses and anisotropies through thick-target emission on WEST

Abstract A new method to obtain the mean energy of fast electron losses in fusion plasmas using a versatile multi-energy hard x-ray (HXR) detector is presented. The method is based on measuring the thick-target emission of tungsten in the divertor region produced by fast electron losses interacting with the target and modeling the tungsten spectra by a Monte Carlo code which simulates the interaction between a beam of electrons and a solid target. The mean energy of the fast electron losses is determined through the comparison between the experimental and synthetic emission. The results show that fast electron losses during lower hybrid current drive discharges at WEST have a mean energy of 90–140 keV and represent only 2% of the total heat flux at the target. Additionally, anisotropic HXR emission has been detected for the first time at the WEST core and edge plasma, with opposite directions. It is due to the forward-peak emission of two distinctive populations of fast electrons: co-current fast electrons in the core and counter-current fast electron losses at the inner strike point. In view of future experiments like ITER where electron cyclotron current drive will generate a fast electron population, this technique could serve as a real-time monitor of fast electron losses and eventually feed an actuator on the current drive generation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Properties of states near 𝐸 𝑥 = 6 MeV in 18 Ne through 17 F +𝑝 scattering

The rate of energy production in the hot-CNO cycle and breakout to the rapid-proton capture process in Type I X-ray bursts is strongly related to the 14 O⁡(𝛼,𝑝)⁢ 17 F reaction rate. The properties of states in 18 Ne near 𝐸 𝑥 = 6.1–6.3 MeV are important for understanding the 14 O⁡(𝛼,𝑝)⁢ 17 F reaction rate. In order to study 18 Ne resonances around this energy region, the RESOLUT radioactive-ion beam facility at Florida State University was used to perform 17 F⁡(𝑝,𝑝)⁢ 17 F elastic scattering on a polypropylene target under inverse kinematics. Scattered protons were detected in a silicon-strip detector array while recoiling 17 F ions were detected in coincidence in a gas ionization detector. An 𝑅-matrix analysis of measured cross sections was conducted along with a reanalysis of data from previous 17 F +𝑝 measurements. All the data analyzed are well described by a consistent set of parameters with a 1 − assignment for a state at 6.14(1) MeV. A second comparable solution is also found with a 3 − assignment for the 6.14(1) MeV state. There is no conclusive evidence supporting one of the two solutions over the other. The rates of the 14 O⁡(𝛼,p)⁢ 17 F reaction that are determined from the two solutions differ by up to an order of magnitude.

6 ≤ A ≤ 19↗

DOE OSTI2026

Flavor, transverse momentum, and azimuthal dependence of charged pion multiplicities in semi-inclusive deep-inelastic scattering with 10.6 GeV electrons

Measurements of semi-inclusive deep-inelastic scattering multiplicities for 𝜋 + and 𝜋 − from proton and deuteron targets are reported on a grid of hadron kinematic variables 𝑧, 𝑃 𝑇 , and 𝜙* for leptonic kinematic variables in the range 0.3<𝑥<0.6 and 3<𝑄 2 <5GeV 2 . Data were acquired in 2018 and 2019 at Jefferson Lab Hall C with a 10.6 GeV electron beam impinging on 10-cm-long liquid hydrogen and deuterium targets. Scattered electrons and charged pions were detected in the High Momentum Spectrometer and Super High Momentum Spectrometer, respectively. The multiplicities were fitted for each bin in (𝑥,𝑄 2 ,𝑧,𝑃𝑡) to extract the 𝜙*—independent 𝑀 0 and the azimuthal modulations ⟨cos⁡(𝜙*)⟩ and ⟨cos⁡(2⁢𝜙*)⟩. The 𝑃𝑡 dependence of the 𝑀 0 results was found to be remarkably consistent for the four cases studied: 𝑒⁢𝑝→𝑒⁢𝜋 + ⁢𝑋, 𝑒⁢𝑝→𝑒⁢𝜋 − ⁢𝑋, 𝑒⁢𝑑→𝑒⁢𝜋 + ⁢𝑋, 𝑒⁢𝑑→𝑒⁢𝜋 − ⁢𝑋 over the range 0GeV<𝑃 𝑡 <0.4GeV, as were the multiplicities evaluated near 𝜙*=180∘ over the extended range 0GeV<𝑃 𝑡 <0.7GeV. The Gaussian widths of the 𝑃 𝑡 dependence exhibit a quadratic increase with 𝑧. The cos⁡(𝜙*) modulations were found to be consistent with zero for 𝜋 + , in agreement with previous world data, while the 𝜋 − moments were, in many cases, significantly greater than zero. The cos⁡(2⁢𝜙*) modulations were found to be consistent with zero. The higher statistical precision of this dataset of about 20 000 individual multiplicity values, compared with previously published data, should allow improved determinations of quark transverse momentum distributions and higher twist contributions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Battery data integrity and usability: Navigating datasets and equipment limitations for efficient and accurate research into battery aging

A tremendous commitment of resources is needed to acquire, understand and apply battery data in terms of performance and aging behavior. There are many state of performance (SOP) and state of health (SOH) metrics that are useful to guide alignment of batteries to end-use, yet how these metrics are measured or extracted can make the difference between usable, valuable datasets versus data that lacks the necessary integrity to meet baseline confidence levels for SOP/SOH quantification. This work will speak to 1) types of data that support SOP and SOH evaluations on mechanistic terms, 2) measurement conditions needed to assure high data integrity, 3) equipment limitations that can compromise data high fidelity, and 4) the impact of cell polarization on data quality. A common goal in battery research and field use is to work from a data platform that supports economical paths of data capture while minimizing down-time for battery diagnostics. An ideal situation would be to utilize data obtained during normal daily use (“pulses or cycles of convenience”) without stopping the daily duty cycles to perform dedicated SOP/SOH diagnostic routines. However, difficulties arise in trying to make use of daily duty cycle data (denoted as cycle-by-cycle, CBC) that underscores the need for standardization of conditions: temperature and duty cycles can vary over the course of a day and throughout a week, month and year; polarization can develop within an immediate cycle and throughout successive cycles as a hysteresis. If CBC data is envisioned as a data source to determine performance and aging trends, it should be recognized that polarization is a frequent consequence of CBC and thus makes it difficult to separate reversible and irreversible components to metrics such as capacity loss and resistance increase over aging. Since CBC conditions can have a major impact on data usability, we will devote part of this paper to CBC data conditioning and management. Differential analyses will also be discussed as a means to detect changing trends in data quality. Our target cell chemistries will be lithium-ion types NMC/graphite and LMO/LTO.

25 ENERGY STORAGE↗

DOE OSTI2024

Validation of the NOνA experiment 2023-tuning on simulated neutrino-matter interactions

NOνA is a long-baseline neutrino oscillation experiment that utilizes a two-detector design to study the oscillations of muon neutrinos into electron neutrinos over a baseline of 810 km. The Near Detector (ND) measures the neutrino beam spectrum and composition before oscillation, which is then compared to the oscillated neutrino energy spectrum observed in the Far Detector (FD). In the ND, the neutrinos are detected through their interactions with the heavy target nuclei within the detector. NOνA employs the GENIE neutrino event generator for simulating these neutrino-nucleus interactions. However, the default GENIE prediction does not adequately reproduce the ND data. To address this, NOνA developed a tune of the neutrino interaction models within GENIE version 3:0:6 to minimize discrepancies between the simulated predictions and the observed data in the ND. This dissertation tests the NOνA’s 2023 tune of the GENIE neutrino cross-section simulations by performing a data/simulations comparison for the ND. The analysis employed datasets comprising $2.55\times10^{21}$ protons-on-target (POT) in neutrino beam mode and $1.14\times10^{21}$ POT in antineutrino beam mode. The NOνA tuning of neutrino-matter interaction simulations matches with ND data within the $1\sigma$ error band, overestimating muon neutrino and antineutrino charged current interactions by approximately 6 % and 9 %, respectively. Discrepancies were observed in the energy region dominated by Quasi-Elastic-like interactions. Systematic uncertainties associated with the modeling of the neutrino cross-section, particularly those pertaining Quasi-Elastic like interactions, contributed considerably to the overall error in the simulations. Furthermore, the reconstruction algorithm used in NOνA for particle classification demonstrated significant misidentifications between charged pions and protons, as well as a tendency to overlook additional pions or protons in multi-particle simulated events.

Cortés Parra, Camilo Andrés↗

DOE OSTI2021

Scheduling strategies for the ESPRESSO follow-up of TESS targets

ABSTRACT Radial-velocity follow-up of stars harbouring transiting planets detected by TESS is expected to require very large amounts of expensive telescope time in the next few years. Therefore, scheduling strategies should be implemented to maximize the amount of information gathered about the target planetary systems. We consider myopic and non-myopic versions of a novel uniform-in-phase scheduler, as well as a random scheduler, and compare these scheduling strategies with respect to the bias, accuracy and precision achieved in recovering the mass and orbital parameters of transiting and non-transiting planets. This comparison is carried out based on realistic simulations of radial-velocity follow-up with ESPRESSO of a sample of 50 TESS target stars, with simulated planetary systems containing at least one transiting planet with a radius below 4R⊕. Radial-velocity data sets were generated under reasonable assumptions about their noise component, including that resulting from stellar activity, and analysed using a fully Bayesian methodology. We find the random scheduler leads to a more biased, less accurate, and less precise, estimation of the mass of the transiting exoplanets. No significant differences are found between the results of the myopic and non-myopic implementations of the uniform-in-phase scheduler. With only about 22 radial velocity measurements per data set, our novel uniform-in-phase scheduler enables an unbiased (at the level of 1 per cent) measurement of the masses of the transiting planets, while keeping the average relative accuracy and precision around 16 per cent and 23 per cent, respectively. The number of non-transiting planets detected is similar for all the scheduling strategies considered, as well as the bias, accuracy and precision with which their masses and orbital parameters are recovered.

Cabona, L.↗

DOE OSTI2023

First detection of the BAO signal from early DESI data

We present the first detection of the baryon acoustic oscillations (BAOs) signal obtained using unblinded data collected during the initial 2 months of operations of the Stage-IV ground-based Dark Energy Spectroscopic Instrument (DESI). From a selected sample of 261 291 luminous red galaxies spanning the redshift interval 0.4 < z < 1.1 and covering 1651 square degrees with a 57.9 per cent completeness level, we report a ∼5σ level BAO detection and the measurement of the BAO location at a precision of 1.7 per cent. Using a bright galaxy sample of 109 523 galaxies in the redshift range 0.1 < z < 0.5, over 3677 square degrees with a 50.0 per cent completeness, we also detect the BAO feature at ∼3σ significance with a 2.6 per cent precision. These first BAO measurements represent an important milestone, acting as a quality control on the optimal performance of the complex robotically actuated, fibre-fed DESI spectrograph, as well as an early validation of the DESI spectroscopic pipeline and data management system. Based on these first promising results, we forecast that DESI is on target to achieve a high-significance BAO detection at sub-per cent precision with the completed 5-yr survey data, meeting the top-level science requirements on BAO measurements. This exquisite level of precision will set new standards in cosmology and confirm DESI as the most competitive BAO experiment for the remainder of this decade.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Dark matter absorption via electronic excitations

We revisit the calculation of bosonic dark matter absorption via electronic excitations. Working in an effective field theory framework and consistently taking into account in-medium effects, we clarify the relation between dark matter and photon absorption. As is well-known, for vector (dark photon) and pseudoscalar (axion-like particle) dark matter, the absorption rates can be simply related to the target material’s optical properties. However, this is not the case for scalar dark matter, where the dominant contribution comes from a different operator than the one contributing to photon absorption, which is formally next-to-leading-order and does not suffer from in-medium screening. It is therefore imperative to have reliable first-principles numerical calculations and/or semi-analytic modeling in order to predict the detection rate. We present updated sensitivity projections for semiconductor crystal and superconductor targets for ongoing and proposed direct detection experiments.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2026

Polarized target nuclear magnetic resonance measurements with deep neural networks

Continuous-wave Nuclear Magnetic Resonance (CW-NMR) operated in constant-current mode has served as a foundational technique for polarization measurement in solid-state dynamically polarized targets within nuclear and high-energy physics experiments for several decades, and it remains an essential tool. Conventional Q-meter-based phase-sensitive detection is critical for precise real-time determination of target polarization during scattering runs. However, the accuracy and reliability of these measurements are frequently compromised by elevated noise levels, baseline drift, and systematic uncertainties arising from signal isolation and fitting, ultimately degrading the overall experimental figure of merit. In this work, we report the first successful application of neural network architectures to continuous-wave NMR polarization metrology. By leveraging advanced machine learning techniques for signal extraction and denoising, we achieve a substantial reduction of fitting uncertainties under a variety of realistic simulated and experimental conditions. These improvements translate directly into more robust real-time (online) polarization monitoring and higher precision in subsequent offline analysis. By reducing analysis-induced uncertainty, the resulting methodology can improve the effective figure of merit for scattering experiments employing dynamically polarized targets and provides a new toolset for NMR-based polarimetry in high-energy and nuclear physics.

Metrology↗

DOE OSTI2023

Prompt Photofission Neutron Detection in Depleted Uranium

The detection of prompt photofission neutrons during active interrogation is a strong indication of the presence of special nuclear materials. However, the high-energy photons used for interrogation create a very challenging radiation environment for the detection of prompt fission signatures. These challenges include detector saturation and pulse pile-up. Additionally, there is an elevated neutron background that further challenges the detection of prompt fission neutrons. This background is produced because of (γ, Xn) photonuclear reactions in the surrounding high-Z materials. Here, we demonstrate the detection of prompt photofission neutrons in these challenging environments. Depleted uranium (DU) and lead targets are interrogated with bremsstrahlung photons produced by a 9-MV electron linear accelerator. Fast neutrons are detected with trans-stilbene organic detectors, and scintillation pulses are analyzed using a previously developed and demonstrated artificial neural network system. We observe a 5 times higher photoneutron count rate when the lead target is replaced with the DU target. Additionally, we observe a difference in the photoneutron light-output distributions of lead and DU. Here, this difference in the measured distributions is due to the difference in the photoneutron-energy spectra; DU photoneutrons are emitted with (γ, n) and watt-energy spectra, whereas lead photoneutrons are emitted with only the (γ, n) spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Astrometric gravitational-wave detection via stellar interferometry

Here, we evaluate the potential for gravitational-wave (GW) detection in the frequency band from 10 nHz to 1 μ Hz using extremely high-precision astrometry of a small number of stars. In particular, we argue that nonmagnetic, photometrically stable, hot white dwarfs (WD) located at ~kpc distances may be optimal targets for this approach. Previous studies of astrometric GW detection have focused on the potential for less precise surveys of large numbers of stars; our work provides an alternative optimization approach to this problem. Interesting GW sources in this band are expected at characteristic strains around h c ~10 -17 × (μHz/ $f$ GW ). The astrometric angular precision required to see these sources is Δθ~h c after integrating for a time T~1/$f$GW. We show that jitter in the photometric center of WD of this type due to starspots is bounded to be small enough to permit this high-precision, small-N approach. We discuss possible noise arising from stellar reflex motion induced by orbiting objects and show how it can be mitigated. The only plausible technology able to achieve the requisite astrometric precision is a space-based stellar interferometer. Such a future mission with few-meter-scale collecting dishes and baselines of $\mathscr{O}$(100 km ) is sufficient to achieve the target precision. This collector size is broadly in line with the collectors proposed for some formation-flown, space-based astrometer or optical synthetic-aperture imaging-array concepts proposed for other science reasons. The proposed baseline is however somewhat larger than the km-scale baselines discussed for those concepts, but we see no fundamental technical obstacle to utilizing such baselines. A mission of this type thus also holds the promise of being one of the few ways to access interesting GW sources in this band.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Quantum-enhanced detection of viral cDNA via luminescence resonance energy transfer using upconversion and gold nanoparticles

Abstract The COVID-19 pandemic has profoundly impacted global economies and healthcare systems, revealing critical vulnerabilities in both. In response, our study introduces a sensitive and highly specific detection method for cDNA, leveraging Luminescence Resonance Energy Transfer (LRET) between upconversion nanoparticles (UCNPs) and gold nanoparticles (AuNPs), and achieves a detection limit of 242 fM for SARS-CoV-2 cDNA. This innovative sensing platform utilizes UCNPs conjugated with one primer and AuNPs with another, targeting the 5′ and 3′ ends of the SARS-CoV-2 cDNA, respectively, enabling precise differentiation of mismatched cDNA sequences and significantly improving detection specificity. Through rigorous experimental analysis, we established a quenching efficiency range from 10.4 % to 73.6 %, with an optimal midpoint of 42 %, thereby demonstrating the superior sensitivity of our method. Our work uses SARS-CoV-2 cDNA as a model system to demonstrate the potential of our LRET-based detection method. This proof-of-concept study highlights the adaptability of our platform for future diagnostic applications. Instrumental validation confirms the synthesis and formation of AuNPs, addressing the need for experimental verification of the preparation of nanomaterial. Our comparative analysis with existing SARS-CoV-2 detection methods revealed that our approach provides a low detection limit and high specificity for target cDNA sequences, underscoring its potential for targeted COVID-19 diagnostics. This study demonstrates the superior sensitivity and adaptability of using UCNPs and AuNPs for cDNA detection, offering significant advances in rapid, accessible diagnostic technologies. Our method, characterized by its low detection limit and high precision, represents a critical step forward in developing next-generation biosensors for managing current and future viral outbreaks. By adjusting primer sequences, this platform can be tailored to detect other pathogens, contributing to the enhancement of global healthcare responsiveness and infectious disease control.

Esmaeili, Shahriar [Institute for Quantum Science ↗

DOE OSTI2025

Vertical column dual-comb spectroscopy to a TBS

Open-path dual-frequency-comb spectroscopy (DCS) is a broadband, high spectral resolution, and high precision method for measuring gas concentrations over kilometer-scale paths. It has been used for detection and quantification of emissions of pollutants, hazardous gasses, and greenhouse gasses (GHGs). DCS has been shown to measure trace-gas mixing ratios with 0.14%-0.4% agreement between instruments. To achieve high signal-to-noise ratios (SNRs) with DCS, comb light is targeted onto a retroreflector at the end of the measurement path, which returns the signal to a detector co-located with the launch signal. Installing the retroreflector on a mobile platform such as a balloon or unmanned aerial vehicle (UAV) extends the capabilities of DCS by enabling variable path lengths, greater mobility, and access to higher altitudes. Mobile-target DCS has many uses in plume and leak detection, emissions modeling, and planetary boundary layer (PBL) studies. It is a promising method for observing vertical distributions of GHGs and mixing processes in the PBL, which are difficult to measure but important for pollution and climate monitoring as well as for understanding transport of gasses through the atmosphere. Tethered balloons are an intriguing platform because they enable longer flight durations and higher altitudes than easily obtainable with a UAV and thus allow for column measurements up to and above the PBL. New measurements completed in October/November 2024 reach the highest altitudes above ground level yet achieved by mobile-target DCS. For these measurements, the retroreflector was mounted on a 7 m diameter tethered helium balloon. An actively tracking gimbal on the ground holds the DCS launch telescope and keeps the 5 cm beam pointed onto the retroreflector while the balloon is lifted, lowered, and moved by wind and turbulence.

atmosphere↗

DOE OSTI2022

Characterizing Heterogeneous Mixtures of Assembled States of the Tobacco Mosaic Virus Using Charge Detection Mass Spectrometry

The tobacco mosaic viral capsid protein (TMV) is a frequent target for derivatization for myriad applications, including drug delivery, biosensing, and light harvesting. However, solutions of the stacked disk assembly state of TMV are difficult to characterize quantitatively due to their large size and multiple assembled states. Charge detection mass spectrometry (CDMS) addresses the need to characterize heterogeneous populations of large protein complexes in solution quickly and accurately. Using CDMS, previously unobserved assembly states of TMV, including 16-monomer disks and odd-numbered disk stacks, have been characterized. We additionally employed a peptide-protein conjugation reaction in conjunction with CDMS to demonstrate that modified TMV proteins do not redistribute between disks. Finally, this technique was used to discriminate between protein complexes of near-identical mass but different configurations. In conclusion, we have gained a greater understanding of the behavior of TMV, a protein used across a broad variety of fields and applications, in the solution state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Emerging Per- and Polyfluoroalkyl Substances in Tap Water from the American Healthy Homes Survey II

Humans experience widespread exposure to anthropogenic per- and polyfluoroalkyl substances (PFAS) through various media, which can lead to a wide range of negative health impacts. Tap water is an important source of exposure in communities with any degree of contamination but routine or large-scale PFAS monitoring often depends on targeted analytical methods limited to measuring specific PFAS. We analyzed 680 tap water samples from the American Healthy Homes Survey II for PFAS using non-targeted analysis (NTA) to expand the range of detectable PFAS. Based on detection frequency and relative abundance, about half of the identified PFAS were found only by NTA. We identified (with varying degrees of confidence) 75 distinct PFAS, including 57 exclusively detected by NTA. The identified PFAS are members of seven structural subclasses differentiated by their head groups and degree of fluorination. Clustering analysis categorized the PFAS into four coabundance groups dominated by specific PFAS subclasses. One group uniquely identified by NTA contains zwitterionic PFAS and other PFAS transformation products which are likely associated with aqueous firefighting foam contaminants in a small number of spatially correlated samples. These results help further characterize the scope of exposure to emerging PFAS experienced by the U.S. population via tap water and augment nationwide targeted-PFAS monitoring programs.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

DOE OSTI2025

Measurement of the Neutron Electromagnetic Form Factors at High Momentum Transfer Using a Polarized 3He Target at Jefferson Lab

Ever since the composite structure of nucleons was uncovered, many experiments have been commissioned with the purpose of extracting parameters that shape our understanding of this structure. Form factors are powerful tools that rest at the forefront of the nucleon structure study. In the non-relativistic limit, they describe the magnetic and charge distributions inside the nucleon. The GEn-II experiment, which ran in Hall A of Jefferson Lab as a part of the SuperBigbite Spectrometer (SBS) program, aimed to extract the ratio of the neutron’s electric to magnetic Sachs form factors (GnE/GnM. This was accomplished using the double polarization technique: scattering polarized electrons with initial energies up to 8.45 GeV off high-density polarized 3He targets. The experiment was a coincidence measurement, with the scattered electrons detected in the BigBite Spectrometer and the recoil nucleons in a hadron calorimeter, a part of the SuperBigbite Spectrometer. The convection-style target cells used in this experiment have a 60cm long target chamber, an increase from the 40 cm cell used in the most recent polarized 3He target experiment. In addition, the cells were optically pumped from two sides of the pumping chamber. These improvements in design and functionality introduced world-record-breaking luminosity. This thesis presents preliminary results of the GEn-II experiment for the following 4-momentum transfer (Q2) values: 2.93, 6.76, and 9.78 GeV2, in addition to target performance and preliminary polarimetry results.

Presley, Hunter [Univ. of Virginia, Charlottesvill↗

DOE OSTI2022

Source-agnostic gravitational-wave detection with recurrent autoencoders

Abstract We present an application of anomaly detection techniques based on deep recurrent autoencoders (AEs) to the problem of detecting gravitational wave (GW) signals in laser interferometers. Trained on noise data, this class of algorithms could detect signals using an unsupervised strategy, i.e. without targeting a specific kind of source. We develop a custom architecture to analyze the data from two interferometers. We compare the obtained performance to that obtained with other AE architectures and with a convolutional classifier. The unsupervised nature of the proposed strategy comes with a cost in terms of accuracy, when compared to more traditional supervised techniques. On the other hand, there is a qualitative gain in generalizing the experimental sensitivity beyond the ensemble of pre-computed signal templates. The recurrent AE outperforms other AEs based on different architectures. The class of recurrent AEs presented in this paper could complement the search strategy employed for GW detection and extend the discovery reach of the ongoing detection campaigns.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Peptoid-Based Programmable 2D Nanomaterial Sensor for Selective and Sensitive Detection of H 2 S in Live Cells

During the past decades, a variety of two-dimensional (2D) nanosheets have been developed through supramolecular self-assembly. Among them, those assembled from sequence-defined molecules have received particularly attention because they enable a precise displaying of functional groups, including fluorescent dyes, within nanosheet surfaces. On the other hand, due to the fluorescence self-quenching, synthesis of organic 2D nanosheets exhibiting high fluorescence quantum yields is a significant challenge. Herein, we report the utilization of H 2 S-responsive probes as peptoid sidechains to design and synthesize crystalline 2D nanomembranes (2DNMs) as selective and sensitive H 2 S sensors. These 2DNM sensors exhibit a high quantum yield as a result of high crystallinity and tunable probe density. Compared with amorphous state of peptoid assembly and pre-assembled peptoid-probe conjugates, these crystalline 2DNM sensors exhibit a significantly strong fluorescence intensity and a high sensitivity (~ 0.36 nM). By sonication-cutting these 2DNM sensors into a colloidal form in aqueous solution, we further demonstrated the use of colloidal 2DNMs for detecting both exogenous and endogenous H 2 S inside cells or targeted cell organelles. As far as we know, this is the first example of using sequence-defined 2D nanomaterials for selective and sensitive detection of H 2 S. Because peptoids are biocompatible and peptoid-based 2DNMs are highly programmable, we expect that this new class of 2DNM sensors offer great potentials for detecting H 2 S and for biological applications.

2D nanomaterials↗