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DOE OSTI2025

Annihilation-limited long-range exciton transport in high-mobility conjugated copolymer films

A combination of ultrafast, long-range, and low-loss excitation energy transfer from the photoreceptor location to a functionally active site is essential for cost-effective polymeric semiconductors. Delocalized electronic wavefunctions along π-conjugated polymer (CP) backbone can enable efficient intrachain transport, while interchain transport is generally thought slow and lossy due to weak chain–chain interactions. In contrast to the conventional strategy of mitigating structural disorder, amorphous layers of rigid CPs, exemplified by highly planar poly(indacenodithiophene-co-benzothiadiazole) (IDT-BT) donor-accepter copolymer, exhibit trap-free transistor performance and charge-carrier mobilities similar to amorphous silicon. Here, we report long-range exciton transport in HJ -aggregated IDTBT thin-film, in which the competing exciton transport and exciton–exciton annihilation (EEA) dynamics are spectroscopically separated using a phase-cycling-based scheme and shown to depart from the classical diffusion-limited and strong-coupling regime. In the thin film, we find an annihilation-limited mechanism with ≪100% per-encounter annihilation probability, facilitating the minimization of EEA-induced excitation losses. In contrast, excitons on isolated IDTBT chains diffuse over 350 nm with 0.56 cm 2 s −1 diffusivity, before eventually annihilating with unit probability on first contact. We complement the pump–probe studies with temperature-dependent photocurrent and EEA measurements from 295 K to 77 K and find a remarkable correspondence of annihilation rate and photocurrent activation energies in the 140 K to 295 K temperature range.

Shi, Yuping (ORCID:0000000318289415)↗

DOE OSTI2020

Warming nuclear pasta with dark matter: kinetic and annihilation heating of neutron star crusts

Neutron stars serve as excellent next-generation thermal detectors of dark matter, heated by the scattering and annihilation of dark matter accelerated to relativistic speeds in their deep gravitational wells. However, the dynamics of neutron star cores are uncertain, making it difficult at present to unequivocally compute dark matter scattering in this region. On the other hand, the physics of an outer layer of the neutron star, the crust, is more robustly understood. We show that dark matter scattering solely with the low-density crust still kinetically heats neutron stars to infrared temperatures detectable by forthcoming telescopes. We find that for both spin-independent and spin-dependent scattering on nucleons, the crust-only cross section sensitivity is 10 -43 - 10 -41 cm 2 for dark matter masses of 100 MeV - 1 PeV, with the best sensitivity arising from dark matter scattering with a crust constituent called nuclear pasta (including gnocchi, spaghetti, and lasagna phases). For dark matter masses from 10 eV to 1 MeV, the sensitivity is 10 -39 - 10 -34 cm 2 , arising from exciting collective phonon modes in a neutron superfluid in the inner crust. Furthermore, for any s-wave or p-wave annihilating dark matter, we show that dark matter will efficiently annihilate by thermalizing just with the neutron star crust, regardless of whether the dark matter ever scatters with the neutron star core. This implies efficient annihilation in neutron stars for any electroweakly interacting dark matter with inelastic mass splittings of up to 200 MeV, including Higgsinos. We conclude that neutron star crusts play a key role in dark matter scattering and annihilation in neutron stars.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Split Ga vacancies and the unusually strong anisotropy of positron annihilation spectra in β–Ga 2 O 3

We report a systematic first-principles study on positron annihilation parameters in the β–Ga 2 O 3 lattice and Ga monovacancy defects complemented with orientation-dependent experiments of the Doppler broadening of the positron-electron annihilation. We find that both the β–Ga 2 O 3 lattice and the considered defects exhibit unusually strong anisotropy in their Doppler broadening signals. This anisotropy is associated with low symmetry of the β–Ga 2 O 3 crystal structure that leads to unusual kind of one-dimensional confinement of positrons even in the delocalized state in the lattice. In particular, the split Ga vacancies recently observed by scanning transmission electron microscopy produce unusually anisotropic positron annihilation signals. Furthermore, we show that in experiments, the positron annihilation signals in β–Ga 2 O 3 samples seem to be often dominated by split Ga vacancies.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Substrate-Dependent Exciton Diffusion and Annihilation in Chemically Treated MoS 2 and WS 2

Atomically thin semiconductors such as monolayer MoS 2 and WS 2 exhibit nonlinear exciton–exciton annihilation at notably low excitation densities (below ~10 excitons/μm 2 in exfoliated MoS 2 ). In this work, we show that the density threshold at which annihilation occurs can be tuned by changing the underlying substrate. When the supporting substrate is changed from SiO 2 to Al 2 O 3 or SrTiO 3 , the rate constant for second-order exciton–exciton annihilation, k XX [cm 2 /s], is reduced by 1 or 2 orders of magnitude, respectively. Using transient photoluminescence microscopy, we measure the effective room-temperature exciton diffusion coefficient in bis(trifluoromethane)sulfonimide-treated MoS 2 to be in the range D = 0.03–0.06 cm 2 /s, corresponding to a diffusion length of L D = 350 nm for an exciton lifetime of τ = 18 ns, which does not depend strongly on the substrate. We discuss possible mechanisms for the observed behavior, including substrate permittivity, long-range exciton–exciton or exciton–charge interactions, defect-mediated Auger recombination, and spatially inhomogeneous exciton populations arising from substrate-induced disorder. Exciton annihilation limits the overall efficiency of 2D semiconductor devices operating at high exciton densities; the ability to tune these interactions via the underlying substrate is an important step toward more efficient optoelectronic technologies featuring atomically thin materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Probing exciton diffusion dynamics in photosynthetic supercomplexes via exciton–exciton annihilation

Photosynthesis converts solar energy into chemical energy through coordinated energy transfer between light-harvesting complexes and reaction centers (RCs). Understanding exciton motion, particularly the exciton diffusion length, is essential for optimizing energy efficiency in photosystems. In this work, we combine intensity-cycling transient absorption spectroscopy with kinetic Monte Carlo (kMC) simulation to investigate exciton motion in the C2S2 photosystem II supercomplex of spinach. Using exciton–exciton annihilation, revealed in the fifth-order response, we experimentally estimate an exciton diffusion length of 10.9 nm based on a 3D normal diffusion model, suggesting the ability of excitons to traverse the supercomplex. However, kMC simulations reveal that exciton motion is sub-diffusive because of spatial constraints and the strong RC traps. An anomalous diffusion model analysis of the experimental data yields a diffusion length of 9.7 nm, while the simulated diffusion length is 7.4 nm. The variable exciton residence time across subunits, partly influenced by their connectivity to the trap, indicates inhomogeneous annihilation probability and suggests how plants balance efficient light harvesting with photoprotection. We also explore the influence of specific assumptions in the annihilation simulation, which are challenging to access in more complex environments, such as the thylakoid membrane. Our study provides a framework for studying exciton dynamics using exciton–exciton annihilation, which can be extended to understand the light-harvesting efficiencies of larger, more complex photosynthetic assemblies.

Zhang, Kunyan (ORCID:000000026830409X)↗

DOE OSTI2022

Searching for velocity-dependent dark matter annihilation signals from extragalactic halos

For this work, we consider gamma-ray signals of dark matter annihilation in extragalactic halos in the case where dark matter annihilates from a p-wave or d-wave state. In these scenarios, signals from extragalactic halos are enhanced relative to other targets, such as the Galactic Center or dwarf spheroidal galaxies, because the typical relative speed of the dark matter is larger in extragalactic halos. We perform a mock data analysis of gamma rays produced by dark matter annihilation in halos detected by the Sloan Digital Sky Survey. We include a model for uncorrelated galactic and extragalactic gamma ray backgrounds, as well as a simple model for backgrounds due to astrophysical processes in the extragalactic halos detected by the survey. We find that, for models which are still allowed by other gamma ray searches, searches of extragalactic halos with the current Fermi exposure can produce evidence for dark matter annihilation, though it is difficult to distinguish the p-wave and d-wave scenarios. With a factor 10x larger exposure, though, discrimination of the velocity-dependence is possible.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Antiproton bounds on dark matter annihilation from a combined analysis using the DRAGON2 code

Abstract Early studies of the AMS-02 antiproton ratio identified a possible excess over the expected astrophysical background that could be fit by the annihilation of a weakly interacting massive particle (WIMP). However, recent efforts have shown that uncertainties in cosmic-ray propagation, the antiproton production cross-section, and correlated systematic uncertainties in the AMS-02 data, may combine to decrease or eliminate the significance of this feature. We produce an advanced analysis using the DRAGON2 code which, for the first time, simultaneously fits the antiproton ratio along with multiple secondary cosmic-ray flux measurements to constrain astrophysical and nuclear uncertainties. Compared to previous work, our analysis benefits from a combination of: (1) recently released AMS-02 antiproton data, (2) updated nuclear fragmentation cross-section fits, (3) a rigorous Bayesian parameter space scan that constrains cosmic-ray propagation parameters.We find no statistically significant preference for a dark matter signal and set strong constraints on WIMP annihilation tobb̅, ruling out annihilation at the thermal cross-section for dark matter masses below ∼ 200 GeV. We do find a positive residual that is consistent with previous work, and can be explained by a ∼ 70 GeV WIMP annihilating below the thermal cross-section. However, our default analysis finds this excess to have a local significance of only 2.8σ, which is decreased to 1.8σwhen the look-elsewhere effect is taken into account.

Astronomy & Astrophysics↗

DOE OSTI2025

Relaxing constraints on dark matter annihilation near the supermassive black hole in M87

The supermassive black hole at the center of M87 could redistribute dark matter particles within its sphere of influence, creating a high-density region known as a density spike. This spike can significantly enhance dark matter annihilation signals, making M87 a critical target for deriving stringent constraints on annihilation cross sections. In this work, we demonstrate that these constraints are highly sensitive to the choice of the halo density profile for M87. Motivated by recent kinematic studies of M87, we adopt a cored halo model and find that the constraints on dark matter annihilation are significantly relaxed. Specifically, in the cored halo scenario, the smooth part of the halo overwhelmingly dominates the annihilation signals, whereas the commonly assumed cuspy halo model attributes a major contribution to the spike. We demonstrate this effect using a dark matter model with a light mediator.

particle dark matter↗

DOE OSTI2020

Effective J -factors for Milky Way dwarf spheroidal galaxies with velocity-dependent annihilation

We calculate the effective J-factors, which determine the strength of indirect detection signals from dark matter annihilation, for 25 dwarf spheroidal galaxies (dSphs). We consider several well-motivated assumptions for the relative velocity dependence of the dark matter annihilation cross section: σAv: s -wave (velocity independent), p -wave (σ A v∝v 2 ), d-wave (σ A v∝v 4 ), and Sommerfeld-enhancement in the Coulomb limit (σ A v∝1/v). As a result we provide the largest and most updated sample of J-factors for velocity-dependent annihilation models. For each scenario, we use Fermi-LAT gamma-ray data to constrain the annihilation cross section. Due to the assumptions made in our gamma-ray data analysis, our bounds are comparable to previous bounds on both the p-wave and Sommerfeld-enhanced cross sections using dSphs. Finally, our bounds on the d-wave cross section are the first such bounds using indirect detection data.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Combined search for neutrinos from dark matter self-annihilation in the Galactic Center with ANTARES and IceCube

In this work, we present the results of the first combined dark matter search targeting the Galactic Centre using the ANTARES and IceCube neutrino telescopes. For dark matter particles with masses from 50 to 1000 GeV, the sensitivities on the self-annihilation cross section set by ANTARES and IceCube are comparable, making this mass range particularly interesting for a joint analysis. Dark matter self-annihilation through the $\tau^+\tau^-$, $\mu^+\mu^-$, $b\bar{b}$ and $W^+W^-$ channels is considered for both the Navarro-Frenk-White and Burkert halo profiles. In the combination of 2,101.6 days of ANTARES data and 1,007 days of IceCube data, no excess over the expected background is observed. Limits on the thermally-averaged dark matter annihilation cross section $\langle\sigma_A\upsilon\rangle$ are set. These limits present an improvement of up to a factor of two in the studied dark matter mass range with respect to the individual limits published by both collaborations. When considering dark matter particles with a mass of 200 GeV annihilating through the $\tau^+\tau^-$ channel, the value obtained for the limit is $7.44 \times 10^{-24} \text{cm}^{3}\text{s}^{-1}$ for the Navarro-Frenk-White halo profile. For the purpose of this joint analysis, the model parameters and the likelihood are unified, providing a benchmark for forthcoming dark matter searches performed by neutrino telescopes.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Optimal observing strategies for velocity-suppressed dark matter annihilation

Numerous particle models for the cosmological dark matter feature a pair-annihilation rate that scales with powers of the relative velocity between the annihilating particles. As a result, the annihilation rate in the central regions of a dark matter halo can be significantly lower than at the halo’s periphery for particular ambient gravitational potentials. While this might be offset by an increasing dark matter pair number density in the inner halo, it raises the question; what angular region for dark matter models with velocity-suppressed annihilation rates optimizes the signal to noise ratio? We consider simplified background models for galactic and extragalactic targets and demonstrate that the optimal observing strategy varies greatly case by case. Generally, a bright central source warrants an annular region of interest, while a flatter background warrants as large as possible an angular region, possibly including the central regions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Search for neutrino lines from dark matter annihilation and decay with IceCube

Dark matter particles in the Galactic Center and halo can annihilate or decay into a pair of neutrinos producing a monochromatic flux of neutrinos. The spectral feature of this signal is unique and it is not expected from any astrophysical production mechanism. Its observation would constitute a dark matter smoking gun signal. Here we performed the first dedicated search with a neutrino telescope for such signal, by looking at both the angular and energy information of the neutrino events. To this end, a total of five years of IceCube’s DeepCore data has been used to test dark matter masses ranging from 10 GeV to 40 TeV. No significant neutrino excess was found and upper limits on the annihilation cross section, as well as lower limits on the dark matter lifetime, were set. The limits reached are of the order of 10 -24 cm 3 /s for an annihilation and up to 10 27 s for decaying dark matter. Using the same data sample we also derive limits for dark matter annihilation or decay into a pair of Standard Model charged particles.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Edge-Mediated Annihilation of Vacancy Clusters in Monolayer Molybdenum Diselenide (MoSe 2 ) under Electron Beam Irradiation

Here annihilation of vacancy clusters in monolayer molybdenum diselenide (MoSe2) under electron beam irradiation is reported. In situ high-resolution transmission electron microscopy observation reveals that the annihilation is achieved by diffusion of vacancies to the free edge near the vacancy clusters. Monte Carlo simulations confirm that it is energetically favorable for the vacancies to locate at the free edge. By computing the minimum energy path for the annihilation of one vacancy cluster as a case study, it is further shown that electron beam irradiation and pre-stress in the suspended MoSe2 monolayer are necessary for the vacancies to overcome the energy barriers for diffusion. The findings suggest a new mechanism of vacancy healing in 2D materials and broaden the capability of electron beam for defect engineering of 2D materials, a promising way of tuning their properties for engineering applications.

2D materials↗

DOE OSTI2024

Limits on dark matter annihilation from the shape of radio emission in M31

Well-motivated models of dark matter often result in a population of electrons and positrons within galaxies produced through dark matter annihilation — usually in association with gamma rays. As they diffuse through galactic magnetic fields, these e ± produce synchrotron radio emission. The intensity and morphology of this signal depends on the properties of the interstellar medium through which the e ± propagate. Using observations of the Andromeda Galaxy (M31) to construct a model of the gas, magnetic fields, and starlight, we set constraints on dark matter annihilation to b$\overline{b}$ using the morphology of 3.6 cm radio emission. As the emission signal at the center of M31 is very sensitive to the diffusion coefficient and dark matter profile, we base our limits on the differential flux in the region between 0.9 – 6.9 kpc from the center. We exclude annihilation cross sections ≳ 3 × 10 −25 cm 3 /s in the mass range 10 – 500 GeV, with a maximum sensitivity of 7 × 10 −26 cm 3 /s at 20 – 40 GeV. Though these limits are weaker than those found in previous studies of M31, they are robust to variations of the diffusion coefficient.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

The Impact of Carotenoid Energy Levels on the Exciton Dynamics and Singlet–Triplet Annihilation in Isolated Bacterial Light-Harvesting 2 Complexes

The light-harvesting 2 (LH2) complex of purple phototrophic bacteria plays a critical role in absorbing solar energy and distributing the excitation energy. Exciton dynamics within LH2 complexes are controlled by the structural arrangement and energy levels of the bacteriochlorophyll (BChl) and carotenoid (Car) pigments. However, there is still debate over the competing light-harvesting versus energy-dissipation pathways. In this work, we compared five variants of the LH2 complex from genetically modified strains of Rhodobacter sphaeroides, all containing the same BChls but different Cars with increasing conjugation: zeta-carotene (N = 7; LH2 Zeta ), neurosporene (N = 9; LH2 Neu ), spheroidene (N = 10; LH2 Spher ), lycopene (N = 11; LH2 Lyco ), and spirilloxanthin (N = 13; LH2 Spir ). Absorption measurements confirmed that the Car excited-state energy decreased with increasing conjugation. Similarly, fluorescence spectra showed that the B850 BChl emission peak had an increasing red shift from LH2 Zeta →(LH2 Neu /LH2 Spher )→LH2 Lyco →LH2 Spir . In contrast, time-resolved fluorescence and ultrafast transient absorption (fs-TA) revealed similar excited-state lifetimes (∼1 ns) for all complexes except LH2 Spir (∼0.7 ns). From fs-TA analysis, an additional ∼7 ps nonradiative dissipation step from B850 BChl was observed for LH2 Zeta . Further, singlet− singlet and singlet−triplet annihilation studies showed a ∼50% average fluorescence lifetime reduction in LH2Zeta at high laser power and high repetition rate, compared to ∼10−15% reductions in LH2 Neu /LH2 Spher /LH2 Lyco and minimal lifetime change in LH2 Spir . In LH2 Zeta , the fastest decay component (<50 ps) became prominent at high repetition rates, consistent with strong singlet−triplet annihilation. Nanosecond TA measurements revealed long-lived (>40 μs) BChl triplet states in LH2 Zeta and signs of damage caused by singlet oxygen, whereas other LH2s showed faster triplet quenching (∼18 ns) by Cars. These findings highlight a key design principle of LH2 complexes: the Car triplet energy must be significantly lower than the BChl triplet energy to efficiently quench BChl triplets that otherwise act as potent “trap states,” causing exciton annihilation in laser-based experiments or photodamage in native membranes.

Absorption↗

DOE OSTI2021

Understanding kinetics of defect annihilation in chemoepitaxy-directed self-assembly.

Directed self-assembly (DSA) of block copolymers (BCP) has attracted considerable interest from the semiconductor industry because it can achieve semiconductor-relevant structures with a relatively simple process and low cost. However, the self-assembling structures can become kinetically trapped into defective states, which greatly impedes the implementation of DSA in high-volume manufacturing. Understanding the kinetics of defect annihilation is crucial to optimizing the process and eventually eliminating defects in DSA. Such kinetic experiments, however, are not commonly available in academic laboratories. To address this challenge, we perform a kinetic study of chemoepitaxy DSA in a 300 mm wafer fab, where the complete defectivity information at various annealing conditions can be readily captured. Through extensive statistical analysis, we reveal the statistical model of defect annihilation in DSA for the first time. The annihilation kinetics can be well described by a power law model, indicating that all dislocations can be removed by sufficiently long annealing time. We further develop image analysis algorithms to analyze the distribution of dislocation size and configurations and discover that the distribution stays relatively constant over time. The defect distribution is determined by the role of the guiding stripe, which is found to stabilize the defects. Although this study is based on polystyrene-b-poly(methyl methacrylate) (PS-b-PMMA), we anticipate that these findings can be readily applied to other BCP platforms as well.

block copolymer↗

DOE OSTI2026

Spontaneous Polarization Suppression of Exciton–Exciton Annihilation in Rhombohedral-Stacked Bilayer Molybdenum Disulfide

Rapid exciton–exciton annihilation (EEA) in two-dimensional semiconductors limits access to high-density excitonic regimes essential for efficient optoelectronic operation under strong excitation. Here, we show that EEA is strongly suppressed in rhombohedral (3R)-stacked MoS 2 bilayers relative to nonpolar 2H bilayers, and that this suppression is quantitatively consistent with repulsive dipole–dipole interactions between layer-polarized excitons induced by spontaneous polarization. Using ultrafast pump–probe spectroscopy, we measure an EEA rate of γ EEA = (5.03 ± 0.99) × 10 –3 cm 2 s –1 in 3R bilayers, which is approximately 18.2-fold smaller than that in monolayers and 2.9-fold smaller than that in nonpolar 2H bilayers. Despite the higher exciton diffusivity recently reported for 3R relative to 2H bilayers, the reduced EEA rate in 3R indicates a rate-limited regime governed by the close-encounter annihilation probability rather than diffusion. A rate-limited annihilation model incorporating a dipole–dipole repulsive potential captures the observed ratio γ EEA,3R /γ EEA,2H ≈ 0.35 for an exciton–exciton encounter distance of ∼1.3 nm, consistent with the bilayer exciton Bohr radius. These results indicate that spontaneous polarization in 3R-stacked bilayers can suppress nonlinear excitonic losses and provide a route toward high-density excitonics.

dipolar excitons↗

DOE OSTI2024

Ligand field exciton annihilation in bulk CrCl 3

The layered van der Waals material CrCl 3 exhibits very strongly bound ligand field excitons that control optoelectronic applications and are connected with magnetic ordering by virtue of their d-orbital origin. Time-resolved photoluminescence of these exciton populations at room temperature shows that their relaxation is dominated by exciton–exciton annihilation and that the spontaneous decay lifetime is very long. Furthermore, these observations allow the rough quantification of the exciton annihilation rate constant and contextualization in light of a recent theory of universal scaling behavior of the annihilation process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗