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Photoredox Catalysis Mediated by Tungsten(0) Arylisocyanides in 1,2-Difluorobenzene
No full textWe have studied the photochemical cyclization of 1-(2-iodobenzyl)-pyrrole (IBP) and 1-(2-bromobenzyl)-pyrrole (BBP) to 5H-pyrrolo[2,1-a]isoindol catalyzed by W(CNDipp)₆ (CNDipp = 2,6-diisopropylphenylisocyanide) in 1,2-difluorobenzene (DFB). Irradiation (445 nm) of W(CNDipp)₆ (5 mol %) in DFB solution converted 78% of IBP (50 mM) to product after 1 h (16 turnovers). Addition of tetra-n-butyl ammonium hexafluorophosphate (TBAPF₆) (0.2 M) to the DFB solution led to rapid photoinduced disappearance of W(CNDipp)₆ but, remarkably, did not inhibit photochemical cyclization of IBP, indicating that IBP cyclization could be driven by a nonluminescent photocatalyst
Single-cell deletion analyses show control of pro–T cell developmental speed and pathways by Tcf7, Spi1, Gata3, Bcl11a, Erg, and Bcl11b
No full textAs early T cell precursors transition from multipotentiality to T lineage commitment, they change expression of multiple transcription factors. It is unclear whether individual transcription factors directly control choices between T cell identity and some alternative fate or whether these factors mostly affect proliferation or survival during the normal commitment process. Here, we unraveled the impacts of deleting individual transcription factors at two stages in early T cell development, using synchronized in vitro differentiation systems, single-cell RNA-seq with batch indexing, and controlled gene-disruption strategies. First, using a customized method for single-cell CRISPR disruption, we defined how the early-acting transcription factors Bcl11a, Erg, Spi1 (PU.1), Gata3, and Tcf7 (TCF1) function before commitment. The results revealed a kinetic tug of war within individual cells between T cell factors Tcf7 and Gata3 and progenitor factors Spi1 and Bcl11a, with an unexpected guidance role for Erg. Second, we tested how activation of transcription factor Bcl11b during commitment altered ongoing cellular programs. In knockout cells where Bcl11b expression was prevented, the cells did not undergo developmental arrest, instead following an alternative path as T lineage commitment was blocked. A stepwise, time-dependent regulatory cascade began with immediate-early transcription factor activation and E protein inhibition, finally leading Bcl11b knockout cells toward exit from the T cell pathway. Last, gene regulatory networks of transcription factor cross-regulation were extracted from the single-cell transcriptome results, characterizing the specification network operating before T lineage commitment and revealing its links to both the Bcl11b knockout alternative network and the network consolidating T cell identity during commitment
Variational modeling of hydromechanical fracture in saturated porous media: A micromechanics-based phase-field approach
No full textThis paper presents a novel variational phase-field model for different fracture processes in fully saturated porous media. As a key feature, the model employs a micromechanics-based theory for the description of brittle-tensile and compressive–ductile fracture. As such, the field variables are linked to physical mechanisms at the microcrack level, with damage emerging as the consequence of microcrack growth. Similarly, plasticity emerges as a consequence of the frictional sliding of closed microcracks. In this way, the evolution of opening microcracks in tension leads to (mode I) brittle fracture, while the evolution of closed microcracks in compression/shear leads to (mode II) ductile fracture. These failure mechanisms are coupled to fluid flow, resulting in a Darcy–Biot–type hydromechanical model. Therein, in the tensile regime, plasticity naturally vanishes, while damage is driven by poroelastic energy, accounting for the pressure in fluid-filled opening microcracks. On the other hand, in the compressive/shear regime, the plastic driving force naturally follows as a Terzaghi-type effective stress in terms of the local stress field acting on the microcrack surfaces, while damage is solely driven by the frictionally blocked free energy. As another important feature, the model includes a non-associative frictional plasticity law. Nevertheless, a thermodynamically consistent variational framework is employed, for which different energetic principles are discussed. Finally, the numerical simulations show that the model captures relevant hydromechanical coupling effects in benchmark problems, including mechanically induced shear fracture and hydraulically induced tensile fracture
Flares in gamma-ray burst X-ray afterglows as prompt emission from slightly misaligned structured jets
No full textWe develop a model to explain the flaring activity in gamma-ray burst X-ray afterglows within the framework of slightly misaligned observers to structured jets. We suggest that flares could be the manifestation of prompt dissipation within the core of the jet, appearing to a misaligned observer in the X-ray band because of less favourable Doppler boosting. These flares appear during the afterglow phase because of core–observer light travel delays. In this picture, the prompt emission recorded by this observer comes from material along their line of sight, in the lateral structure of the jet, outside the jet’s core. We start by laying down the basic analytical framework to determine the flares characteristics as a function of those of the gamma-ray pulse an aligned observer would see. We show that there is viable parameter space to explain flares with typical observing times and luminosities. We then analytically explore this model, showing that it naturally produces flares with small aspect ratios, as observed. We perform fits of our model to two Swift/XRT flares representing two different types of morphology, to show that our model can capture both. The ejection time of the core jet material responsible of the flare is a critical parameter. While it always remains small compared to the observed time of the flare, confirming that our model does not require very late central engine activity, late ejection times are strongly favoured, sometimes larger than the observed duration of the parent gamma-ray burst’s prompt emission as measured by T90
Progenitor and close-in circumstellar medium of type II supernova 2020fqv from high-cadence photometry and ultra-rapid UV spectroscopy
No full textWe present observations of SN 2020fqv, a Virgo-cluster type II core-collapse supernova (CCSN) with a high temporal resolution light curve from the Transiting Exoplanet Survey Satellite (TESS) covering the time of explosion; ultraviolet (UV) spectroscopy from the Hubble Space Telescope (HST) starting 3.3 d post-explosion; ground-based spectroscopic observations starting 1.1 d post-explosion; along with extensive photometric observations. Massive stars have complicated mass-loss histories leading up to their death as CCSNe, creating circumstellar medium (CSM) with which the SNe interact. Observations during the first few days post-explosion can provide important information about the mass-loss rate during the late stages of stellar evolution. Model fits to the quasi-bolometric light curve of SN 2020fqv reveal 0.23 M_⊙ of CSM confined within 1450 R_⊙ (10¹⁴ cm) from its progenitor star. Early spectra (<4 d post-explosion), both from HST and ground-based observatories, show emission features from high-ionization metal species from the outer, optically thin part of this CSM. We find that the CSM is consistent with an eruption caused by the injection of ∼5 × 10⁴⁶ erg into the stellar envelope ∼300 d pre-explosion, potentially from a nuclear burning instability at the onset of oxygen burning. Light-curve fitting, nebular spectroscopy, and pre-explosion HST imaging consistently point to a red supergiant (RSG) progenitor with M_(ZAMS) ~ 13.5-15 M_⊙, typical for SN II progenitor stars. This finding demonstrates that a typical RSG, like the progenitor of SN 2020fqv, has a complicated mass-loss history immediately before core collapse
High precision ringdown modeling: Multimode fits and BMS frames
No full textQuasinormal mode (QNM) modeling is an invaluable tool for characterizing remnant black holes, studying strong gravity, and testing general relativity. Only recently have QNM studies begun to focus on multimode fitting to numerical relativity strain waveforms. As gravitational wave observatories become even more sensitive they will be able to resolve higher-order modes. Consequently, multimode QNM fits will be critically important, and in turn require a more thorough treatment of the asymptotic frame at I⁺. The first main result of this work is a method for systematically fitting a QNM model containing many modes to a numerical waveform produced using Cauchy-characteristic extraction (CCE), a waveform extraction technique which is known to resolve memory effects. We choose the modes to model based on their power contribution to the residual between numerical and model waveforms. We show that the all-mode strain mismatch improves by a factor of ∼10⁵ when using multimode fitting as opposed to only fitting the (2, ±2, n) modes. Our most significant result addresses a critical point that has been overlooked in the QNM literature: the importance of matching the Bondi-van der Burg-Metzner-Sachs (BMS) frame of the numerical waveform to that of the QNM model. We show that by mapping the numerical waveforms—which exhibit the memory effect—to a BMS frame known as the super rest frame, there is an improvement of ∼10⁵ in the all-mode strain mismatch compared to using a strain waveform whose BMS frame is not fixed. Furthermore, we find that by mapping CCE waveforms to the super rest frame, we can obtain all-mode mismatches that are, on average, a factor of ∼4 better than using the publicly available extrapolated waveforms. We illustrate the effectiveness of these modeling enhancements by applying them to families of waveforms produced by numerical relativity and comparing our results to previous QNM studies
Impact of noise transients on low latency gravitational-wave event localization
No full textGravitational-wave (GW) data contains non-Gaussian noise transients called “glitches.” During the third LIGO-Virgo observing run about 24% of all gravitational-wave candidates were in the vicinity of a glitch, while even more events could be affected in future observing runs due to increasing detector sensitivity. This poses a problem since glitches can affect the estimation of GW source parameters, including sky localization, which is crucial to identify an electromagnetic counterpart. This is the first of its kind study that evaluates the importance of relative glitch positioning in time with respect to a GW signal. In this paper we estimate how much sky localization is affected by a nearby glitch in low latency. We injected binary black hole (BBH), binary neutron star (BNS), and neutron star-black hole (NSBH) signals into data containing three different classes of glitches: blips, thunderstorms and fast scatterings. The impact of these glitches was assessed by estimating the number of tile pointings that a telescope would need to search over until the true sky location of an event is observed. We find that blip glitches generally do not affect the localization of our tested GW signals, however in very rare cases of a blip glitch overlap with a BBH or a NSBH signal can cause the true position of the event to lie well outside the 90% computed sky localization, severely compromising electromagnetic follow-up. Thunderstorm glitches have a noticeable impact on BBH and NSBH events, especially if there is no third interferometer. In such cases we find that the electromagnetic follow-up efforts with telescopes as large as 20 deg² field of view (FOV) are affected. Observing BBH and NBSH signals with three-detector network reduces the bias in sky localization caused by thunderstorm glitches, making the bias to affect only small (FOV = 1 deg²) telescopes. BNS events appear to be not affected by thunderstorm glitches. Fast scattering glitches have no impact on the low latency localization of BBH and BNS signals. For NSBH signals observed with two-detector network, the sky localization bias due to fast scattering glitches is significant enough to affect even large (FOV = 20 deg²) telescopes. Observing NSBH signals with three interferometers reduces the bias such that it impacts only small (FOV = 1 deg²) telescopes
Intermittent lab earthquakes in dynamically weakening fault gouge
No full textLarge and destructive earthquakes on mature faults in Earth’s crust occur as slip in a layer of a fine granular material—fault gouge—produced by comminution during sliding. A range of insights into the frictional resistance of faults—one of the main factors controlling earthquake nucleation, dynamic propagation and arrest, and hence the destructive ground shaking of earthquakes—has been obtained in experiments with spatially uniform slip imposed in small samples. However, how various features of gouge friction combine to determine spontaneous progression of earthquakes is difficult to study in the lab owing to substantial challenges with sample sizes and adequate imaging. Here, using lab experiments, we show that spontaneously propagating dynamic ruptures navigate a fault region with fine rock gouge through complex, intermittent slip processes with dramatic friction evolution. These include repeated arrest of rupture propagation caused by friction strengthening at lower slip rates and dynamic earthquake re-nucleation enabled by pronounced rapid friction weakening at higher slip rates consistent with flash heating. The spontaneous repeated weakening and strengthening of friction in fine rock gouge highlights the fundamental dependence of friction on slip rate and associated processes, such as shear heating, localization and delocalization of shear, and dilation and compaction of the shear layer. Our findings expand experimental support of the concept that co-seismic weakening may enable earthquake rupture to break through stable fault regions, with substantial implications for seismic hazard
Copper(II) Binding to the Intrinsically Disordered C-Terminal Peptide of SARS-CoV-2 Virulence Factor Nsp1
No full textThe first encoded SARS-CoV-2 protein (Nsp1) binds to the human 40S ribosome and blocks synthesis of host proteins, thereby inhibiting critical elements of the innate immune response. The final 33 residues of the natively unstructured Nsp1 C-terminus adopt a helix-turn-helix geometry upon binding to the ribosome. We have characterized the fluctuating conformations of this peptide using circular dichroism spectroscopy along with measurements of tryptophan fluorescence and energy transfer. Tryptophan fluorescence decay kinetics reveal that copper(II) binds to the peptide at micromolar concentrations, and electron paramagnetic resonance spectroscopy indicates that the metal ion coordinates to the lone histidine residue
Mid-ultraviolet Hubble Observations of Europa and the Global Surface Distribution of SO₂
No full textWe present spatially resolved reflectance spectra of Europa’s surface in the wavelength range of 210–315 nm obtained by the Hubble Space Telescope Imaging Spectrograph in 2018 and 2019. These data provide the first high-quality, near-global spectral observations of Europa from 210 to 240 nm. They show that the reflectance of Europa’s leading, trailing, anti-Jovian, and sub-Jovian hemispheres is ∼5% near 210 nm, with varying spectral slopes across the mid-UV. This low albedo, even on the more “pristine” leading hemisphere, indicates a lack of the signature far-UV spectral edge characteristic of water ice. We detected and mapped a strong absorption feature at 280 nm that is consistent with an S–O bond that has previously been attributed to SO₂ on the surface, hypothesized to be formed through radiolytic processing of Iogenic sulfur ions that have been preferentially emplaced on Europa’s trailing hemisphere by Jupiter’s magnetic field. Our models show that small inclusions of SO₂ (0.1%) within the water ice are sufficient to produce the 280 nm feature without producing a feature at 4.07 μm, which has not been observed in ground-based spectral observations of Europa. This data set is the first to produce a spatially resolved, near-global map of the assumed SO₂ feature, which is primarily concentrated near the apex of the trailing hemisphere and correlated with large-scale darker regions in both the visible and the ultraviolet. This distribution is consistent with “cold” exogenic sulfur ion bombardment on Europa