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Phased-necklace driving beams enable precise coherent control over the line spacing and divergence of EUV/soft x-ray harmonics. 

Recent observations of chloromethane in interstellar environments suggest that other organohalogens, which are known to be critically important in Earth's atmosphere, may also be of significance beyond our own terrestrial veil. This raises the question of how such molecules behave under extreme conditions such as when exposed to vacuum ultraviolet (VUV) radiation. VUV photons promote molecules to highly excited states that fragment in non-statistical patterns controlled by the initial femtosecond dynamics. A detailed understanding of VUV-driven photochemistry in complex organic molecules that consist of more than one functional group is a particularly challenging task. This quantum chemical analysis reports the electronic states and ionization potentials up to the VUV range (6–11 eV) of the chlorine-substituted cumulenone series molecules. The valence and Rydberg properties of lone-pair terminated, π-conjugated systems are explored for their potential resonance with lone pairs from elsewhere in the system. The carbon chain elongation within the family ClHC n O, where n = 1–4, influences the electronic excitations, associated wavefunctions, and ionization potentials of the molecules. The predicted geometries and ionization potentials are in good agreement with the available experimental photoelectron spectra for formyl chloride and chloroketene, n = 1–2. Furthermore, comparison between the regular cumulenone species and the corresponding chlorinated derivatives exhibit similar behaviors especially for n = 3, where the allene backbone in propadienone chloride is severely bent. Most notably for the excited states is that the Rydberg character becomes more dominant as the energy increases, with some retaining valence characters. 

Carboxylic acids are important combustion intermediates, especially regarding the combustion of oxygenates such as ethyl esters. The purpose of this study is to discern the unimolecular decomposition pathways of one such carboxylic acid, propionic acid, using microreactor flow experiments with line‐tunable photoionization mass spectrometry and infrared spectroscopy, along with high‐level electronic structure calculations (CCSD(T)/cc‐pV∞Z//M06‐2X/cc‐pVTZ level of theory) and master equation theory. Microreactor experiments were performed at 300–1500 K, pressures decreasing from roughly 300 Torr to vacuum pressure, and around 100 μs residence times. Primary products are methyl ketene, ketene, ethylene, and methyl radical. Theory suggests the two lowest energy bond fissions are active at these conditions and responsible for the production of ketene, methyl radical, and some ethylene. Importantly, theory revealed the significance of the isomerization of propionic acid to propene‐1,1‐diol, and the subsequent dehydrogenation reaction of the diol as an alternative explanation for the unimolecular formation of methyl ketene. This is predicted to be the dominant thermal decomposition pathway at lower temperatures (up to ∼850 K). Line‐tunable VUV photons allowed for isomer resolution of the products and showed no evidence of the diol of propionic acid surviving until detection, suggesting propene‐1,1‐diol decomposes either to methyl ketene and water rapidly, fragments upon ionization to a distonic ion inseparable from methyl ketene through our detection methods, or never stabilizes as propionic acid well‐skips directly to methyl ketene. Infrared spectroscopy showed no evidence of the decarboxylation of propionic acid at these conditions. Updated rate constants and branching ratios for propionic acid decomposition are calculated and provided for future modeling studies.

 

Light fields carrying orbital angular momentum (OAM) provide powerful capabilities for applications in optical communications, microscopy, quantum optics, and microparticle manipulation. We introduce a property of light beams, manifested as a temporal OAM variation along a pulse: the self-torque of light. Although self-torque is found in diverse physical systems (i.e., electrodynamics and general relativity), it was not realized that light could possess such a property. We demonstrate that extreme-ultraviolet self-torqued beams arise in high-harmonic generation driven by time-delayed pulses with different OAM. We monitor the self-torque of extreme-ultraviolet beams through their azimuthal frequency chirp. This class of dynamic-OAM beams provides the ability for controlling magnetic, topological, and quantum excitations and for manipulating molecules and nanostructures on their natural time and length scales. 

Abstract The global network of gravitational-wave observatories now includes five detectors, namely LIGO Hanford, LIGO Livingston, Virgo, KAGRA, and GEO 600. These detectors collected data during their third observing run, O3, composed of three phases: O3a starting in 2019 April and lasting six months, O3b starting in 2019 November and lasting five months, and O3GK starting in 2020 April and lasting two weeks. In this paper we describe these data and various other science products that can be freely accessed through the Gravitational Wave Open Science Center at https://gwosc.org . The main data set, consisting of the gravitational-wave strain time series that contains the astrophysical signals, is released together with supporting data useful for their analysis and documentation, tutorials, as well as analysis software packages. 

Intermediate-mass black holes (IMBHs) span the approximate mass range 100−10 5   M ⊙ , between black holes (BHs) that formed by stellar collapse and the supermassive BHs at the centers of galaxies. Mergers of IMBH binaries are the most energetic gravitational-wave sources accessible by the terrestrial detector network. Searches of the first two observing runs of Advanced LIGO and Advanced Virgo did not yield any significant IMBH binary signals. In the third observing run (O3), the increased network sensitivity enabled the detection of GW190521, a signal consistent with a binary merger of mass ∼150  M ⊙ providing direct evidence of IMBH formation. Here, we report on a dedicated search of O3 data for further IMBH binary mergers, combining both modeled (matched filter) and model-independent search methods. We find some marginal candidates, but none are sufficiently significant to indicate detection of further IMBH mergers. We quantify the sensitivity of the individual search methods and of the combined search using a suite of IMBH binary signals obtained via numerical relativity, including the effects of spins misaligned with the binary orbital axis, and present the resulting upper limits on astrophysical merger rates. Our most stringent limit is for equal mass and aligned spin BH binary of total mass 200  M ⊙ and effective aligned spin 0.8 at 0.056 Gpc −3 yr −1 (90% confidence), a factor of 3.5 more constraining than previous LIGO-Virgo limits. We also update the estimated rate of mergers similar to GW190521 to 0.08 Gpc −3 yr −1 . 

Abstract We present a search for continuous gravitational-wave emission due to r-modes in the pulsar PSR J0537–6910 using data from the LIGO–Virgo Collaboration observing run O3. PSR J0537–6910 is a young energetic X-ray pulsar and is the most frequent glitcher known. The inter-glitch braking index of the pulsar suggests that gravitational-wave emission due to r-mode oscillations may play an important role in the spin evolution of this pulsar. Theoretical models confirm this possibility and predict emission at a level that can be probed by ground-based detectors. In order to explore this scenario, we search for r-mode emission in the epochs between glitches by using a contemporaneous timing ephemeris obtained from NICER data. We do not detect any signals in the theoretically expected band of 86–97 Hz, and report upper limits on the amplitude of the gravitational waves. Our results improve on previous amplitude upper limits from r-modes in J0537-6910 by a factor of up to 3 and place stringent constraints on theoretical models for r-mode-driven spin-down in PSR J0537–6910, especially for higher frequencies at which our results reach below the spin-down limit defined by energy conservation.