Under strong electromagnetic excitation, electron–hole (e-h) pairs may be generated in solids, which are subsequently driven to high energy and high momentum, producing high harmonics (HH) of the ...driving field. The HH efficiency depends on the degree of coherence between the driven electron and hole created by the laser field. Here, we disrupt this e-h coherence in an atomically thin semiconductor by photodoping via incoherent e-h pairs. We observe a strong, systematic harmonic order-dependent intensity reduction. This trend is explained by an exponential decay of the inter-band polarization, proportional to the sub-cycle excursion time of the e-h pair. Our study provides a platform to probe the importance of many-body effects, such as excitation density-dependent decoherence time for strongly driven electrons without the need of ultrashort laser pulses.
•Line coupling and line mixing in CH3I spectra perturbed by N2 and O2 have been calculated.•The semi-classical method correctly takes into account the k-degeneracy of the transitions.•It leads to a ...reasonable agreement with the available data, including the T-dependence.•New experiments at higher pressures are suggested to check the description of inter-doublets couplings.
Calculations of the N2-, O2-, and air-broadened widths, together with their temperature dependence exponents have been made for transitions of CH3I in the ν5 and ν6 bands. The calculations are based on a semi-classical line shape formalism developed by the current authors through modifying and refining the Robert-Bonamy formalism. In recent years, we have applied this formalism for linear molecules, symmetric-top molecules with inversion symmetry, and asymmetric-top molecules. For symmetric-top molecules with the k degeneracy such as CH3I, the formalism has a new feature. In this case, one should consider each of the CH3I transitions labeled by ki or f ≠ 0 as a doublet. Then, one needs to consider the effects of the line mixing process between these two components. Comparisons of our theoretical predictions with some data available demonstrate a very reasonable agreement. Finally we propose new experiments at higher perturber pressures that would enable one to check the theoretically calculated relaxation matrices and to extend the analysis to the inter-doublet mixing effects.
Here,iIonically conductive, hydrated polyelectrolyte nanocomposites are prepared from iodomethane-treated poly(2-vinylpyridine) (mPV)-grafted cellulose nanocrystals (MxG-CNC-g-mPV). These ...polyelectrolyte-grafted nanoparticle (PEGN) films exhibit an order-of-magnitude higher iodide ion conductivity relative to mPV films and a high in-plane/through-plane anisotropy. The PEGN architecture prevents CNC aggregation, maximizing the CNC/polyelectrolyte interface. PEGN films were prepared with varying polymer graft density (0.03-0.12 chains/nm2) and molecular weight (7k-30k g/mol). The greatest ion conductivity enhancement is observed with lower molecular weight, higher density grafts: ca. 89 ± 6 mS/cm (140 ±10 mS/cm accounting for the volume of the CNC) versus 3.3 ± 0.4 mS/cm for ungrafted mPV. Poly(styrene-block-2-vinylpyridine)-grafted CNCs were prepared in which the insulating polystyrene block or the conducting mPV block was directly attached to the CNCs; only the films with the mPV block closest to the CNCs exhibited an enhancement in conductivity relative to mPV. Together, these data point to beneficial CNC/polyelectrolyte interfacial effects, resulting in significant ionic conductivity enhancement along the length of the CNCs in these films.
Here, we present calculations for the c coefficients of the isobaric mass multiplet equation for nuclei from A = 42 to A = 54 based on input from three realistic nucleon-nucleon interactions. We ...demonstrate that there is a clear dependence on the short-range charge-symmetry-breaking (CSB) part of the strong interaction and that there is significant disagreement in the CSB part between the commonly used CD-Bonn, chiral effective field theory at next-to-next-to-next-to-leading-order, and Argonne V18 nucleon-nucleon interactions. In addition, we show that all three interactions give a CSB contribution to the c coefficient that is too large when compared to experiment.
We demonstrate a widely applicable technique to absolutely calibrate the energy scale of x-ray spectra with experimentally well-known and accurately calculable transitions of highly charged ions, ...allowing us to measure the K-shell Rydberg spectrum of molecular O_{2} with 8 meV uncertainty. We reveal a systematic ∼450 meV shift from previous literature values, and settle an extraordinary discrepancy between astrophysical and laboratory measurements of neutral atomic oxygen, the latter being calibrated against the aforementioned O_{2} literature values. Because of the widespread use of such, now deprecated, references, our method impacts on many branches of x-ray absorption spectroscopy. Moreover, it potentially reduces absolute uncertainties there to below the meV level.
We present a comprehensive set of vibrationally-resolved cross sections for electron-impact electronic excitation of the isotopologues of molecular hydrogen (D2, T2, HD, HT, and DT) initially in the ...ground electronic state. We apply the adiabatic-nuclei molecular convergent close-coupling (MCCC) method to calculate cross sections from threshold to 500 eV for excitation of all bound vibrational levels and dissociative excitation of the B1Σu+, C1Πu, EF1Σg+, B′1Σu+, GK1Σg+, I1Πg, J1Δg, D1Πu, H1Σg+, b3Σu+, c3Πu, a3Σg+, e3Σu+, d3Πu, h3Σg+, g3Σg+, i3Πg, and j3Δg electronic states from all bound vibrational levels of the ground electronic (X1Σg+) state. Including the previously-published MCCC e-H2 cross sections (Scarlett et al., Atom. Data Nucl. Data Tables 137 (2021) 101361) the data set contains cross sections for over 60,000 electronic and vibrational transitions. The cross sections are presented in graphical form and provided as both numerical values and analytic fit functions in supplementary data files. The data can also be downloaded from the MCCC database at mccc-db.org.
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