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X-ray Transient Absorption Spectroscopy near the carbon K-edge (1s, $\sim$ 285 eV) and chlorine L$_{2,3}$ edges (2p, $\sim$ 200 eV) is used to study the nuclear dynamics of CCl$_4$ vibrationally activated by impulsive stimulated Raman scattering with a few-cycle 800 nm pump pulse. The totally symmetric stretching mode leads to a strong response in the inner-shell spectra, with the concerted elongation (contraction) in bond lengths leading to a red (blue) shift in the X-ray absorption energies associated with core-to-antibonding excitations. The relative slopes of the potential energy surfaces associated with the relevant core-excited states along the symmetric stretching mode are experimentally measured and compared to results from restricted open-shell Kohn-Sham calculations. A combination of experiment and theory indicates that the slope of the core-excited potential energy surface vs totally symmetric bond elongation is $-11.1 \pm 0.8$ eV/{\AA} for the Cl 2p$\to7a_1^*$ excitation, $-9.0\pm0.6$ eV/{\AA} for the Cl 2p$\to8t_2^*$ excitation and $-5.2\pm 0.4$ eV/{\AA} for the C 1s$\to8t_2^*$ excitation, to 95% confidence. The much larger slopes for the Cl 2p excitations compared to the C 1s state are attributed to greater contributions from Cl to the $7a_1^*$ or $8t_2^*$ antibonding orbitals to which the inner-shell electrons are being excited. No net displacement of the center of the vibrational wavefunction along the other vibrational modes is induced by the pump pulse, leading to absence of transient signal. The results highlight the ability of X-ray Transient Absorption Spectroscopy to reveal nuclear dynamics involving tiny ($<0.01$ {\AA}) atomic displacements and also provide direct measurement of forces on core-excited potential energy surfaces., Comment: ADR and DH contributed equally to this work

Understanding the relaxation pathways of photoexcited molecules is essential to gain atomistic level insight into photochemistry. Herein, we perform a time-resolved study of ultrafast molecular symmetry breaking via geometric relaxation (Jahn-Teller distortion) on the methane cation. Attosecond transient absorption spectroscopy with soft X-rays at the carbon K-edge reveals that the distortion occurs within $10\pm 2$ femtoseconds after few-femtosecond strong-field ionization of methane. The distortion activates coherent oscillations in the scissoring vibrational mode of the symmetry broken cation, which are detected in the X-ray signal. These oscillations are damped within $58\pm13$ femtoseconds, as vibrational coherence is lost with the energy redistributing into lower-frequency vibrational modes. This study completely reconstructs the molecular relaxation dynamics of this prototypical example and opens new avenues for exploring complex systems.

Spintronic nano-synapses and nano-neurons perform complex cognitive computations with high accuracy thanks to their rich, reproducible and controllable magnetization dynamics. These dynamical nanodevices could transform artificial intelligence hardware, provided that they implement state-of-the art deep neural networks. However, there is today no scalable way to connect them in multilayers. Here we show that the flagship nano-components of spintronics, magnetic tunnel junctions, can be connected into multilayer neural networks where they implement both synapses and neurons thanks to their magnetization dynamics, and communicate by processing, transmitting and receiving radio frequency (RF) signals. We build a hardware spintronic neural network composed of nine magnetic tunnel junctions connected in two layers, and show that it natively classifies nonlinearly-separable RF inputs with an accuracy of 97.7%. Using physical simulations, we demonstrate that a large network of nanoscale junctions can achieve state-of the-art identification of drones from their RF transmissions, without digitization, and consuming only a few milliwatts, which is a gain of more than four orders of magnitude in power consumption compared to currently used techniques. This study lays the foundation for deep, dynamical, spintronic neural networks.

A vibrational wavepacket in SF$_6$, created by impulsive stimulated Raman scattering with a few-cycle infrared pulse, is mapped onto five sulfur core-excited states using table-top soft X-ray transient absorption spectroscopy between 170-200 eV. The amplitudes of the X-ray energy shifts of the femtosecond oscillations depend strongly on the nature of the state. The prepared wavepacket is controlled with the pump laser intensity to probe the core-excited levels for various extensions of the S-F stretching motion. This allows the determination of the relative core-level potential energy gradients, in good agreement with TDDFT calculations. This experiment demonstrates a new means of characterizing core-excited potential energy surfaces.

When Harvard University moved all instruction into an online modality in response to the COVID-19 pandemic, The Language Center positioned itself as a critical source of guidance on best practices in this new environment. For Harvard, an institution that has always prioritized face-to-face instruction above all other formats, 2020 has been a watershed moment that has forced faculty to reconsider nearly everything about the way they organize and deliver their courses. Owing to the pandemic crisis, we find ourselves in a moment in which the efficacy of these modalities in language learning is, despite initial concerns, being proven day after day. In the context of this crisis, The Language Center has developed training and support mechanisms for this transition, focusing on desired learning outcomes, centering instructor and student experience, and positioning the language faculty to be able to successfully employ hybrid and online approaches to instruction that will continue to serve them well after the crisis abates. This contribution describes the strategies and actions that The Language Center took to ensure the success of the remote teaching and learning of languages at Harvard University in the first term of the 2020-2021 academic year, after the emergency evacuation of campus in March of 2020, and offers a model for other centers engaged in academic support. While extensive insights on the success of these efforts are still pending, given the timing of this crisis and the interventions undertaken, early feedback suggests that faculty have found provided resources to be useful, and their intention is to adopt aspects of technologically-mediated instruction in their face-to-face teaching going forward. [For the complete volume, "The World Universities' Response to COVID-19: Remote Online Language Teaching," see ED614006.]

X-ray Transient Absorption Spectroscopy (XTAS) and theoretical calculations are used to study CCl$_4^+$ prepared by 800 nm strong-field ionization. XTAS simultaneously probes atoms at the carbon K-edge (280-300 eV) and chlorine L-edge (195-220 eV). Comparison of experiment to X-ray spectra computed by orbital-optimized density functional theory (OO-DFT) indicates that after ionization, CCl$_4^+$ undergoes symmetry breaking driven by Jahn-Teller distortion away from the initial tetrahedral structure (T$_d$) in 6$\pm$2 fs. The resultant symmetry-broken covalently bonded form subsequently separates to a noncovalently bound complex between CCl$_3^+$ and Cl over 90$\pm$10 fs, which is again predicted by theory. Finally, after more than 800 fs, L-edge signals for atomic Cl are observed, indicating dissociation to free CCl$_3^+$ and Cl. The results for Jahn-Teller distortion to the symmetry-broken form of CCl$_4^+$ and formation of the Cl -- CCl$_3^+$ complex characterize previously unobserved new species along the route to dissociation.

We study magneto-transport in heterostructures composed of the van der Waals antiferromagnet CrPS$_{4}$ and the heavy metals Pt and Pd. The transverse resistance (R$_{xy}$) signal reveals the spin-flop transition of CrPS$_{4}$ and a strongly enhanced magnetic ordering temperature (>300 K), which might originate from a strong spin-orbit coupling at the interface. While CrPS$_{4}$/Pt devices allow for easy detection of the spin-flop transition, CrPS$_{4}$/Pd devices show a more substantial enhancement in magnetic ordering temperature and exhibit a topological Hall effect signal, possibly related to chiral spin structures at the interface. The longitudinal magnetoresistance (R$_{xx}$) results from a combination of spin-Hall magnetoresistance and the negative magnetoresistance that can be explained by a field-induced change of the electronic band structure of CrPS$_{4}$., Comment: 19 pages, 4 figures