Inner Valence Hole Migration in Isopropanol

Even within the sudden approximation, the removal of one neutral Hartree-Fock orbital does not leave the molecule in a pure one-hole state of the cation; coupling to virtual orbitals leads to a breakdown in the molecular orbital picture. This can be understood as interaction with two-hole one-particle states (singly excited cations) and becomes significant when those states are energetically similar to the one-hole states. This splitting of states is most relevant for inner valence holes which lie above the double ionisation potential. As such, impulsive creation of an inner valence hole (IVH) wavepacket results in a time dependent charge density which is purely electronic in nature (charge migration) [1] , [2] , though it depends on the nuclear geometry at the time of excitation, and subsequent nuclear motion will result in decoherence [3]

Have you forgotten? A method to assess if machine learning models have forgotten data

In the era of deep learning, aggregation of data from several sources is a common approach to ensuring data diversity. Let us consider a scenario where several providers contribute data to a consortium for the joint development of a classification model (hereafter the target model), but, now one of the providers decides to leave. This provider requests that their data (hereafter the query dataset) be removed from the databases but also that the model `forgets' their data. In this paper, for the first time, we want to address the challenging question of whether data have been forgotten by a model. We assume knowledge of the query dataset and the distribution of a model's output. We establish statistical methods that compare the target's outputs with outputs of models trained with different datasets. We evaluate our approach on several benchmark datasets (MNIST, CIFAR-10 and SVHN) and on a cardiac pathology diagnosis task using data from the Automated Cardiac Diagnosis Challenge (ACDC). We hope to encourage studies on what information a model retains and inspire extensions in more complex settings.Comment: Accepted by MICCAI 202

Wave Function Microscopy of Quasibound Atomic States

In the 1980s Demkov, Kondratovich, and Ostrovsky and Kondratovich and Ostrovsky proposed an experiment based on the projection of slow electrons emitted by a photoionized atom onto a position-sensitive detector. In the case of resonant excitation, they predicted that the spatial electron distribution on the detector should represent nothing else but a magnified image of the projection of a quasibound electronic state. By exciting lithium atoms in the presence of a static electric field, we present in this Letter the first experimental photoionization wave function microscopy images where signatures of quasibound states are evident. Characteristic resonant features, such as (i) the abrupt change of the number of wave function nodes across a resonance and (ii) the broadening of the outer ring of the image (associated with tunneling ionization), are observed and interpreted via wave packet propagation simulations and recently proposed resonance tunneling mechanisms. The electron spatial distribution measured by our microscope is a direct macroscopic image of the projection of the microscopic squared modulus of the electron wave that is quasibound to the atom and constitutes the first experimental realization of the experiment proposed 30 years ago

Wave-function imaging of quasibound and continuum Stark states

Photoionization of an atom in the presence of a uniform static electric field provides the unique opportunity to expand and visualize the atomic wave function at a macroscopic scale. In a number of seminal publications dating back to the 1980s, Fabrikant, Demkov, Kondratovich, and Ostrovsky showed that this goal could be achieved by projecting slow (meV) photoionized electrons onto a position-sensitive detector and underlined the distinction between continuum and resonant contributions. The uncovering of resonant signatures was achieved fairly recently in experiments on the nonhydrogenic lithium atoms [Cohen et al., Phys. Rev. Lett. 110, 183001 (2013)]. The purpose of the present article is the general description of these findings, with emphasis on the various manifestations of resonant character. From this point of view, lithium has been chosen as an illustrative example between the two limiting cases of hydrogen, where resonance effects are more easily identified, and heavy atoms like xenon, where resonant effects were not observed

Synchronized pulses generated at 20 eV and 90 eV for attosecond pump-probe experiments

The development of attosecond pulses across different photon energies is an essential precursor to performing pump–probe attosecond experiments in complex systems, where the potential of attosecond science1 can be further developed2,3. We report the generation and characterization of synchronized extreme ultraviolet (90 eV) and vacuum ultraviolet (20 eV) pulses, generated simultaneously via high-harmonic generation. The vacuum ultraviolet pulses are well suited for pump–probe experiments that exploit the high photo-ionization cross-sections of many molecules in this spectral region4 as well as the higher photon flux due to the higher conversion efficiency of the high harmonic generation process at these energies5. We temporally characterized all pulses using the attosecond streaking technique6 and the FROG-CRAB retrieval method7. We report 576 ± 16 as pulses at 20 eV and 257 ± 21 as pulses at 90 eV. Our demonstration of synchronized attosecond pulses at different photon energies, which are inherently jitter-free due to the common-path geometry implemented, offers unprecedented possibilities for pump–probe studies

Group testing with Random Pools: Phase Transitions and Optimal Strategy

The problem of Group Testing is to identify defective items out of a set of objects by means of pool queries of the form "Does the pool contain at least a defective?". The aim is of course to perform detection with the fewest possible queries, a problem which has relevant practical applications in different fields including molecular biology and computer science. Here we study GT in the probabilistic setting focusing on the regime of small defective probability and large number of objects, $p \to 0$ and $N \to \infty$. We construct and analyze one-stage algorithms for which we establish the occurrence of a non-detection/detection phase transition resulting in a sharp threshold, $\bar M$, for the number of tests. By optimizing the pool design we construct algorithms whose detection threshold follows the optimal scaling $\bar M\propto Np|\log p|$. Then we consider two-stages algorithms and analyze their performance for different choices of the first stage pools. In particular, via a proper random choice of the pools, we construct algorithms which attain the optimal value (previously determined in Ref. [16]) for the mean number of tests required for complete detection. We finally discuss the optimal pool design in the case of finite $p$

Spatial partitioning of the regulatory landscape of the X-inactivation centre

In eukaryotes transcriptional regulation often involves multiple long-range elements and is influenced by the genomic environment. A prime example of this concerns the mouse X-inactivation centre (Xic), which orchestrates the initiation of X-chromosome inactivation (XCI) by controlling the expression of the non-protein-coding Xist transcript. The extent of Xic sequences required for the proper regulation of Xist remains unknown. Here we use chromosome conformation capture carbon-copy (5C) and super-resolution microscopy to analyse the spatial organization of a 4.5-megabases (Mb) region including Xist. We discover a series of discrete 200-kilobase to 1 Mb topologically associating domains (TADs), present both before and after cell differentiation and on the active and inactive X. TADs align with, but do not rely on, several domain-wide features of the epigenome, such as H3K27me3 or H3K9me2 blocks and lamina-associated domains. TADs also align with coordinately regulated gene clusters. Disruption of a TAD boundary causes ectopic chromosomal contacts and long-range transcriptional misregulation. The Xist/Tsix sense/antisense unit illustrates how TADs enable the spatial segregation of oppositely regulated chromosomal neighbourhoods, with the respective promoters of Xist and Tsix lying in adjacent TADs, each containing their known positive regulators. We identify a novel distal regulatory region of Tsix within its TAD, which produces a long intervening RNA, Linx. In addition to uncovering a new principle of cis-regulatory architecture of mammalian chromosomes, our study sets the stage for the full genetic dissection of the X-inactivation centre

XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment

Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10−15s) and even attosecond (as) (1 as=10−18 s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation

TERRISCOPE: AN OPTICAL REMOTE SENSING RESEARCH PLATFORM USING AIRCRAFT AND UAS FOR THE CHARACTERIZATION OF CONTINENTAL SURFACES

ONERA is developing TERRISCOPE, a new platform to characterize the environment and the continental surfaces by optical remote sensing using manned aircrafts and UAS (Unmanned Airborne System). The objective of TERRISCOPE is to make available to the scientific community combinations of optical measurements remotely sensed with the best level state-of-the-art sensors. Different kinds of sensors have already been acquired or are still being acquired: Hyperspectral sensors (0.5–2.5 μm range), visible high resolution cameras, multispectral infrared cameras and airborne laser scanners. Each sensor is declined in two versions: one high performance for manned aircrafts and one more compact for UAS. This paper describes the whole equipment, and presents the main characteristics and performances of the carriers, the sensors and the processing chain. Possible sensors combinations on airplanes and UAS are also presented, as well as preliminary results