Search

We investigate correlated three-electron escape in Ne when driven by an intense, infrared laser field. We do so by employing a reduced-dimensionality quantum-mechanical model and two three-dimensional semi-classical models. One semi-classical model is a recently developed one that accounts with effective coulomb potentials for the interaction between two bound electrons (ECBB) while it fully accounts for all other interactions. The other semi-classical model is the Heisenberg one, which effectively accounts for the interaction of each electron with the core via a soft-core potential. We identify and compare the signatures of correlated three-electron escape for both quantum and semi-classical models on Dalitz plots and find a better agreement between the quantum and the ECBB model. We also show that a central ``spot'' on the Dalitz plots is reproduced by all models. Using the ECBB model we associate this ``spot'' with the direct triple ionization pathway and argue this to be the case also for the quantum model. Devising a simple classical model that accounts for the direct pathway of triple ionization, we show that the width of this spot in the Dalitz plots solely depends on the time of tunnel-ionization., Comment: 11 pages, 6 figures, original article

The subjective nature of music emotion introduces inherent bias in both recognition and generation, especially when relying on a single audio encoder, emotion classifier, or evaluation metric. In this work, we conduct a study on Music Emotion Recognition (MER) and Emotional Music Generation (EMG), employing diverse audio encoders alongside the Frechet Audio Distance (FAD), a reference-free evaluation metric. Our study begins with a benchmark evaluation of MER, highlighting the limitations associated with using a single audio encoder and the disparities observed across different measurements. We then propose assessing MER performance using FAD from multiple encoders to provide a more objective measure of music emotion. Furthermore, we introduce an enhanced EMG approach designed to improve both the variation and prominence of generated music emotion, thus enhancing realism. Additionally, we investigate the realism disparities between the emotions conveyed in real and synthetic music, comparing our EMG model against two baseline models. Experimental results underscore the emotion bias problem in both MER and EMG and demonstrate the potential of using FAD and diverse audio encoders to evaluate music emotion objectively.

Compared to time-reversal symmetry-protected Z2 topological insulators and Dirac/Weyl semimetals, there are significantly fewer candidates for topological crystalline insulators. SrAg4Sb2 is predicted to exhibit topological crystalline insulator behavior when considering spin-orbit coupling. In this study, we systematically investigate single crystals of SrAg4Sb2 using electrical transport and magnetic torque measurements, along with first-principles calculations. Our transport data reveals its compensated semimetal nature with a magnetoresistance up to around 700% at 2 K and 9 T. Analysis of de Haas-van Alphen oscillations uncovers a Fermi surface consisting of three distinct Fermi pockets with light effective masses. Comparison between the three-dimensional fermiology obtained from our oscillation data and the first-principles calculations demonstrates excellent agreement. This confirms the accuracy of the calculations, which indicate a band inversion centered at the {\Gamma} point and identify the existence of nontrivial tube and needle hole Fermi pockets at {\Gamma}, alongside one trivial diamond electron pocket at the T point in the Brillouin zone. Furthermore, symmetry and topology analysis results in two potential sets of topological invariants, suggesting the emergence of two-dimensional gapless Dirac surface states either on the ab planes or on both the ab planes and mirror planes, protected by crystal symmetries. Therefore, SrAg4Sb2 emerges as a promising candidate topological crystalline insulator., Comment: 9 pages, 5 figures

We formulate a general hybrid quantum-classical technique to describe the interaction of diatomic molecules with XUV pulses. We demonstrate the accuracy of our model in the context of the interaction of the O$_2$ molecule with an XUV pulse with photon energy ranging from 20 eV to 42 eV. We account for the electronic structure and electron ionization quantum mechanically employing accurate molecular continuum wavefunctions. We account for the motion of the nuclei using classical equations of motion. However, the force of the nuclei is computed by obtaining accurate potential-energy curves of O$_2$ up to O$_2^{2+}$, relevant to the 20 eV-42 eV photon-energy range, using advanced quantum-chemistry techniques. We find the dissociation limits of these states and the resulting atomic fragments and employ the Velocity Verlet algorithm to compute the velocities of these fragments. We incorporate both electron ionization and nuclear motion in a stochastic Monte-Carlo simulation and identify the ionization and dissociation pathways when O$_2$ interacts with an XUV pulse. Focusing on the O$^+$ + O$^+$ dissociation pathway, we obtain the kinetic-energy release distributions of the atomic fragments and find very good agreement with experimental results. Also, we explain the main features of the KER in terms of ionization sequences consisting of two sequential single-photon absorptions resulting in different O$^+$ and O$^{2+}$ electronic state configurations involved in the two transitions., Comment: 15 pages, 10 Figures

The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. The results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

The growing popularity of generative music models underlines the need for perceptually relevant, objective music quality metrics. The Frechet Audio Distance (FAD) is commonly used for this purpose even though its correlation with perceptual quality is understudied. We show that FAD performance may be hampered by sample size bias, poor choice of audio embeddings, or the use of biased or low-quality reference sets. We propose reducing sample size bias by extrapolating scores towards an infinite sample size. Through comparisons with MusicCaps labels and a listening test we identify audio embeddings and music reference sets that yield FAD scores well-correlated with acoustic and musical quality. Our results suggest that per-song FAD can be useful to identify outlier samples and predict perceptual quality for a range of music sets and generative models. Finally, we release a toolkit that allows adapting FAD for generative music evaluation., Comment: Submitted to IEEE ICASSP 2024

Automated Audio Captioning (AAC) is the task of generating natural language descriptions given an audio stream. A typical AAC system requires manually curated training data of audio segments and corresponding text caption annotations. The creation of these audio-caption pairs is costly, resulting in general data scarcity for the task. In this work, we address this major limitation and propose an approach to train AAC systems using only text. Our approach leverages the multimodal space of contrastively trained audio-text models, such as CLAP. During training, a decoder generates captions conditioned on the pretrained CLAP text encoder. During inference, the text encoder is replaced with the pretrained CLAP audio encoder. To bridge the modality gap between text and audio embeddings, we propose the use of noise injection or a learnable adapter, during training. We find that the proposed text-only framework performs competitively with state-of-the-art models trained with paired audio, showing that efficient text-to-audio transfer is possible. Finally, we showcase both stylized audio captioning and caption enrichment while training without audio or human-created text captions.

The potential energy curves for molecular ions up to $N_2^{4+}$ are calculated in an ab initio manner using the multi configurational self-consistent field method. Specifically, we implement in an automatic way a previously used double loop optimisation scheme within the multi configurational self-consisted field method. We obtain the potential energy curves up to $N_2^{4+}$ ions with any combination of core, inner valence, and outer valence holes. Finally, we provide the code used to generate these potential energy curves., Comment: 20 pages, 16 figures

We obtain continuum molecular wavefunctions for open-shell molecules in the Hartree-Fock framework. We do so while accounting for the singlet or triplet total spin symmetry of the molecular ion, that is, of the open-shell orbital and the initial orbital where the electron ionizes from. Using these continuum wavefunctions, we obtain the dipole matrix elements for a core electron that ionizes due to single-photon absorption by a linearly polarized X-ray pulse. After ionization from the X-ray pulse, we control or streak the electron dynamics using a circularly polarized infrared (IR) pulse. For a high intensity IR pulse and photon energies of the X-ray pulse close to the ionization threshold of the $1{\sigma}$ or $2{\sigma}$ orbitals, we achieve control of the angle of escape of the ionizing electron by varying the phase delay between the X-ray and IR pulses. For a low intensity IR pulse, we obtain final electron momenta distributions on the plane of the IR pulse and we find that many features of these distributions correspond to the angular patterns of electron escape solely due to the X-ray pulse., Comment: 12 pages, 7 figures

We demonstrate a general three-dimensional semiclassical model as a powerful technique for the study of correlated multi-electron escape in atoms driven by infrared laser pulses at intensities where electron-electron correlation prevails. We do so in the context of triple ionization of strongly driven Ne. We show that a drawback of other current quantum mechanical and classical models of triple ionization is that they soften the Coulomb potential of each electron with the core. The model we employ fully accounts for the singularity in the Coulomb potentials of a recolliding electron with the core and a bound electron with the core as well as for the interaction of a recolliding with a bound electron. Our model treats approximately only the interaction between bound electrons through the use of effective potentials. These effective potentials ensure that no artificial autoionization takes place as a result of the full treatment of the electron-core potential. We demonstrate the accuracy of our model by obtaining triple ionization distributions of the sum of the final electron momenta which we find to be in very good agreement with experiments. Also, we explain the main features of these momenta distributions in terms of the prevalent pathways of correlated three-electron escape in Ne. We also show that the different ionization pathways prevailing in three-electron escape in strongly driven Ne versus Ar give rise to different momenta distributions in these two atoms., Comment: 6 pages, 4 figures. arXiv admin note: substantial text overlap with arXiv:2210.17394

The analysis, processing, and extraction of meaningful information from sounds all around us is the subject of the broader area of audio analytics. Audio captioning is a recent addition to the domain of audio analytics, a cross-modal translation task that focuses on generating natural descriptions from sound events occurring in an audio stream. In this work, we identify and improve on three main challenges in automated audio captioning: i) data scarcity, ii) imbalance or limitations in the audio captions vocabulary, and iii) the proper performance evaluation metric that can best capture both auditory and semantic characteristics. We find that generally adopted loss functions can result in an unfair vocabulary imbalance during model training. We propose two audio captioning augmentation methods that enrich the training dataset and the vocabulary size. We further underline the need for in-domain pretraining by exploring the suitability of audio encoders that were previously trained on different audio tasks. Finally, we systematically explore five performance metrics borrowed from the image captioning domain and highlight their limitations for the audio domain., Comment: Submitted to EUSIPCO 2023

We employ a recently developed three-dimensional semiclassical model to identify nondipole effects in triple ionization of Ne driven by infrared laser pulses at intensities where electron-electron correlation prevails. This model fully accounts for the Coulomb interaction of each electron with the core and avoids artificial autoionization by employing effective Coulomb potentials to describe the interaction between bound electrons (ECBB). Using the ECBB model, we identify a prominent signature of nondipole effects. Namely, the component along the direction of light propagation of the average sum of the final electron momenta is large and positive. That is, we identify a positive momentum offset, absent in the dipole approximation. We find that this positive momentum offset stems mostly from the momentum change due to the magnetic field. To further understand this momentum change, we also develop a simple model for the motion of an electron inside an electromagnetic field. This simple model accounts for the effect of the Coulomb forces only as a sharp change in the momentum of the electron during recollision. We show that the momentum change due to the magnetic field is related with the sharp change in momentum during recollision for the recolliding electron as well as with the time of recollision for both the recolliding and bound electrons. Hence, we demonstrate that the final electron momentum offset probes the strength of a recollision and hence the degree of correlation in multielectron ionization., Comment: 10 pages, 8 figures

We theoretically demonstrate a one-to-one mapping between the direction of electron ionization and the phase delay between a linearly polarized VUV and a circular IR laser pulse. To achieve this, we use an ultrashort VUV pulse that defines the moment in time and space when an above threshold electron is released in the IR pulse. The electron can then be accelerated to high velocities escaping in a direction completely determined by the phase delay between the two pulses. The dipole matrix element to transition from an initial bound state of the N$_2$ molecule, considered in this work, to the continuum is obtained using quantum mechanical techniques that involve computing accurate continuum molecular states. Following release of the electron in the IR pulse, we evolve classical trajectories, neglecting the Coulomb potential and accounting for quantum interference, to compute the distribution of the direction and magnitude of the final electron momentum. The concept we theoretically develop can be implemented to produce nanoscale ring currents that generate large magnetic fields., Comment: 10 pages, 6 figures

The quantum anomalous Hall (QAH) effect is characterized by a dissipationless chiral edge state with a quantized Hall resistance at zero magnetic field. Manipulating the QAH state is of great importance in both the understanding of topological quantum physics and the implementation of dissipationless electronics. Here, we realized the QAH effect in the magnetic topological insulator Cr-doped (Bi,Sb)2Te3 (CBST) grown on an uncompensated antiferromagnetic insulator Al-doped Cr2O3. Through polarized neutron reflectometry (PNR), we find a strong exchange coupling between CBST and Al-Cr2O3 surface spins fixing interfacial magnetic moments perpendicular to the film plane. The interfacial coupling results in an exchange-biased QAH effect. We further demonstrate that the magnitude and sign of the exchange bias can be effectively controlled using a field training process to set the magnetization of the Al-Cr2O3 layer. Our work demonstrates the use of the exchange bias effect to effectively manipulate the QAH state, opening new possibilities in QAH-based spintronics.

Activating metamagnetic transitions between ordered states in van der Waals magnets and devices bring great opportunities in spintronics. We show that external pressure, which enhances the interlayer hopping without introducing chemical disorders, triggers multiple metamagnetic transitions upon cooling in the topological van der Waals magnets Mn(Bi$_{1-x}$Sb$_x$)$_4$Te$_7$, where the antiferromagnetic interlayer superexchange coupling competes with the ferromagnetic interlayer coupling mediated by the antisite Mn spins. The temperature-pressure phase diagrams reveal that while the ordering temperature from the paramagnetic to ordered states is almost pressure-independent, the metamagnetic transitions show non-trivial pressure and temperature dependence, even re-entrance. For these highly anisotropic magnets, we attribute the former to the ordering temperature being only weakly dependent on the intralayer parameters, the latter to the parametrically different pressure and temperature dependence of the two interlayer couplings. Our independent probing of these disparate magnetic interactions paves an avenue for efficient magnetic manipulations in van der Waals magnets., Comment: 10 pages, 4 figures

We formulate a three-dimensional semi-classical model to address triple and double ionization in three-electron atoms driven by intense infrared laser pulses. During time propagation, our model fully accounts for the Coulomb singularities, the magnetic field of the laser pulse and for the motion of the nucleus at the same time as for the motion of the three electrons. The framework we develop is general and can account for multi-electron ionization in strongly-driven atoms with more than three electrons. To avoid unphysical autoionization arising in classical models of three or more electrons, we replace the Coulomb potential between pairs of bound electrons with effective Coulomb potentials. The Coulomb forces between electrons that are not both bound are fully accounted for. We develop a set of criteria to determine when electrons become bound during time propagation. We compare ionization spectra obtained with the model developed here and with the Heisenberg model that includes a potential term restricting an electron from closely approaching the core. Such spectra include the sum of the electron momenta along the direction of the laser field as well as the correlated electron momenta. We also compare these results with experimental ones.

We formulate a transparent measure that quantifies chirality in single electron ionization triggered in atoms, which are achiral systems. We do so in the context of Ar driven by a new type of optical fields that consists of two non-collinear laser beams giving rise to chirality that varies in space across the focus of the beams. Our computations account for realistic experimental conditions. To define this measure of chirality, we first find the sign of the electron final momentum scalar triple product $\mathrm{{\bf{p}}_{k}\cdot ({\bf{p}}_{i}\times {\bf p}_{j})}$ and multiply it with the probability for an electron to ionize with certain values for both $\mathrm{p_{k}}$ and $\mathrm{p_{i}p_{j}}$. Then, we integrate this product over all values of $\mathrm{p_{k}}$ and $\mathrm{p_{i}p_{j}}$. We show this to be a robust measure of chirality in electron ionization triggered by globally chiral electric fields., Comment: 6 pages, 4 figures

High concentration of negatively charged nitrogen-vacancy ($\text{NV}^{-}$) centers was created in diamond single crystals containing approximately 100 ppm nitrogen using electron and neutron irradiation and subsequent thermal annealing in a stepwise manner. Continuous wave electron paramagnetic resonance (EPR) was used to determine the transformation efficiency from isolated N atoms to $\text{NV}^{-}$ centers in each production step and its highest value was as high as 17.5 %. Charged vacancies are formed after electron irradiation as shown by EPR spectra, but the thermal annealing restores the sample quality as the defect signal diminishes. We find that about 25 % of the vacancies form NVs during the annealing process. The large $\text{NV}^{-}$ concentration allows to observe orientation dependent spin-relaxation times and also the determination of the hyperfine and quadrupole coupling constants with high precision using electron spin echo (ESE) and electron-nuclear double resonance (ENDOR). We also observed the EPR signal associated with the so-called W16 centers, whose spectroscopic properties might imply a nitrogen dimer-vacancy center for its origin.

Multi-electron dynamics in atoms and molecules very often occur on sub- to few-femtosecond timescales. The available intensities of extreme-ultraviolet (XUV) attosecond pulses have previously only allowed the time-resolved investigation of two-photon, two-electron interactions. Here we demonstrate attosecond control over double and triple ionization of argon atoms involving the absorption of up to five XUV photons. In an XUV-pump XUV-probe measurement using a pair of attosecond pulse trains (APTs), the Ar$^{2+}$ ion yield exhibits a weak delay dependence, showing that its generation predominantly results from the sequential emission of two electrons by photoabsorption from the two APTs. In contrast, the Ar$^{3+}$ ion yield exhibits strong modulations as a function of the delay, which is a clear signature of the simultaneous absorption of at least two XUV photons. The experimental results are well reproduced by numerical calculations that provide detailed insights into the ionization dynamics. Our results open up new opportunities for the investigation and control of multi-electron dynamics and complex electron correlation mechanisms on extremely short timescales., Comment: 8 pages, 4 figures

For two-electron diatomic molecules, we investigate magnetic field effects in non-sequential double ionization where recollisions prevail. We do so by formulating a three-dimensional semi-classical model that fully accounts for the Coulomb singularities and for magnetic field effects during time propagation. Using this model, we identify a prominent signature of non-dipole effects. Namely, we demonstrate that the recolliding electron back-scatters along the direction of light propagation. Hence, this electron escapes opposite to the direction of change in momentum due to the magnetic field. This is in striking contrast to strongly-driven atoms where the recolliding electron forward-scatters along the direction of light propagation. We attribute these distinct signatures to the different gate that the magnetic field creates jointly with a soft recollision in molecules compared to a hard recollision in atoms. These two different gates give rise, shortly before recollision, to different momenta and positions of the recolliding electron along the direction of light propagation. As a result, we show that the Coulomb forces from the nuclei act to back-scatter the recolliding electron in molecules and forward-scatter it in atoms along the direction of light propagation., Comment: 14 pages, 8 figures

We formulate a three-dimensional semi-classical model to treat three-electron escape dynamics in a strongly-driven linear triatomic molecule, HeH$_{2}^{+}$. Our model includes the Coulomb singularities. Hence, to avoid unphysical autoionization, we employ two criteria to switch off the Coulomb repulsive force between two bound electrons and switch it on when the motion of one electron is mostly determined by the laser field. We investigate triple and "frustrated" triple ionization. In the latter process two electrons escape while one electron remains bound in a Rydberg state. We find that two pathways prevail in "frustrated" triple ionization, as in "frustrated" double ionization. We also find that the electron that remains in a Rydberg state is more likely to be attached to He$^{2+}$ compared to H$^{+}$. Our results indicate that in triple and "frustrated" triple ionization electronic correlation is weak. Moreover, we compute the sum of the kinetic energies as well as the angular patterns of the final ion fragments in triple and "frustrated" triple ionization. These patterns suggest that the fragmenting molecule deviates from its initial linear configuration., Comment: 7 pages, 4 figures

We investigate the interaction of Xe with isolated attosecond XUV pulses. Specifically, we calculate the ion yields and determine the pathways leading to the formation of ionic charged states up to Xe$^{5+}$. To do so, in our formulation we account for single-photon absorption, sequential multi-photon absorption, direct two-photon absorption, single and double Auger decays, and shake-off. We compare our results for the ion yields and for ion yield ratios with recent experimental results obtained for 93 eV and 115 eV attosecond XUV pulses. In particular, we investigate the role that a sequence of two single-photon ionization processes plays in the formation of Xe$^{4+}$. We find that each one of these two processes ionizes a core electron and thus leads to the formation of a double core-hole state. Remarkably, we find that the formation of Xe$^{5+}$ involves a direct two-photon absorption process and the absorption of a total of three photons., Comment: 8 pages, 4 figures

We study the interaction of a heteronuclear diatomic molecule, carbon monoxide, with a free-electron laser (FEL) pulse. We compute the ion yields and the intermediate states by which the ion yields are populated. We do so using rate equations, computing all relevant molecular and atomic photoionisation cross-sections and Auger rates. We find that the charge distribution of the carbon and oxygen ion yields differ. By varying the photon energy, we demonstrate how to control higher-charged states being populated mostly by carbon or oxygen. Moreover, we identify the differences in the resulting ion yields and pathways populating these yields between a homonuclear molecule, molecular nitrogen, and a heteronuclear molecule, carbon monoxide, interacting with an FEL pulse. These two molecules have similar electronic structure. We also identify the proportion of each ion yield which accesses a two-site double-core-hole state and tailor pulse parameters to maximise this proportion., Comment: 16 pages, 4 figures

Audio event classification is an important task for several applications such as surveillance, audio, video and multimedia retrieval etc. There are approximately 3M people with hearing loss who can't perceive events happening around them. This paper establishes the CURE dataset which contains curated set of specific audio events most relevant for people with hearing loss. We propose a ladder network based audio event classifier that utilizes 5s sound recordings derived from the Freesound project. We adopted the state-of-the-art convolutional neural network (CNN) embeddings as audio features for this task. We also investigate extreme learning machine (ELM) for event classification. In this study, proposed classifiers are compared with support vector machine (SVM) baseline. We propose signal and feature normalization that aims to reduce the mismatch between different recordings scenarios. Firstly, CNN is trained on weakly labeled Audioset data. Next, the pre-trained model is adopted as feature extractor for proposed CURE corpus. We incorporate ESC-50 dataset as second evaluation set. Results and discussions validate the superiority of Ladder network over ELM and SVM classifier in terms of robustness and increased classification accuracy. While Ladder network is robust to data mismatches, simpler SVM and ELM classifiers are sensitive to such mismatches, where the proposed normalization techniques can play an important role. Experimental studies with ESC-50 and CURE corpora elucidate the differences in dataset complexity and robustness offered by proposed approaches., Comment: 6 pages, 2 Figures

Reverberation negatively impacts the performance of automatic speech recognition (ASR). Prior work on quantifying the effect of reverberation has shown that clarity (C50), a parameter that can be estimated from the acoustic impulse response, is correlated with ASR performance. In this paper we propose predicting ASR performance in terms of the word error rate (WER) directly from acoustic parameters via a polynomial, sigmoidal, or neural network fit, as well as blindly from reverberant speech samples using a convolutional neural network (CNN). We carry out experiments on two state-of-the-art ASR models and a large set of acoustic impulse responses (AIRs). The results confirm C50 and C80 to be highly correlated with WER, allowing WER to be predicted with the proposed fitting approaches. The proposed non-intrusive CNN model outperforms C50-based WER prediction, indicating that WER can be estimated blindly, i.e., directly from the reverberant speech samples without knowledge of the acoustic parameters., Comment: Presented at IEEE 45th International Conference on Acoustics, Speech, and Signal Processing (ICASSP 2020)