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Interatomic Coulombic Decay (ICD) and related interatomic and intermolecular autoionization mechanisms are ubiquitous decay processes of excited atoms and molecules in an environment. It is commonly accepted that the efficiency of ICD of an ionized atom in a cluster increases with an increasing number of nearest neighbors. Here, we present a method for experimental validation of this assumption by a site-specific and quantitative comparison of ICD and its main competitor, Auger decay, in core-level ionized Kr clusters. Our results are in quantitative agreement with scaled theoretical calculations on Kr2.

Nature Communications 12(1), 6107 (1-11) (2021). doi:10.1038/s41467-021-26193-z, Polycyclic aromatic hydrocarbons (PAHs) play an important role in interstellar chemistry and are subject to high energy photons that can induce excitation, ionization, and fragmentation. Previous studies have demonstrated electronic relaxation of parent PAH monocations over 10���100 femtoseconds as a result of beyond-Born-Oppenheimer coupling between the electronic and nuclear dynamics. Here, we investigate three PAH molecules: fluorene, phenanthrene, and pyrene, using ultrafast XUV and IR laser pulses. Simultaneous measurements of the ion yields, ion momenta, and electron momenta as a function of laser pulse delay allow a detailed insight into the various molecular processes. We report relaxation times for the electronically excited PAH*, PAH$^+$* and PAH$^{2+}$* states, and show the time-dependent conversion between fragmentation pathways. Additionally, using recoil-frame covariance analysis between ion images, we demonstrate that the dissociation of the PAH$^{2+}$ ions favors reaction pathways involving two-body breakup and/or loss of neutral fragments totaling an even number of carbon atoms., Published by Nature Publishing Group UK, [London]

Experiments involving the irradiation of water contained within magnesium hydroxide and alumina nanoparticle sludges were conducted and culminated in observations of an increased yield of molecular hydrogen when compared to the yield from the irradiation of bulk water. We show that there is a relationship linking this increased yield to the direct nanoscale ionization mechanism in the nanoparticles, indicating that electron emission from the nanoparticles drives new radiative pathways in the water. Because the chemical changes in these sludges are introduced by irradiation only, we have a genuinely unstirred system. This feature allows us to determine the diffusivity of the dissolved gas. Using the measured gas production rate, we have developed a method for modelling when hydrogen bubble formation will occur within the nanoparticle sludges. This model facilitates the determination of a consistent radiolytic consumption rate coinciding with the observations of bubble formation. Thus, we demonstrate a nanoscale radiation effect directly influencing the formation of molecular hydrogen.

Using multi-electron–ion coincidence measurements combined with high level calculations, we show that double ionisation of SO2 at 40.81 eV can be state selective. It leads to high energy products, in good yield, via a newly identified mechanism, which is likely to apply widely to multiple ionisation by almost all impact processes.

Optically pumped magnetometers (OPMs) based on alkali-atom vapors are ultra-sensitive devices for dc and low-frequency ac magnetic measurements. Here, in combination with fast-field-cycling hardware and high-resolution spectroscopic detection, we demonstrate applicability of OPMs in quantifying nuclear magnetic relaxation phenomena. Relaxation rate dispersion across the nT to mT field range enables quantitative investigation of extremely slow molecular motion correlations in the liquid state, with time constants > 1 ms, and insight into the corresponding relaxation mechanisms. The 10-20 fT/\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\sqrt{{\rm{H}}}{\rm{z}}$$\end{document}Hz sensitivity of an OPM between 10 Hz and 5.5 kHz 1H Larmor frequency suffices to detect magnetic resonance signals from ~ 0.1 mL liquid volumes imbibed in simple mesoporous materials, or inside metal tubing, following nuclear spin prepolarization adjacent to the OPM. High-resolution spectroscopic detection can resolve inter-nucleus spin-spin couplings, further widening the scope of application to chemical systems. Expected limits of the technique regarding measurement of relaxation rates above 100 s−1 are discussed., Nuclear spin polarization and relaxation can be studied using nuclear magnetic resonance (NMR). Here the authors demonstrate a combination of fast-field cycling and optical magnetometry techniques, to realize a NMR sensor that operates in the region of very low frequency and high relaxation rate.

Scientific reports 12(1), 20783 (2022). doi:10.1038/s41598-022-25249-4, We present real-world data processing on measured electron time-of-flight data via neural networks.Specifically, the use of disentangled variational autoencoders on data from a diagnostic instrumentfor online wavelength monitoring at the free electron laser FLASH in Hamburg. Without a-prioriknowledge the network is able to find representations of single-shot FEL spectra, which have a lowsignal-to-noise ratio. This reveals, in a directly human-interpretable way, crucial information aboutthe photon properties. The central photon energy and the intensity as well as very detector-specificfeatures are identified. The network is also capable of data cleaning, i.e. denoising, as well as theremoval of artefacts. In the reconstruction, this allows for identification of signatures with very lowintensity which are hardly recognisable in the raw data. In this particular case, the network enhancesthe quality of the diagnostic analysis at FLASH. However, this unsupervised method also has thepotential to improve the analysis of other similar types of spectroscopy data., Published by Macmillan Publishers Limited, part of Springer Nature, [London]

Enhanced high repetition rate coherent extreme ultraviolet (XUV) harmonics represent efficient probe of electron dynamics in atoms, molecules and solids. In this work, we used orthogonally-polarized two-color laser field to generate strong even and odd high order harmonics from molecular gas targets. The dynamics of odd and even harmonics from O2, and N2 gases were investigated by employing single- and two-color laser fields using the fundamental radiation and second harmonic of 1030 nm, 37 fs, 50 kHz pulses. The relative efficiencies of harmonics were analyzed as a function of the thickness of the barium borate crystal used for second harmonic generation. Defocusing-assisted phase matching conditions were achieved in N2 gas for different groups of XUV harmonics.

Scientific reports 11(1), 505 (2021). doi:10.1038/s41598-020-79818-6, Molecules can sequentially absorb multiple photons when irradiated by an intense X-ray pulse from a free-electron laser. If the time delay between two photoabsorption events can be determined, this enables pump-probe experiments with a single X-ray pulse, where the absorption of the first photon induces electronic and nuclear dynamics that are probed by the absorption of the second photon. Here we show a realization of such a single-pulse X-ray pump-probe scheme on N2 molecules, using the X-ray induced dissociation process as an internal clock that is read out via coincident detection of photoelectrons and fragment ions. By coincidence analysis of the kinetic energies of the ionic fragments and photoelectrons, the transition from a bound molecular dication to two isolated atomic ions is observed through the energy shift of the inner-shell electrons. Via ab-initio simulations, we are able to map characteristic features in the kinetic energy release and photoelectron spectrum to specific delay times between photoabsorptions. In contrast to previous studies where nuclear motions were typically revealed by measuring ion kinetics, our work shows that inner-shell photoelectron energies can also be sensitive probes of nuclear dynamics, which adds one more dimension to the study of light-matter interactions with X-ray pulses., Published by Macmillan Publishers Limited, part of Springer Nature, [London]

Various efforts have been made to overcome Doppler broadening in hyperfine measurement limitations in the atomic vapors spectroscopy and associated applications. The present study measured and calculated hyperfine resolved ellipsometric parameters through the near-normal reflectance spectra of the rubidium vapor cell in two experimental setups based on continuous and modulated pathway. The results indicated that valuable information could be extracted from the ellipsometric parameters about the atomic medium. Change in the ellipsometric parameters in each transition line confirms the existence of the elliptical polarization of the reflected light when it is exposed to the alkali metal vapor. Our results show that the ellipticity at 5S1/2 (Fg = 1, 2) → 5P1/2 (Fe = 1, 2) hyperfine transitions of 87Rb (D1 line) is small, and accordingly hyperfine transitions between the ground 5S1/2 (Fg = 2, 3) and excited 5P1/2 (Fe = 2, 3) states of the 85Rb isotope are considerable. These ellipsometric parameters, as phase difference, can trace the behavior of the relative orientation of the electric field and atom velocity in the interface based on van der Waals dipole–dipole interaction and is directly proportional to the strength of the light-matter interaction which extremely useful instead complicated atomic spectroscopic methods.

Trapped molecular ions in pure rovibronic states are desirable in experiments ranging from cold chemistry to searches for physics beyond the Standard Model. Resonance-enhanced multiphoton ionisation (REMPI) can be used to prepare molecular ions in specific internal states with high fidelities. However, in the presence of electric fields, ionisation spectra exhibit frequency shifts and the ionisation thresholds are broadened. For this reason, REMPI studies are normally conducted in low and highly homogeneous electric fields, whereas the operating principle of rf ion traps requires electric fields that vary in space and time. In order to investigate the impact of this on the state-selectivity of REMPI in ion traps, we have simulated the expected broadening of the ionisation threshold under various operating conditions of a typical linear Paul trap. In many cases, the width of the ionisation threshold exceeds the separation between rotational energy levels, preventing state-selective ionisation. Careful choice of the trapping and laser parameters during loading can reduce this broadening, enabling state-selective ionisation in some instances. Where this strategy is not sufficient, the broadening can be reduced further by rapidly switching the trapping voltages off and on again during loading. This has been demonstrated experimentally for a Coulomb crystal of $$^{40}\hbox {Ca}^+$$ 40 Ca + ions without descrystallising it.

Chiral molecules and their interactions are critical in a variety of chemical and biological processes. Circular dichroism (CD) is the most widely used optical technique to study chirality, often performed in a solution phase. However, CD has low-efficiency on the order of 0.01–1$$\%$$ % . Therefore, there is a growing need to develop high-efficiency chiroptical techniques, especially in gas-phase, to gain background-free in-depth insight into chiral interactions. By using mass spectrometry and strong-field ionization of limonene with elliptically polarized light, we demonstrate an efficient chiral discrimination method that produces a chiral signal of one to two orders of magnitude higher than the conventional CD. The chiral response exhibits a strong dependence on wavelength in the range of 1,300–2,400 nm, where the relative abundance of the ion yields alternates between the two enantiomers. The origin of enhanced enantio-sensitivity in intense laser fields is attributed to two mechanisms that rely on the recollision dynamics in a chiral system: (1) the excited ionic state dynamics mediated either by the laser field or by the recollision process, and (2) non-dipole effects that alter the electron’s trajectories. Our results can serve as a benchmark for testing and developing theoretical tools involving non-dipole effects in strong-field ionization of molecules.

A major challenge for organic solar cell (OSC) research is how to minimize the tradeoff between voltage loss and charge generation. In early 2019, we reported a non-fullerene acceptor (named Y6) that can simultaneously achieve high external quantum efficiency and low voltage loss for OSC. Here, we use a combination of experimental and theoretical modeling to reveal the structure-property-performance relationships of this state-of-the-art OSC system. We find that the distinctive π–π molecular packing of Y6 not only exists in molecular single crystals but also in thin films. Importantly, such molecular packing leads to (i) the formation of delocalized and emissive excitons that enable small non-radiative voltage loss, and (ii) delocalization of electron wavefunctions at donor/acceptor interfaces that significantly reduces the Coulomb attraction between interfacial electron-hole pairs. These properties are critical in enabling highly efficient charge generation in OSC systems with negligible donor-acceptor energy offset., Y6, as a non-fullerene acceptor for organic solar cells, has attracted intensive attention because of the low voltage loss and high charge generation efficiency. Here, Zhang et al. find that the delocalization of exciton and electron wavefunction due to strong π-π packing of Y6 is the key for the high performance.

This paper presents information on the gross alpha and gross beta activity concentrations of two hundred twenty-six groundwater samples collected by gas flow proportional counters in southern Vietnam. The gross alpha results in the water samples ranged from 0.024 to 0.748 Bq L−1 with a mean of 0.183 ± 0.034 Bq L−1, and the gross beta results in the water samples ranged from 0.027–0.632 Bq L−1 with a mean of 0.152 ± 0.015 Bq L−1. The values obtained in this work were compared with those previously published for various regions or countries. Next, untreated and treated groundwater samples were analyzed to assess their influences on the treatment process. The results showed that there were differences in the minimum detection concentrations and the mean activity values between the untreated and treated groundwater samples (The p-value of the mean comparison tests is significant with p 0.6). This means that among the radionuclides, the major sources of beta radiation are uranium and thorium decay series radionuclides. Finally, the annual effective dose for adults (>17 years) was calculated based on the assumption that major radionuclides have the highest effective dose conversion factors. In general, the results for Pb-210, Ra-226, and Ra-228 were observed to be lower than the recommended reference values established by the World Health Organization and the International Atomic Energy Agency, except for the value of Po-210.

The quantum mechanical motion of electrons and nuclei in systems spatially confined to the molecular dimensions occurs on the sub-femtosecond to the femtosecond timescales respectively. Consequently, the study of ultrafast electronic and, in specific cases, nuclear dynamics requires the availability of light pulses with attosecond (asec) duration and of sufficient intensity to induce two-photon processes, essential for probing the intrinsic system dynamics. The majority of atoms, molecules and solids absorb in the extreme-ultraviolet (XUV) spectral region, in which the synthesis of the required attosecond pulses is feasible. Therefore, the XUV spectral region optimally serves the study of such ultrafast phenomena. Here, we present a detailed review of the first 10-GW class XUV attosecond source based on laser driven high harmonic generation in rare gases. The pulse energy of this source largely exceeds other laser driven attosecond sources and is comparable to the pulse energy of femtosecond Free-Electron-Laser (FEL) XUV sources. The measured pulse duration in the attosecond pulse train is 650 ± 80 asec. The uniqueness of the combined high intensity and short pulse duration of the source is evidenced in non-linear XUV-optics experiments. It further advances the implementation of XUV-pump-XUV-probe experiments and enables the investigation of strong field effects in the XUV spectral region.

Air quality control is an important task in prevention of human exposure to toxic and harmful gases and requires reliable gas sensors. During last decades many gas sensing mechanisms, based on different physical or chemical interactions with sensitive materials, have been developed, but the problem of precise analysis of gas mixtures still remains. The problem can be solved by introducing new sensing mechanism based on an adiabatically changing electric field interacting with the rotational structure of the molecules with dipole moments. We have theoretically demonstrated a single low frequency gas detector that can be used for sensing of gas mixtures with high selectivity, accuracy, and sensitivity. The enhancement of the population difference between corresponding molecular levels and reached the theoretical maximum of absorption have been shown.

The relaxation of photoexcited nanosystems is a fundamental process of light–matter interaction. Depending on the couplings of the internal degrees of freedom, relaxation can be ultrafast, converting electronic energy in a few fs, or slow, if the energy is trapped in a metastable state that decouples from its environment. Here, we study helium nanodroplets excited resonantly by femtosecond extreme-ultraviolet (XUV) pulses from a seeded free-electron laser. Despite their superfluid nature, we find that helium nanodroplets in the lowest electronically excited states undergo ultrafast relaxation. By comparing experimental photoelectron spectra with time-dependent density functional theory simulations, we unravel the full relaxation pathway: Following an ultrafast interband transition, a void nanometer-sized bubble forms around the localized excitation (He∗) within 1 ps. Subsequently, the bubble collapses and releases metastable He∗ at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses., Funding from the Deutsche Forschungsgemeinschaft (MU 2347/8-1, STI 125/19-1, and the priority program 1840 QUTIF, the Carlsberg Foundation, National Science Foundation (DMR-1828019), Carl-Zeiss-Stiftung, Grant No. FIS2017-87801-P (AEI/FEDER, UE), and Swiss National Science Foundation (200020_162434) is gratefully acknowledged. O.G., D.M.N., and M.P.Z. were supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, through Contract No. DE-AC02-05CH11231.

We formulate a computationally efficient time-independent method based on the multi-electron molecular R-matrix formalism. This method is used to calculate transition matrix elements for the multi-photon ionization of atoms and molecules under the influence of a perturbative field. The method relies on the partitioning of space which allows us to calculate the infinite-range free-free dipole integrals analytically in the outer region, beyond the range of the initial bound wave function. This approach is valid for an arbitrary order, that is, any number of photons absorbed both in the bound and the continuum part of the spectrum (below- and above-threshold ionization). We calculate generalized multi-photon cross sections and angular distributions of different systems (H, He, \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\hbox {H}_{{2}}$$\end{document}H2, \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\hbox {CO}_{{2}}$$\end{document}CO2) and validate our approach by comparison with data from the literature.

The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220–250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states., Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe; 1301

Communications Physics 5(1), 110 (2022). doi:10.1038/s42005-022-00883-6, The driven quantum asymmetric top is an important paradigm in molecular physics with applications ranging from quantum information to chiral-sensitive spectroscopy. A key prerequisite for these applications is the ability to completely control the rotational dynamics. The inherent degeneracy of quantum rotors poses a challenge for quantum control since selecting a particular rotational state cannot be achieved by spectral selection alone. Here, we prove complete controllability for rotational states of an asymmetric top belonging to degenerate values of the orientational quantum number M. Based on this insight, we construct a pulse sequence that energetically separates population in degenerate M-states. Introducing the concept of enantio-selective controllability, we determine the conditions for complete enantiomer-specific population transfer in chiral molecules and construct pulse sequences for the example of propanediol and carvone molecules for population initially distributed over degenerate M-states. Our work shows how to leverage controllability analysis for the solution of practical quantum control problems., Published by Springer Nature, London

We study propagation effects due to the finite speed of light in ionization of extended molecular systems. We present a general quantitative theory of these effects and show under which conditions such effects should appear. The finite speed of light propagation effects are encoded in the non-dipole terms of the time-dependent Shrödinger equation and display themselves in the photoelectron momentum distribution projected on the molecular axis. Our numerical modeling for the $$\hbox {H}_{2}^{+}$$ H 2 + molecular ion and the $$\hbox {Ne}_2$$ Ne 2 dimer shows that the finite light propagation time from one atomic center to another can be accurately determined in a table top laser experiment which is much more readily accessible than the ground breaking synchrotron measurement by Grundmann et al. (Science 370:339, 2020).

The positron, the antiparticle of the electron, predicted by Dirac in 1931 and discovered by Anderson in 1933, plays a key role in many scientific and everyday endeavours. Notably, the positron is a constituent of antihydrogen, the only long-lived neutral antimatter bound state that can currently be synthesized at low energy, presenting a prominent system for testing fundamental symmetries with high precision. Here, we report on the use of laser cooled Be+ ions to sympathetically cool a large and dense plasma of positrons to directly measured temperatures below 7 K in a Penning trap for antihydrogen synthesis. This will likely herald a significant increase in the amount of antihydrogen available for experimentation, thus facilitating further improvements in studies of fundamental symmetries., Positrons are key to the production of cold antihydrogen. Here the authors report the sympathetic cooling of positrons by interacting them with laser-cooled Be+ ions resulting in a three-fold reduction of the temperature of positrons for antihydrogen synthesis.

We propose a novel and simple method for the laser isotope separation of 176Lu a precursor for the production of 177Lu medical isotope. The physics of the laser-atom interaction has been studied through the dynamics of the atomic level populations using the density matrix formalism. It has been shown that a combination of cw excitation lasers and pulsed ionization laser can be used for the laser isotope separation of 176Lu. The optimum conditions for the efficient and selective separation of 176Lu have been derived by studying the time evolution of level population under laser excitation. It has also been shown that, it might be possible to produce ~ 100% enriched 176Lu isotope at a rate of 5 mg/h, which is higher than all previously reported methods so far. The isotope separation process proposed can be easily adopted using off-the-shelf lasers, for similar atomic systems.

We present a computational case study of X-ray single-particle imaging of hydrated proteins on an example of 2-Nitrogenase–Iron protein covered with water layers of various thickness, using a start-to-end simulation platform and experimental parameters of the SPB/SFX instrument at the European X-ray Free-Electron Laser facility. The simulations identify an optimal thickness of the water layer at which the effective resolution for imaging the hydrated sample becomes significantly higher than for the non-hydrated sample. This effect is lost when the water layer becomes too thick. Even though the detailed results presented pertain to the specific sample studied, the trends which we identify should also hold in a general case. We expect these findings will guide future single-particle imaging experiments using hydrated proteins.

Characterizing time delays in molecular photoionization as a function of the ejected electron emission direction relative to the orientation of the molecule and the light polarization axis provides unprecedented insights into the attosecond dynamics induced by extreme ultraviolet or X-ray one-photon absorption, including the role of electronic correlation and continuum resonant states. Here, we report completely resolved experimental and computational angular dependence of single-photon ionization delays in NO molecules across a shape resonance, relying on synchrotron radiation and time-independent ab initio calculations. The angle-dependent time delay variations of few hundreds of attoseconds, resulting from the interference of the resonant and non-resonant contributions to the dynamics of the ejected electron, are well described using a multichannel Fano model where the time delay of the resonant component is angle-independent. Comparing these results with the same resonance computed in e-NO+ scattering highlights the connection of photoionization delays with Wigner scattering time delays., It is an interesting topic to find the time it takes for an electron to escape an atom or a molecule after photoionization. Here the authors measure the angular dependence of photoionization time delay in the molecular frame and discuss the role of shape resonances.

Laser-assisted electron scattering (LAES), a light–matter interaction process that facilitates energy transfer between strong light fields and free electrons, has so far been observed only in gas phase. Here we report on the observation of LAES at condensed phase particle densities, for which we create nano-structured systems consisting of a single atom or molecule surrounded by a superfluid He shell of variable thickness (32–340 Å). We observe that free electrons, generated by femtosecond strong-field ionization of the core particle, can gain several tens of photon energies due to multiple LAES processes within the liquid He shell. Supported by Monte Carlo 3D LAES and elastic scattering simulations, these results provide the first insight into the interplay of LAES energy gain/loss and dissipative electron movement in a liquid. Condensed-phase LAES creates new possibilities for space-time studies of solids and for real-time tracing of free electrons in liquids., Laser-assisted electron scattering (LAES) is a commonly observed strong field process in gas phase systems. Here the authors use helium droplets with core atoms and molecules to observe increased electron energy due to multiple LAES events within the droplets.

We realize a two-stage, hexagonal pyramid magneto-optical trap (MOT) with strontium, and demonstrate loading of cold atoms into cavity-enhanced 1D and 2D optical lattice traps, all within a single compact assembly of in-vacuum optics. We show that the device is suitable for high-performance quantum technologies, focusing especially on its intended application as a strontium optical lattice clock. We prepare 2 × 104 spin-polarized atoms of 87Sr in the optical lattice within 500 ms; we observe a vacuum-limited lifetime of atoms in the lattice of 27 s; and we measure a background DC electric field of 12 V m−1 from stray charges, corresponding to a fractional frequency shift of (−1.2 ± 0.8) × 10−18 to the strontium clock transition. When used in combination with careful management of the blackbody radiation environment, the device shows potential as a platform for realizing a compact, robust, transportable optical lattice clock with systematic uncertainty at the 10−18 level.

Atomic systems have long provided a useful material platform with unique quantum properties. The efficient light-matter interaction in atomic vapors has led to numerous seminal scientific achievements including accurate and precise metrology and quantum devices. In the last few decades, the field of thin optical elements with miniscule features has been extensively studied demonstrating an unprecedented ability to control photonic degrees of freedom, both linearly and non-linearly, with applications spanning from photography and spatial light modulators to cataract surgery implants. Hybridization of atoms with such thin devices may offer a new material system allowing traditional vapor cells with enhanced functionality. Here, we fabricate and demonstrate chip-scale, quantum diffractive optical elements which map atomic states to the spatial distribution of diffracted light. Two foundational diffractive elements, lamellar gratings and Fresnel lenses, are hybridized with atomic channels containing hot atomic vapors which demonstrate exceptionally strong frequency dependent behaviors. Providing the design tools for chip-scale atomic diffractive optical elements develops a path for a variety of compact thin quantum-optical elements., Comment: 9 Pages, including supplementary

Exotic spin-dependent interactions between fermions have recently attracted attention in relation to theories beyond the Standard Model. The exotic interactions can be mediated by hypothetical fundamental bosons which may explain several unsolved mysteries in physics. Here we expand this area of research by probing an exotic parity-odd spin- and velocity-dependent interaction between the axial-vector electron coupling and the vector nucleon coupling for polarized electrons. This experiment utilizes a high-sensitivity atomic magnetometer, based on an optically polarized vapor that is a source of polarized electrons, and a solid-state mass containing unpolarized nucleons. The atomic magnetometer can detect an effective magnetic field induced by the exotic interaction between unpolarized nucleons and polarized electrons. We set an experimental limit on the electron-nucleon coupling \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$g_{\mathrm{A}}^{\mathrm{e}}g_{\mathrm{V}}^{\mathrm{N}} \, < \, 10^{ - 30}$$\end{document}gAegVN, Symmetry breaking is an important process in fundamental understanding of matter and dark matter. Here the authors discuss an experimental bound on an exotic parity odd spin- and velocity-dependent interaction between electron and nucleon by using a sensitive spin-exchange relaxation-free atomic magnetometer.

Non-classical photon sources are a crucial resource for distributed quantum networks. Photons generated from matter systems with memory capability are particularly promising, as they can be integrated into a network where each source is used on-demand. Among all kinds of solid state and atomic quantum memories, room-temperature atomic vapours are especially attractive due to their robustness and potential scalability. To-date room-temperature photon sources have been limited either in their memory time or the purity of the photonic state. Here we demonstrate a single-photon source based on room-temperature memory. Following heralded loading of the memory, a single photon is retrieved from it after a variable storage time. The single-photon character of the retrieved field is validated by the strong suppression of the two-photon component with antibunching as low as \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${g}_{{\rm{RR| W = 1}}}^{(2)}=0.20\pm 0.07$$\end{document}gRR∣W=1(2)=0.20±0.07. Non-classical correlations between the heralding and the retrieved photons are maintained for up to \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${\tau }_{{\rm{NC}}}^{{\mathcal{R}}}=(0.68\pm 0.08)\ {\rm{ms}}$$\end{document}τNCR=(0.68±0.08)ms, more than two orders of magnitude longer than previously demonstrated with other room-temperature systems. Correlations sufficient for violating Bell inequalities exist for up to τBI = (0.15 ± 0.03) ms., Room-temperature single photon sources with memory capabilities are promising for quantum information processing, but are currently limited in their memory time or photon purity. Here, the authors report single photon emission with good antibunching from an atomic vapour cell source with 0.68 ms memory time.

For more than one century, low-energy (

More than 100 years after its discovery and its explanation in the energy domain, the duration of the photoelectric effect is still heavily studied. The emission time of a photoelectron can be quantified by the Wigner time delay. Experiments addressing this time delay for single-photon ionization became feasible during the last 10 years. A missing piece, which has not been studied, so far, is the Wigner time delay for strong-field ionization of molecules. Here we show experimental data on the Wigner time delay for tunnel ionization of $H_{2}$ molecules and demonstrate its dependence on the emission direction of the electron with respect to the molecular axis. We find, that the observed changes in the Wigner time delay can be quantitatively explained by elongated/shortened travel paths of the electrons that are due to spatial shifts of the electron's birth position after tunneling. This introduces an intuitive perspective towards the Wigner time delay in strong-field ionization., Comment: 17 pages, 6 figures

We describe a procedure that allows us to solve the three-dimensional time-dependent Schrödinger equation for an atom interacting with a quantized one-mode electromagnetic field. Atom-field interaction is treated in an ab initio way prescribed by quantum electrodynamics. We use the procedure to calculate probability distributions of absorbed photons in the regime of tunneling ionization. We analyze evolution of the reduced photon density matrix describing the state of the field. We show that non-diagonal density matrix elements decay quickly, as a result of the decoherence process. A stochastic model, viewing ionization as a Markovian birth-death process, reproduces the main features of the calculated photon distributions.

Hyperradiance in which radiation rate exceeds that of superradiance has been theoretically investigated in various coherently-coupled emitter-field systems. In most cases, either proposed setups were experimentally challenging or the mean photon number in a cavity was limited. In this paper, with numerical simulations and analytic calculations, we demonstrate that significant hyperradiance with a large mean photon number can occur in a microlaser system, where pairs of two-level atoms prepared in quantum superposition states traverse a high-Q cavity in the presence of a pump field intersecting the cavity mode. Hyperradiance is induced when the intracavity-pump Rabi frequency is out of phase with respect to the atom-cavity coupling so that the reduction of atomic polarization by the atom-cavity coupling is compensated by the pump Rabi frequency in the steady state to maximize atomic photoemission.

Realizing a long coherence time quantum memory is a major challenge of current quantum technology. Until now, the longest coherence-time of a single qubit was reported as 660 s in a single 171Yb+ ion-qubit through the technical developments of sympathetic cooling and dynamical decoupling pulses, which addressed heating-induced detection inefficiency and magnetic field fluctuations. However, it was not clear what prohibited further enhancement. Here, we identify and suppress the limiting factors, which are the remaining magnetic-field fluctuations, frequency instability and leakage of the microwave reference-oscillator. Then, we observe the coherence time of around 5500 s for the 171Yb+ ion-qubit, which is the time constant of the exponential decay fit from the measurements up to 960 s. We also systematically study the decoherence process of the quantum memory by using quantum process tomography and analyze the results by applying recently developed resource theories of quantum memory and coherence. Our experimental demonstration will accelerate practical applications of quantum memories for various quantum information processing, especially in the noisy-intermediate-scale quantum regime., Extending qubit coherence times represent one of the key challenges for quantum technologies. Here, after properly suppressing magnetic-field fluctuations, frequency instability and leakage of the microwave reference-oscillator, the authors infer coherence times of 5500 s for an Yb ion qubit.

Nature Communications 12(1), 6657 (2021). doi:10.1038/s41467-021-26994-2, How long does it take to emit an electron from an atom? This question has intrigued scientists for decades. As such emission times are in the attosecond regime, the advent of attosecond metrology using ultrashort and intense lasers has re-triggered strong interest on the topic from an experimental standpoint. Here, we present an approach to measure such emission delays, which does not require attosecond light pulses, and works without the presence of superimposed infrared laser fields. We instead extract the emission delay from the interference pattern generated as the emitted photoelectron is diffracted by the parent ion���s potential. Targeting core electrons in CO, we measured a 2d map of photoelectron emission delays in the molecular frame over a wide range of electron energies. The emission times depend drastically on the photoelectrons��� emission directions in the molecular frame and exhibit characteristic changes along the shape resonance of the molecule., Published by Nature Publishing Group UK, [London]

Improved optical control of molecular quantum states promises new applications including chemistry in the quantum regime, precision tests of fundamental physics, and quantum information processing. While much work has sought to prepare ground state molecules, excited states are also of interest. Here, we demonstrate a broadband optical approach to pump trapped SiO+ molecules into pure super rotor ensembles maintained for many minutes. Super rotor ensembles pumped up to rotational state N = 67, corresponding to the peak of a 9400 K distribution, had a narrow N spread comparable to that of a few-kelvin sample, and were used for spectroscopy of the previously unobserved C2Π state. Significant centrifugal distortion of super rotors pumped up to N = 230 allowed probing electronic structure of SiO+ stretched far from its equilibrium bond length., Optical pulses can be useful to create and control molecules in higher quantum states. Here the authors use optical pumping to create rotationally excited states of SiO+ molecular ion into super rotor ensemble.

Extinction spectroscopy is a powerful tool for demonstrating the coupling of a single quantum emitter to a photonic structure. However, it can be challenging in all but the simplest of geometries to deduce an accurate value of the coupling efficiency from the measured spectrum. Here we develop a theoretical framework to deduce the coupling efficiency from the measured transmission and reflection spectra without precise knowledge of the photonic environment. We then consider the case of a waveguide interrupted by a transverse cut in which an emitter is placed. We apply that theory to a silicon nitride waveguide interrupted by a gap filled with anthracene that is doped with dibenzoterrylene molecules. We describe the fabrication of these devices, and experimentally characterise the waveguide coupling of a single molecule in the gap., 10 page article with 3 figures and 6 page supplementary information with 3 figures. Comments welcome