We fabricate an extremely thin optical fiber that supports a super-extended mode with a diameter as large as 13 times the optical wavelength, residing almost entirely outside the fiber and guided over thousands of wavelengths (5 mm), in order to couple guided light to warm atomic vapor. This unique configuration balances between strong confinement, as evident by saturation powers as low as tens of nW, and long interaction times with the thermal atoms, thereby enabling fast and coherent interactions. We demonstrate narrow coherent resonances (tens of MHz) of electromagnetically induced transparency for signals at the single-photon level and long relaxation times (10 ns) of atoms excited by the guided mode. The dimensions of the guided mode's evanescent field are compatible with the Rydberg blockade mechanism, making this platform particularly suitable for observing quantum non-linear optics phenomena.

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We describe the setup and the performance of a new pulsed Stern-Gerlach deflector and present results for small sodium-doped ammonia clusters Na(NH3)n (n = 1-4) in a molecular beam. NaNH3 shows the expected deflection of a spin ½ system, while all lager clusters show much smaller deflections. Experimental deflection ratios are compared with the values calculated from molecular dynamics simulations. The comparison reveals that intracluster spin relaxation in NaNH3 takes place on a time scale significantly longer than 200 μs. Assuming that intracluster relaxation is the cause of the reduced deflection, relaxation times seem to be on the order of 200 μs for all larger clusters Na(NH3)n (n = 2-4). Our work is a first attempt to understand the magnetic properties of isolated, weakly-bound clusters with relevance to the variety of diamagnetic and paramagnetic species expected in solvated electron systems. 

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Radical pairs and the dynamics they undergo are prevalent in many chemical and biological systems. Specifically, it has been proposed that the radical-pair mechanism results from a relatively strong hyperfine interaction with its intrinsic nuclear spin environment. While the existence of this mechanism is undisputed, the nanoscale details remain to be experimentally shown. Here, we analyze the role of a quantum sensor in detecting the spin dynamics (non-Markovian) of individual radical pairs in the presence of a weak magnetic field. We show how quantum control methods can be used to set apart the dynamics of the radical-pair mechanism at various stages of the evolution. We expect these findings to have implications to the understanding of the physical mechanism in magnetoreception and other biochemical processes with a microscopic detail.

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This Conceptual Design Report describes LUXE (Laser Und XFEL Experiment), an experimental campaign that aims to combine the high-quality and high-energy electron beam of the European XFEL with a powerful laser to explore the uncharted terrain of quantum electrodynamics characterised by both high energy and high intensity. We will reach this hitherto inaccessible regime of quantum physics by analysing high-energy electron-photon and photon-photon interactions in the extreme environment provided by an intense laser focus. The physics background and its relevance are presented in the science case which in turn leads to, and justifies, the ensuing plan for all aspects of the experiment: Our choice of experimental parameters allows (i) effective field strengths to be probed at and beyond the Schwinger limit and (ii) a precision to be achieved that permits a detailed comparison of the measured data with calculations. In addition, the high photon flux predicted will enable a sensitive search for new physics beyond the Standard Model. The initial phase of the experiment will employ an existing 40 TW laser, whereas the second phase will utilise an upgraded laser power of 300 TW. All expectations regarding the performance of the experimental set-up as well as the expected physics results are based on detailed numerical simulations throughout.

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Correlations between excitons, that is, electron-hole pairs, have a great impact on the optoelectronic properties of semiconductor quantum dots and thus are relevant for applications such as lasers and photovoltaics. Upon multiphoton excitation, these correlations lead to the formation of multiexciton states. It is challenging to observe these states spectroscopically, especially higher multiexciton states, because of their short lifetimes and nonradiative decay. Moreover, solvent contributions in experiments with coherent signal detection may complicate the analysis. Here we employ multiple-quantum two-dimensional (2D) fluorescence spectroscopy on colloidal CdSe1-xS x /ZnS alloyed core/shell quantum dots. We selectively map the electronic structure of multiexcitons and their correlations by using two- and three-quantum 2D spectroscopy, conducted in a simultaneous measurement. Our experiments reveal the characteristics of biexcitons and triexcitons such as transition dipole moments, binding energies, and correlated transition energy fluctuations. We determine the binding energies of the first six biexciton states by simulating the two-quantum 2D spectrum. By analyzing the line shape of the three-quantum 2D spectrum, we find strong correlations between biexciton and triexciton states. Our method contributes to a more comprehensive understanding of multiexcitonic species in quantum dots and other semiconductor nanostructures.

Read more » about Observing Multiexciton Correlations in Colloidal Semiconductor Quantum Dots via Multiple-Quantum Two-Dimensional Fluorescence Spectroscopy, Open in new window

Nuclear spins of noble gases feature extremely long coherence times but are inaccessible to optical photons. Here, we realize a coherent interface between light and noble-gas spins that is mediated by alkali atoms. We demonstrate the optical excitation of the noble-gas spins and observe the coherent back action on the light in the form of high-contrast two-photon spectra. We report on a record two-photon linewidth of 5 ± 0.7 mHz above room temperature, corresponding to a 1-min coherence time. This experiment provides a demonstration of coherent bidirectional coupling between light and noble-gas spins, rendering their long-lived spin coherence accessible for manipulations in the optical domain.

Read more » about Coupling light to a nuclear spin gas with a two-photon linewidth of five millihertz, Open in new window

A quantum Kerr-nonlinear oscillator is a paradigmatic model in cavity and circuit quantum electrodynamics, and quantum optomechanics. We theoretically study the echo phenomenon in a single impulsively excited ("kicked") Kerr-nonlinear oscillator. We reveal two types of echoes, "quantum"and "classical"ones, emerging on the long and short time scales, respectively. The mechanisms of the echoes are discussed, and their sensitivity to dissipation is considered. These echoes may be useful for studying decoherence processes in a number of systems related to quantum information processing.

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Chirality and chiral molecules are key elements in modern chemical and biochemical industries. Individual addressing and the eventual separation of chiral enantiomers have been and still are important elusive tasks in molecular physics and chemistry, and a variety of methods have been introduced over the years to achieve these goals. Here, we theoretically demonstrate that a pair of cross-polarized THz pulses interacting with chiral molecules through their permanent dipole moments induces in these molecules an enantioselective orientation. This orientation persists for a long time, exceeding the duration of the THz pulses by several orders of magnitude, and its dependency on temperature and pulses' parameters is investigated. This persistent orientation may enhance the deflection of the molecules in inhomogeneous electromagnetic fields, potentially leading to viable separation techniques.

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The Coulomb interaction between a photoelectron and its parent ion plays an important role in a large range of light-matter interactions. In this paper we obtain a direct insight into the Coulomb interaction and resolve, for the first time, the phase accumulated by the laser-driven electron as it interacts with the Coulomb potential. Applying extreme-ultraviolet interferometry enables us to resolve this phase with attosecond precision over a large energy range. Our findings identify a strong laser-Coulomb coupling, going beyond the standard recollision picture within the strong-field framework. Transformation of the results to the time domain reveals Coulomb-induced delays of the electrons along their trajectories, which vary by tens of attoseconds with the laser field intensity.

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The rediscovery of the halide perovskite class of compounds and, in particular, the organic and inorganic lead halide perovskite (LHP) materials and lead-free derivatives has reached remarkable landmarks in numerous applications. First among these is the field of photovoltaics, which is at the core of today’s environmental sustainability efforts. Indeed, these efforts have born fruit, reaching to date a remarkable power conversion efficiency of 25.2% for a double-cation Cs, FA lead halide thin film device. Other applications include light and particle detectors as well as lighting. However, chemical and thermal degradation issues prevent perovskite-based devices and particularly photovoltaic modules from reaching the market. The soft ionic nature of LHPs makes these materials susceptible to delicate changes in the chemical environment. Therefore, control over their interface properties plays a critical role in maintaining their stability. Here we focus on LHP nanocrystals, where surface termination by ligands determines not only the stability of the material but also the crystallographic phase and crystal habit. A surface analysis of nanocrystal interfaces revealed the involvement of Brønsted type acid–base equilibrium in the modification of the ligand moieties present, which in turn can invoke dissolution and recrystallization into the more favorable phase in terms of minimization of the surface energy. A large library of surface ligands has already been developed showing both good chemical stability and good electronic surface passivation, resulting in near-unity emission quantum yields for some materials, particularly CsPbBr3. However, most of those ligands have a large organic tail hampering charge carrier transport and extraction in nanocrystal-based solid films.

Read more » about Effect of Surface Ligands in Perovskite Nanocrystals: Extending in and Reaching out, Open in new window

Chirality and chiral molecules are key elements in modern chemical and biochemical industries. Individual addressing and the eventual separation of chiral enantiomers have been and still are important elusive tasks in molecular physics and chemistry, and a variety of methods have been introduced over the years to achieve these goals. Here, we theoretically demonstrate that a pair of cross-polarized THz pulses interacting with chiral molecules through their permanent dipole moments induces in these molecules an enantioselective orientation. This orientation persists for a long time, exceeding the duration of the THz pulses by several orders of magnitude, and its dependency on temperature and pulses' parameters is investigated. This persistent orientation may enhance the deflection of the molecules in inhomogeneous electromagnetic fields, potentially leading to viable separation techniques.

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We present a new design for a pulsed supersonic-beam source, inspired by the Even-Lavie valve, which is about four times more energy efficient than its predecessor and can run at more than double the repetition rate without experiencing resonances. Its characteristics make it a better candidate as a source for cryogenic-related experiments as well as spectroscopy with rapidly pulsed lasers. The new design is also simpler to build and is more robust, making it accessible to a larger portion of the scientific community.

Read more » about Improved design for a highly efficient pulsed-valve supersonic source with extended operating frequency range, Open in new window

We present a new trajectory formulation of high harmonic generation that treats classically allowed and classically forbidden processes within a single dynamical framework. Complex trajectories orbit the nucleus, producing the stationary Coulomb ground state. When the field is turned on, these complex trajectories continue their motion in the field-dressed Coulomb potential and therefore tunnel ionization, unbound evolution and recollision are described within a single, seamless framework. The new formulation can bring mechanistic understanding to a broad range of strong field physics effects.

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Fast speckle suppression is crucial for time-resolved full-field imaging with laser illumination. Here, we introduce a method to accelerate the spatial decoherence of laser emission, achieving speckle suppression in the nanosecond integration time scale. The method relies on the insertion of an intracavity phase diffuser into a degenerate cavity laser to break the frequency degeneracy of transverse modes and broaden the lasing spectrum. The ultrafast decoherence of laser emission results in the reduction of speckle contrast to 3% in less than 1 ns.

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A plethora of single-photon emitters have been identified in the atomic layers of two-dimensional van der Waals materials1,2,3,4,5,6,7,8. Here, we report on a set of isolated optical emitters embedded in hexagonal boron nitride that exhibit optically detected magnetic resonance. The defect spins show an isotropic ge-factor of ~2 and zero-field splitting below 10 MHz. The photokinetics of one type of defect is compatible with ground-state electron-spin paramagnetism. The narrow and inhomogeneously broadened magnetic resonance spectrum differs significantly from the known spectra of in-plane defects. We determined a hyperfine coupling of ~10 MHz. Its angular dependence indicates an unpaired, out-of-plane delocalized π-orbital electron, probably originating from substitutional impurity atoms. We extracted spin–lattice relaxation times T1 of 13–17 μs with estimated spin coherence times T2 of less than 1 μs. Our results provide further insight into the structure, composition and dynamics of single optically active spin defects in hexagonal boron nitride.

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Scattering resonances play a central role in collision processes in physics and chemistry. They help build an intuitive understanding of the collision dynamics due to the spatial localization of the scattering wavefunctions. For resonances that are localized in the reaction region, located at short separation behind the centrifugal barrier, sharp peaks in the reaction rates are the characteristic signature, observed recently with state-of-the-art experiments in low-energy collisions. If, however, the localization occurs outside of the reaction region, mostly the elastic scattering is modified. This may occur due to above-barrier resonances, the quantum analogue of classical orbiting. By probing both elastic and inelastic scattering of metastable helium with deuterium molecules in merged-beam experiments, we differentiate between the nature of quantum resonances—tunnelling resonances versus above-barrier resonances—and corroborate our findings by calculating the corresponding scattering wavefunctions.

Read more » about Determining the nature of quantum resonances by probing elastic and reactive scattering in cold collisions, Open in new window

Fast speckle suppression is crucial for time-resolved full-field imaging with laser illumination. Here, we introduce a method to accelerate the spatial decoherence of laser emission, achieving speckle suppression in the nanosecond integration time scale. The method relies on the insertion of an intracavity phase diffuser into a degenerate cavity laser to break the frequency degeneracy of transverse modes and broaden the lasing spectrum. The ultrafast decoherence of laser emission results in the reduction of speckle contrast to 3% in less than 1 ns.

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Image scanning microscopy (ISM), an upgraded successor of the ubiquitous confocal microscope, facilitates up to two-fold improvement in lateral resolution, and has become an indispensable element in the toolbox of the bio-imaging community. Recently, super-resolution optical fluctuation image scanning microscopy (SOFISM) integrated the analysis of intensity-fluctuations information into the basic ISM architecture, to enhance its resolving power. Both of these techniques typically rely on pixel-reassignment as a fundamental processing step, in which the parallax of different detector elements to the sample is compensated by laterally shifting the point spread function (PSF). Here, we propose an alternative analysis approach, based on the recent high-performing sparsity-based super-resolution correlation microscopy (SPARCOM) method. Through measurements of DNA origami nano-rulers and fixed cells labeled with organic dye, we experimentally show that confocal SPARCOM (cSPARCOM), which circumvents pixel-reassignment altogether, provides enhanced resolution compared to pixel-reassigned based analysis. Thus, cSPARCOM further promotes the effectiveness of ISM, and particularly that of correlation based ISM implementations such as SOFISM, where the PSF deviates significantly from spatial invariance.

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We theoretically study an impulsively excited quantum bouncer (QB)—a particle bouncing off a surface in the presence of gravity. A pair of time-delayed pulsed excitations is shown to induce a wave-packet echo effect—a partial rephasing of the QB wave function appearing at twice the delay between pulses. In addition, an appropriately chosen observable [here, the population of the ground gravitational quantum state (GQS)] recorded as a function of the delay is shown to contain the transition frequencies between the GQSs, their populations, and partial phase information about the wave-packet quantum amplitudes. The wave-packet echo effect is a promising candidate method for precision studies of GQSs of ultracold neutrons, atoms, and antiatoms confined in closed gravitational traps.

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We fabricate an extremely thin optical fiber that supports a super-extended mode with a diameter as large as 13 times the optical wavelength, residing almost entirely outside the fiber and guided over thousands of wavelengths (5 mm), in order to couple guided light to warm atomic vapor. This unique configuration balances between strong confinement, as evident by saturation powers as low as tens of nW, and long interaction times with the thermal atoms, thereby enabling fast and coherent interactions. We demonstrate narrow coherent resonances (tens of MHz) of electromagnetically induced transparency for signals at the single-photon level and long relaxation times (10 ns) of atoms excited by the guided mode. The dimensions of the guided mode's evanescent field are compatible with the Rydberg blockade mechanism, making this platform particularly suitable for observing quantum non-linear optics phenomena.

Read more » about Super-extended nanofiber-guided field for coherent interaction with hot atoms, Open in new window