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.

Read more » about Direct measurement of Coulomb-laser coupling, Open in new window

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.

Read more » about Enantioselective orientation of chiral molecules induced by terahertz pulses with twisted polarization, Open in new window

Impulsive orientation of symmetric-top molecules excited by two-color femtosecond pulses is considered. In addition to the well-known transient orientation appearing immediately after the pulse and then reemerging periodically due to quantum revivals, we report the phenomenon of field-free long-lasting orientation. Long-lasting means that the time averaged orientation remains non-zero until destroyed by other physical effects, e.g., intermolecular collisions. The effect is caused by the combined action of the field-polarizability and field-hyperpolarizability interactions. The dependence of degree of long-lasting orientation on temperature and pulse parameters is considered. The effect can be measured by means of second (or higher-order) harmonic generation, and may be used to control the deflection of molecules traveling through inhomogeneous electrostatic fields.

Read more » about Long-Lasting Orientation of Symmetric-top Molecules Excited by Two-Color Femtosecond Pulses, Open in new window

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.

Read more » about A three-step model of high harmonic generation using complex classical trajectories, Open in new window

Impulsive orientation of symmetric-top molecules excited by two-color femtosecond pulses is considered. In addition to the well-known transient orientation appearing immediately after the pulse and then reemerging periodically due to quantum revivals, we report the phenomenon of field-free long-lasting orientation. Long-lasting means that the time averaged orientation remains non-zero until destroyed by other physical effects, e.g., intermolecular collisions. The effect is caused by the combined action of the field-polarizability and field-hyperpolarizability interactions. The dependence of degree of long-lasting orientation on temperature and pulse parameters is considered. The effect can be measured by means of second (or higher-order) harmonic generation, and may be used to control the deflection of molecules traveling through inhomogeneous electrostatic fields.

Read more » about Long-Lasting Orientation of Symmetric-top Molecules Excited by Two-Color Femtosecond Pulses, 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.

Read more » about Fast laser speckle suppression with an intracavity diffuser, Open in new window

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.

Read more » about Single-spin resonance in a van der Waals embedded paramagnetic defect, Open in new window

Gibbons and Hawking [Phys. Rev. D 15, 2738 (1977)] have shown that the horizon of de Sitter space emits radiation in the same way as the event horizon of the black hole. But actual cosmological horizons are not event horizons, except in de Sitter space. Nevertheless, this paper proves Gibbons' and Hawking's radiation formula as an exact result for any flat space expanding with strictly positive Hubble parameter. The paper gives visual and intuitive insight into why this is the case. The paper also indicates how cosmological horizons are related to the dynamical Casimir effect, which makes experimental tests with laboratory analogues possible.

Read more » about Cosmological horizons radiate, Open in new window

Multiply excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room-temperature single-particle spectroscopy of their emission has proved elusive due to the temporal and spectral overlap with emission from the singly excited and charged states. Here, we introduce biexciton heralded spectroscopy enabled by a single-photon avalanche diode array based spectrometer. This allows us to directly observe biexciton–exciton emission cascades and measure the biexciton binding energy of single quantum dots at room temperature, even though it is well below the scale of thermal broadening and spectral diffusion. Furthermore, we uncover correlations hitherto masked in ensembles of the biexciton binding energy with both charge-carrier confinement and fluctuations of the local electrostatic potential. Heralded spectroscopy has the potential of greatly extending our understanding of charge-carrier dynamics in multielectron systems and of parallelization of quantum optics protocols.

Read more » about Heralded Spectroscopy Reveals Exciton–Exciton Correlations in Single Colloidal Quantum Dots, Open in new window

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.

Read more » about Fast laser speckle suppression with an intracavity diffuser, Open in new window

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.

Read more » about cSPARCOM: Multi-detector reconstruction by confocal super-resolution correlation microscopy, Open in new window

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.

Read more » about Impulsively Excited Gravitational Quantum States: Echoes and Time-resolved Spectroscopy, Open in new window

Upconverting semiconductor quantum dots (QDs) combine the stability of an inorganic crystalline structure with the spectral tunability afforded by quantum confinement. Here, we present upconverting type-II/type-I colloidal double QDs that enable enhancement of the performance of near-infrared to visible photon upconversion in QDs and broadening the range of relevant materials used. The resulting ZnTe/CdSe@CdS@CdSe/ZnSe type-II/type-I double QDs possess a very high photoluminescence quantum yield, monoexponential decay dynamics, and a narrow line width, approaching those of state-of-the-art upconverting QDs. We quantitatively characterize the upconversion cross section by direct comparison with two-photon absorption when varying the pump frequency across the absorption edge. Finally, we show that these upconversion QDs maintain their optical performance in a much more demanding geometry of a dense solid film and can thus be incorporated in devices as upconversion films. Our design provides guidance for fabricating highly efficient upconverting QDs with potential applications such as security coding and bioimaging.

Read more » about Bright Near-Infrared to Visible Upconversion Double Quantum Dots Based on a Type-II/Type-I Heterostructure, Open in new window

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

We introduce and demonstrate a scheme for eliminating the inhomogeneous dephasing of a collective quantum state. The scheme employs off-resonant fields that continuously dress the collective state with an auxiliary sensor state, which has an enhanced and opposite sensitivity to the same source of inhomogeneity. We derive the optimal conditions under which the dressed state is fully protected from dephasing when using either one or two dressing fields. The latter provides better protection, circumvents qubit phase rotation, and suppresses the sensitivity to drive noise. We further derive expressions for all residual, higher-order sensitivities. We experimentally study the scheme by protecting a collective excitation of an atomic ensemble, where inhomogeneous dephasing originates from thermal motion. Using photon storage and retrieval, we demonstrate complete suppression of inhomogeneous dephasing and, consequently, a prolonged memory time. Our scheme may be applied to eliminate motional dephasing in other systems, improving the performance of quantum gates and memorieswith neutral atoms. It is also generally applicable to various gas, solid, and engineered systems, where sensitivity to variations in time, space, or other domains limits possible scale-up of the system.

Read more » about Continuous Protection of a Collective State from Inhomogeneous Dephasing, Open in new window

We study the evolution of a Bose–Einstein condensate in a two-state superposition due to inter-state interactions. Using a population imbalanced dynamic decoupling scheme, we measure inter-state interactions while canceling intra-state density shifts and external noise sources. Our measurements show low statistical uncertainties for both magnetic sensitive and insensitive superpositions, indicating that we successfully decoupled our system from strong magnetic noises. We experimentally show that the Bloch sphere representing general superposition states is 'twisted' by inter-state interactions, as predicted in [1, 2] and the twist rate depends on the difference between inter-state and intra-state scattering lengths a22 + a11 − 2a12. We use the non-linear spin dynamics to demonstrate squeezing of Gaussian noise, showing 2.79 ± 0.43 dB squeezing when starting with a noisy state and applying 160 echo pulses, which can be used to increase sensitivity when there are errors in state preparation. Our results allow for a better understanding of inter-atomic potentials in 87Rb. Our scheme can be used for spin-squeezing beyond the standard quantum limit and observing polaron physics close to Feshbach resonances, where interactions diverge, and strong magnetic noises are ever present.

Read more » about Observation of nonlinear spin dynamics and squeezing in a BEC using dynamic decoupling, Open in new window

Localized surface plasmon resonances of individual sub-wavelength cavities milled in metallic films can couple to each other to form a collective behavior. This coupling leads to a delocalization of the plasmon field at the film surface and drastically alters both the linear and nonlinear optical properties of the sample. In periodic arrays of nanocavities, the coupling results in the formation of propagating surface plasmon polaritons (SPP), eigenmodes extending across the array. When artificially introducing dislocations, defects and imperfections, multiple scattering of these SPP modes can lead to hot-spot formation, intense and spatially confined fluctuations of the local plasmonic field within the array. Here, we study the underlying coupling effects by probing plasmonic modes in well-defined individual triangular dimer cavities and in arrays of triangular cavities with and without artificial defects. Nonlinear confocal spectro-microscopy is employed to map the second harmonic (SH) radiation from these systems. Pronounced spatial localization of the SPP field and significant enhancements of the SH intensity in certain, randomly distributed hot spots by more than an order of magnitude are observed from the triangular arrays as compared to a bare silver film by introducing a finite degree of disorder into the array structure. Hot-spot formation and the resulting enhancement of the nonlinear efficiency are correlated with an increase in the lifetime of the localized SPP modes. By using interferometric SH autocorrelation measurements, we reveal lifetimes of hot-spot resonances in disordered arrays that are much longer than the few-femtosecond lifetimes of the localized surface plasmon resonances of individual nanocavity dimers. This suggests that hot spot lifetime engineering provides a path for manipulating the linear and nonlinear optical properties of nanosystems by jointly exploiting coherent couplings and tailored disorder.

Read more » about Space- and time-resolved second harmonic spectroscopy of coupled plasmonic nanocavities, Open in new window