High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration.

High-harmonic spectroscopy is an all-optical technique with inherent attosecond temporal resolution that has been successfully employed to reconstruct charge migration, electron-tunneling dynamics, and conical-intersection dynamics. Here, we demonstrate the extension of two key components of high-harmonic spectroscopy, i.e.

Bioactive Protein and Peptide Release from a Mucoadhesive Electrospun Membrane.

Protein-based biologics constitute a rapidly expanding category of therapeutic agents with high target specificity. Their clinical use has dramatically increased in recent years, but administration is largely via injection. Drug delivery across the oral mucosa is a promising alternative to injections, in order to avoid the gastrointestinal tract and first-pass metabolism.

Oral lichen planus clinician reported outcome measure: Development, content validity, and further development.

Objective: To establish and test a clinician-reported outcome measure of oral lichen planus (OLP): OLP Investigator global assessment (IGA).

Methods: OLP IGA scale was tested with retrospective data from clinical practice and a phase II clinical trial. A comparison of the OLP IGA score with patient-reported outcomes was completed.

Entanglement of orbital angular momentum in non-sequential double ionization.

Entanglement has a capacity to enhance imaging procedures, but this remains unexplored for attosecond imaging. Here, we elucidate that possibility, addressing orbital angular momentum (OAM) entanglement in ultrafast processes. In the correlated process non-sequential double ionization (NSDI) we demonstrate robust photoelectron entanglement.

Quantum computational advantage with a programmable photonic processor.

A quantum computer attains computational advantage when outperforming the best classical computers running the best-known algorithms on well-defined tasks. No photonic machine offering programmability over all its quantum gates has demonstrated quantum computational advantage: previous machines were largely restricted to static gate sequences. Earlier photonic demonstrations were also vulnerable to spoofing, in which classical heuristics produce samples, without direct simulation, lying closer to the ideal distribution than do samples from the quantum hardware.

Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in - 2 Intense Laser Fields.

Dissociative ionization of tetrafluoromethane (CF) in linearly polarized -2 ultrashort intense laser fields (1.4 × 10 W/cm, 800 and 400 nm) has been investigated by three-dimensional momentum ion imaging. The spatial distribution of produced by CF → + F + e exhibited a clear asymmetry with respect to the laser polarization direction.

Modelling of the dynamic polarizability of macromolecules for single-molecule optical biosensing.

The structural dynamics of macromolecules is important for most microbiological processes, from protein folding to the origins of neurodegenerative disorders. Noninvasive measurements of these dynamics are highly challenging. Recently, optical sensors have been shown to allow noninvasive time-resolved measurements of the dynamic polarizability of single-molecules.

Quantum computational advantage via high-dimensional Gaussian boson sampling.

Photonics is a promising platform for demonstrating a quantum computational advantage (QCA) by outperforming the most powerful classical supercomputers on a well-defined computational task. Despite this promise, existing proposals and demonstrations face challenges. Experimentally, current implementations of Gaussian boson sampling (GBS) lack programmability or have prohibitive loss rates.

Efficacy and safety of a novel mucoadhesive clobetasol patch for treatment of erosive oral lichen planus: A phase 2 randomized clinical trial.

Background: Oral lichen planus (OLP) is a chronic inflammatory disorder of the oral mucosa. Currently there is no approved treatment for OLP. We report on the efficacy and safety of a novel mucoadhesive clobetasol patch (Rivelin -CLO) for the treatment of OLP.

Quantum-enhanced nonlinear microscopy.

The performance of light microscopes is limited by the stochastic nature of light, which exists in discrete packets of energy known as photons. Randomness in the times that photons are detected introduces shot noise, which fundamentally constrains sensitivity, resolution and speed. Although the long-established solution to this problem is to increase the intensity of the illumination light, this is not always possible when investigating living systems, because bright lasers can severely disturb biological processes.

Quantum noise limited nanoparticle detection with exposed-core fiber.

Label-free biosensors are important tools for clinical diagnostics and for studying biology at the single molecule level. The development of optical label-free sensors has allowed extreme sensitivity but can expose the biological sample to photodamage. Moreover, the fragility and complexity of these sensors can be prohibitive to applications.

Excitation spectra of systems of indistinguishable particles by the autocorrelation function technique: Circumventing the exponential scaling for bosons.

We consider the autocorrelation function technique for obtaining excitation spectra for indistinguishable particles. The interacting particles are described by coherent superpositions of configurations built from time-dependent spin-orbitals. The fermionic or bosonic character of the particles is taken into account by considering Slater determinants or permanents, respectively.

Novel Oral Lichen Planus Symptom Severity Measure for assessing patients' daily symptom experience.

Objective: A novel Oral Lichen Planus Symptom Severity Measure was developed as a clinical outcome assessment of the daily symptom experience of patients with oral lichen planus.

Methods: A literature review and expert input were followed by open-ended concept elicitation interviews with 17 adults with oral lichen planus in the United States and Ireland. Item content was generated, and the interviews continued until input saturation was reached.

Effects of core space and excitation levels on ground-state correlation and photoionization dynamics of Be and Ne.

We explore the effects of correlation on the ground-state energies and on photoionization dynamics in atomic Be and Ne. We apply the time-dependent restricted-active-space self-consistent-field method for several excitation schemes and active orbital spaces with and without a dynamic core to address the effects systematically at different levels of approximation. For the ground-state many-electron wave functions, we compare the correlation energies with entropic measures of entanglement.

Structure factors for tunneling ionization rates of molecules: General grid-based methodology and convergence studies.

We present a general methodology for evaluating structure factors defining the orientation dependence of tunneling ionization rates of molecules, which is a key process in strong-field physics. The method is implemented at the Hartree-Fock level of electronic structure theory and is based on an integral-equation approach to the weak-field asymptotic theory of tunneling ionization, which expresses the structure factor in terms of an integral involving the ionizing orbital and a known analytical function. The evaluation of the required integrals is done by three-dimensional quadrature which allows calculations using conventional quantum chemistry software packages.

Entangled Quantum Dynamics of Many-Body Systems using Bohmian Trajectories.

Bohmian mechanics is an interpretation of quantum mechanics that describes the motion of quantum particles with an ensemble of deterministic trajectories. Several attempts have been made to utilize Bohmian trajectories as a computational tool to simulate quantum systems consisting of many particles, a very demanding computational task. In this paper, we present a novel ab-initio approach to solve the many-body problem for bosonic systems by evolving a system of one-particle wavefunctions representing pilot waves that guide the Bohmian trajectories of the quantum particles.

Signatures of a Conical Intersection in Attosecond Transient Absorption Spectroscopy.

We characterize attosecond transient absorption spectroscopy (ATAS) in molecules with coupled nuclear and electronic dynamics in the vicinity of a conical intersection between adiabatic potential energy surfaces. With respect to ATAS, the nonadiabatic vibronic coupling strength can be divided into weak, intermediate, and strong, and the characteristics of spectra belonging to each of these domains are discussed. The results can guide the analysis of ATAS experiments in molecules with conical intersections.

Nondestructive Profilometry of Optical Nanofibers.

Single-mode optical nanofibers are a central component of a broad range of applications and emerging technologies. Their fabrication has been extensively studied over the past decade, but imaging of the final submicrometer products has been restricted to destructive or low-precision techniques. Here, we demonstrate an optical scattering-based scanning method that uses a probe nanofiber to locally scatter the evanescent field of a sample nanofibre.

Illuminating Molecular Symmetries with Bicircular High-Order-Harmonic Generation.

We present a general theory of bicircular high-order-harmonic generation from N-fold rotationally symmetric molecules. Using a rotating frame of reference we predict the complete structure of the high-order-harmonic spectra for arbitrary driving frequency ratios and show how molecular symmetries can be directly identified from the harmonic signal. Our findings reveal that a characteristic fingerprint of rotational molecular symmetries can be universally observed in the ultrafast response of molecules to strong bicircular fields.

Role of Multi-Electron Effects in the Asymmetry of Strong-Field Ionization and Fragmentation of Polar Molecules: The Methyl Halide Series.

We report angle- and momentum-resolved measurements of the dissociative ionization and Coulomb explosion of methyl halides (CH3F, CH3Cl, CH3Br, and CH3I) in intense phase-controlled two-color laser fields. At moderate laser intensities, we find that the emission asymmetry of low-energy CH3(+) fragments from the CH3(+) + X(+) (X = F, Cl, Br, or I) channel reflects the asymmetry of the highest occupied molecular orbital of the neutral molecule with important contributions from the Stark effect. This asymmetry is correctly predicted by the weak-field asymptotic theory, provided that the Stark effect on the ionization potentials is calculated using a nonperturbative multielectron approach.

Characterization of Molecular Breakup by Very Intense Femtosecond XUV Laser Pulses.

We study the breakup of H2+ exposed to superintense, femtosecond laser pulses with frequencies greater than that corresponding to the ionization potential. By solving the time-dependent Schrödinger equation in an extensive field parameter range, it is revealed that highly nonresonant dissociation channels can dominate over ionization. By considering field-dressed Born-Oppenheimer potential energy curves in the reference frame following a free electron in the field, we propose a simple physical model that characterizes this dissociation mechanism.

Dynamic stark control of torsional motion by a pair of laser pulses.

The torsional motion of a molecule composed of two substituted benzene rings, linked by a single bond, is coherently controlled by a pair of strong (3×10^{13}  W cm^{-2}), nonresonant (800 nm) 200-fs-long laser pulses-both linearly polarized perpendicular to the single-bond axis. If the second pulse is sent at the time when the two benzene rings rotate toward (away from) each other the amplitude of the torsion is strongly enhanced (reduced). The torsional motion persists for more than 150 ps corresponding to approximately 120 torsional oscillations.

Time-dependent restricted-active-space self-consistent-field singles method for many-electron dynamics.

The time-dependent restricted-active-space self-consistent-field singles (TD-RASSCF-S) method is presented for investigating TD many-electron dynamics in atoms and molecules. Adopting the SCF notion from the muticonfigurational TD Hartree-Fock (MCTDHF) method and the RAS scheme (single-orbital excitation concept) from the TD configuration-interaction singles (TDCIS) method, the TD-RASSCF-S method can be regarded as a hybrid of them. We prove that, for closed-shell Ne-electron systems, the TD-RASSCF-S wave function can be fully converged using only Ne/2 + 1 ⩽ M ⩽ Ne spatial orbitals.