Genetic algorithm for the response of arbitrarily twisted nematic liquid crystals to an applied field.

When an external field is applied across a liquid-crystal cell, the twist and tilt distributions cannot be calculated analytically and must be extracted numerically. In the standard approach, the Euler-Lagrange equations are derived from the minimization of the free energy of the system and then solved via finite-difference methods, often implemented in commercial software. These tools iterate from initial solutions that are compatible with the boundary conditions, providing limited to no flexibility for customization. Here we present a genetic algorithm that outputs fast and accurate solutions to the integral form of the equations. In our approach, the evolutionary routine is sequentially applied at each position within the bulk of the cell, thus overcoming the necessity of assuming trial solutions. The full range of twist angles from -90^{∘} to 90^{∘} is considered. In this way, the predictions of our routine strongly support the experimentally observed polarization transformations of light incident on different spatially varying twisted nematic liquid-crystal cells, patterned with different topologies on the two alignment layers.

Full Spatial Characterization of Entangled Structured Photons.

Vector modes are fully polarized modes of light with spatially varying polarization distributions, and they have found widespread use in numerous applications such as microscopy, metrology, optical trapping, nanophotonics, and communications. The entanglement of such modes has attracted significant interest, and it has been shown to have tremendous potential in expanding existing applications and enabling new ones. However, due to the complex spatially varying polarization structure of entangled vector modes (EVMs), a complete entanglement characterization of these modes remains challenging and time consuming. Here, we have used a time-tagging event camera to demonstrate the ability to completely characterize the entanglement of EVMs. Leveraging the camera's capacity to provide independent measurements for each pixel, we simultaneously characterize the entanglement of approximately 2.6×10^{6} modes between a bipartite EVM through measuring only 16 observables in polarization. We reveal that EVMs can naturally generate various polarization-entangled Bell states. This achievement is an important milestone in high-dimensional entanglement characterization of structured light, and it could significantly impact the implementation of related quantum technologies. The potential applications of this technique are extensive, and it could pave the way for advancements in quantum communication, quantum imaging, and other areas where structured entangled photons play a crucial role.

Two-photon interference: the Hong-Ou-Mandel effect.

Nearly 30 years ago, two-photon interference was observed, marking the beginning of a new quantum era. Indeed, two-photon interference has no classical analogue, giving it a distinct advantage for a range of applications. The peculiarities of quantum physics may now be used to our advantage to outperform classical computations, securely communicate information, simulate highly complex physical systems and increase the sensitivity of precise measurements. This separation from classical to quantum physics has motivated physicists to study two-particle interference for both fermionic and bosonic quantum objects. So far, two-particle interference has been observed with massive particles, among others, such as electrons and atoms, in addition to plasmons, demonstrating the extent of this effect to larger and more complex quantum systems. A wide array of novel applications to this quantum effect is to be expected in the future. This review will thus cover the progress and applications of two-photon (two-particle) interference over the last three decades.

Characterization of an underwater channel for quantum communications in the Ottawa River.

We examine the propagation of optical beams possessing different polarization states and spatial modes through the Ottawa River in Canada. A Shack-Hartmann wavefront sensor is used to record the distorted beam's wavefront. The turbulence in the underwater channel is analysed, and associated Zernike coefficients are obtained in real-time. Finally, we explore the feasibility of transmitting polarization states as well as spatial modes through the underwater channel for applications in quantum cryptography.

Interaction-free ghost-imaging of structured objects.

Quantum - or classically correlated - light can be employed in various ways to improve resolution and measurement sensitivity. In an "interaction-free" measurement, a single photon can be used to reveal the presence of an object placed within one arm of an interferometer without being absorbed by it. With a technique known as "ghost-imaging", entangled photon pairs are used for detecting an opaque object with significantly improved signal-to-noise ratio while preventing over-illumination. Here, we integrate these two methods to obtain a new imaging technique which we term "interaction-free ghost-imaging" (IFGI). With this new technique, we reduce photon illumination on the object by up to 26.5% while still maintaining at least the same image quality of conventional ghost-imaging. Alternatively, IFGI can improve image signal-to-noise ratio by 18% when given the same number of interacting photons as in standard ghost-imaging. IFGI is also sensitive to phase and polarisation changes of the photons introduced by a structured object. These advantages make IFGI superior for probing light-sensitive materials and biological tissues.

Quantum cryptography with structured photons through a vortex fiber.

Optical fiber links and networks are integral components within and between cities' communication infrastructures. Implementing quantum cryptographic protocols on either existing or new fiber links will provide information-theoretical security to fiber data transmissions. However, there is a need for ways to increase the channel bandwidth. Using the transverse spatial degree of freedom is one way to transmit more information and increase tolerable error thresholds by extending the common qubit protocols to high-dimensional quantum key distribution (QKD) schemes. Here we use one type of vortex fiber where the transverse spatial modes serves as an additional channel to encode quantum information by structuring the spin and orbital angular momentum of light. In this proof-of-principle experiment, we show that two-dimensional structured photons can be used in such vortex fibers in addition to the common two-dimensional polarization encryption, thereby paving the path to QKD multiplexing schemes.

Quantum cryptography with twisted photons through an outdoor underwater channel.

Quantum communication has been successfully implemented in optical fibres and through free-space. Fibre systems, though capable of fast key and low error rates, are impractical in communicating with destinations without an established fibre link. Free-space quantum channels can overcome such limitations and reach long distances with the advent of satellite-to-ground links. However, turbulence, resulting from local fluctuations in refractive index, becomes a major challenge by adding errors and losses. Recently, an interest in investigating the possibility of underwater quantum channels has arisen. Here, we investigate the effect of turbulence on an underwater quantum channel using twisted photons in outdoor conditions. We study the effect of turbulence on transmitted error rates, and compare different quantum cryptographic protocols in an underwater quantum channel, showing the feasibility of high-dimensional encoding schemes. Our work may open the way for secure high-dimensional quantum communication between submersibles, and provides important input for potential submersibles-to-satellite quantum communication.

Unimolecular reaction energies for polycyclic aromatic hydrocarbon ions.

Imaging photoelectron photoion coincidence spectroscopy was employed to explore the unimolecular dissociation of the ionized polycyclic aromatic hydrocarbons (PAHs) acenaphthylene, fluorene, cyclopenta[d,e,f]phenanthrene, pyrene, perylene, fluoranthene, dibenzo[a,e]pyrene, dibenzo[a,l]pyrene, coronene and corannulene. The primary reaction is always hydrogen atom loss, with the smaller species also exhibiting loss of C2H2 to varying extents. Combined with previous work on smaller PAH ions, trends in the reaction energies (E0) for loss of H from sp2-C and sp3-C centres, along with hydrocarbon molecule loss were found as a function of the number of carbon atoms in the ionized PAHs ranging in size from naphthalene to coronene. In the case of molecules which possessed at least one sp3-C centre, the activation energy for the loss of an H atom from this site was 2.34 eV, with the exception of cyclopenta[d,e,f]phenanthrene (CPP) ions, for which the E0 was 3.44 ± 0.86 eV due to steric constraints. The hydrogen loss from PAH cations and from their H-loss fragments exhibits two trends, depending on the number of unpaired electrons. For the loss of the first hydrogen atom, the energy is consistently ca. 4.40 eV, while the threshold to lose the second hydrogen atom is much lower at ca. 3.16 eV. The only exception was for the dibenzo[a,l]pyrene cation, which has a unique structure due to steric constraints, resulting in a low H loss reaction energy of 2.85 eV. If C2H2 is lost directly from the precursor cation, the energy required for this dissociation is 4.16 eV. No other fragmentation channels were observed over a large enough sample set for trends to be extrapolated, though data on CH3 and C4H2 loss obtained in previous studies is included for completeness. The dissociation reactions were also studied by collision induced dissociation after ionization by atmospheric pressure chemical ionization. When modeled with a simple temperature-based theory for the post-collision internal energy distribution, there was reasonable agreement between the two sets of data.

Nondestructive Measurement of Orbital Angular Momentum for an Electron Beam.

Free electrons with a helical phase front, referred to as "twisted" electrons, possess an orbital angular momentum (OAM) and, hence, a quantized magnetic dipole moment along their propagation direction. This intrinsic magnetic moment can be used to probe material properties. Twisted electrons thus have numerous potential applications in materials science. Measuring this quantity often relies on a series of projective measurements that subsequently change the OAM carried by the electrons. In this Letter, we propose a nondestructive way of measuring an electron beam's OAM through the interaction of this associated magnetic dipole with a conductive loop. Such an interaction results in the generation of induced currents within the loop, which are found to be directly proportional to the electron's OAM value. Moreover, the electron experiences no OAM variations and only minimal energy losses upon the measurement, and, hence, the nondestructive nature of the proposed technique.

Dissociative photoionization and threshold photoelectron spectra of polycyclic aromatic hydrocarbon fragments: an imaging photoelectron photoion coincidence (iPEPICO) study of four substituted benzene radical cations.

Four molecules were investigated by imaging photoelectron photoion coincidence (iPEPICO) spectroscopy: 1-propynylbenzene, indene, ethynylbenzene, and benzocyclobutene. Their threshold photoelectron spectrum was obtained and electronic transitions were assigned by OVGF (outer valence Green's function) calculations. Vibrational progressions observed in the electronic ground and excited states were simulated by calculating Franck-Condon factors based on the neutral as well as the cation ground and excited state geometries. iPEPICO was used to obtain ion dissociation data in threshold photoionization as a function of photon energy, which were modeled with RRKM theory to extract kinetic parameters for the reactions C9H8(+•) (1-propynylbezene) → C9H7(+) + H (R1); C9H8(+•) (indene) → C9H7(+) + H (R2); C8H8(+•) (benzocyclobutene) → C8H7(+) + H (R3); C8H8(+•) (benzocyclobutene) → C6H6(+) + C2H2 (R4); C8H6(+•) (1-ethynylbenzene, aka phenylacetylene) → C6H4(+) + C2H2 (R5). These results were compared to G3 level calculations. In addition, the enthalpy of formation of the indenyl radical was estimated to be ΔfH°0K = 249 ± 50 kJ mol(-1) based on a previously measured IE and a cation ΔfH°0K = 976 kJ mol(-1), determined herein.

Dissociation of the anthracene radical cation: a comparative look at iPEPICO and collision-induced dissociation mass spectrometry results.

The dissociation of the anthracene radical cation has been studied using two different methods: imaging photoelectron photoion coincidence spectrometry (iPEPCO) and atmospheric pressure chemical ionization-collision induced dissociation mass spectrometry (APCI-CID). Four reactions were investigated: (R1) C14H10(+•) → C14H9(+) + H, (R2) C14H9(+) → C14H8(+•) + H, (R3) C14H10(+•) → C12H8(+•) + C2H2 and (R4) C14H10(+•) → C10H8(+•) + C4H2. An attempt was made to assign structures to each fragment ion, and although there is still room for debate whether for the C12H8(+•) fragment ion is a cyclobuta[b]naphthalene or a biphenylene cation, our modeling results and calculations appear to suggest the more likely structure is cyclobuta[b]naphthalene. The results from the iPEPICO fitting of the dissociation of ionized anthracene are E0 = 4.28 ± 0.30 eV (R1), 2.71 ± 0.20 eV (R2), and 4.20 ± 0.30 eV (average of reaction R3) whereas the Δ(‡)S values (in J K(-1) mol(-1)) are 12 ± 15 (R1), 0 ± 15 (R2), and either 7 ± 10 (using cyclobuta[b]naphthalene ion fragment in reaction R3) or 22 ± 10 (using the biphenylene ion fragment in reaction R3). Modeling of the APCI-CID breakdown diagrams required an estimate of the postcollision internal energy distribution, which was arbitrarily assumed to correspond to a Boltzmann distribution in this study. One goal of this work was to determine if this assumption yields satisfactory energetics in agreement with the more constrained and theoretically vetted iPEPICO results. In the end, it did, with the APCI-CID results being similar.