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The realization of on-chip quantum interfaces between flying photons and solid-state spins is a key building block for quantum-information processors, enabling, e.g., distributed quantum computing, where remote quantum registers are interconnected by flying photons. Self-assembled quantum dots integrated into nanostructures are one of the most promising systems for such an endeavor thanks to their near-unity photon-emitter coupling and fast spontaneous emission rate. Here we demonstrate high-fidelity on-chip entanglement between an incoming photon and a stationary quantum-dot hole spin qubit. The entanglement is induced by sequential scattering of the time-bin encoded photon interleaved with active spin control within a microsecond, two orders of magnitude faster than those achieved in other solid-state platforms. Conditioning on the detection of a reflected photon renders the entanglement fidelity immune to the spectral wandering of the emitter. These results represent a major step towards realizing a quantum node capable of interchanging information with flying photons and on-chip quantum logic, as required for quantum networks and quantum repeaters.

The development of multireference coupled cluster (MRCC) techniques has remained an open area of study in electronic structure theory for decades due to the inherent complexity of expressing a multi-configurational wavefunction in the fundamentally single-reference coupled cluster framework. The recently developed multireference coupled cluster Monte Carlo (mrCCMC) technique uses the formal simplicity of the Monte Carlo approach to Hilbert space quantum chemistry to avoid some of the complexities of conventional MRCC, but there is room for improvement in terms of accuracy and, particularly, computational cost. In this paper we explore the potential of incorporating ideas from conventional MRCC - namely the treatment of the strongly correlated space in a configuration interaction formalism - to the mrCCMC framework, leading to a series of methods with increasing relaxation of the reference space in the presence of external amplitudes. These techniques offer new balances of stability and cost against accuracy, as well as a means to better explore and better understand the structure of solutions to the mrCCMC equations., Comment: 13 pages, 10 figures, 3 tables

A spectroscopic study of atomic oxygen (O i) is performed using the Fourier-transform vacuum ultraviolet (VUV) spectrometer at the Dichroïsme Et Spectroscopie par Interaction avec le Rayonnement Synchrotron beamline of the SOLEIL synchrotron. Transition frequencies of O i lines in the range between 76,000 and 151,000 cm−1, corresponding to wavelengths between 665 and 1306 Å, are presented. In the wavelength window a data set of 208 lines is obtained for which line centers were determined at an accuracy of ≤0.035 cm−1, verified through a comparison with previous VUV-laser spectroscopy at an accuracy of 0.008 cm−1. Transitions to upper states belonging to several ns and nd Rydberg series that converge to the 4S3/2, 2D, and 2P ionization limits are presented. Besides studies on the main 16O isotope, measurements of the 18O isotope are also performed, for which an enriched sample of 18O2 gas is used. A least-squares optimization analysis is performed after merging the present new data set with some relevant accurate literature data to extract a list of level energies at high accuracy. When comparing with the database of the National Institute of Standards and Technology, good agreement is found for levels with low principal quantum numbers n ≤ 7 or below excitation energies of 108,000 cm−1; however, significant deviations were found for levels with n > 7. The main result of the present study is the realization of an improved data set of transition frequencies and level energies for O i, with its usefulness demonstrated in a comparison with high-resolution astronomical spectra showing absorption in the line of sight to distant quasars.

The “quasi-constant” smooth overlap of atomic position and atom-centered symmetry function fingerprint manifolds recently discovered by Parsaeifard and Goedecker [J. Chem. Phys. 156, 034302 (2022)] are closely related to the degenerate pairs of configurations, which are known shortcomings of all low-body-order atom-density correlation representations of molecular structures. Configurations that are rigorously singular—which we demonstrate can only occur in finite, discrete sets and not as a continuous manifold—determine the complete failure of machine-learning models built on this class of descriptors. The “quasi-constant” manifolds, on the other hand, exhibit low but non-zero sensitivity to atomic displacements. As a consequence, for any such manifold, it is possible to optimize model parameters and the training set to mitigate their impact on learning even though this is often impractical and it is preferable to use descriptors that avoid both exact singularities and the associated numerical instability.

The stochastic wave function method is proposed to study the diffusion regimes of alkali atoms on metallic surfaces. The Lindblad approach, based on the microscopic Hamiltonian information in the Caldeira-Leggett model, is presented and numerical calculations of the dynamics are carried out to characterize surface diffusion for two different systems: Na-Cu(111) and Li-Cu(111). Calculations of the intermediate scattering function for an isolated adsorbate are compared, in the Brownian limit, with results deduced from helium spin-echo (HeSE) experiments after reducing them to single adsorbate dynamics. To illustrate the method we present the dependence on momentum transfer and the temperature dependency. Results show that the experiment can be described at a quantitative level by the 1-D quantum model (reduced dimensionality).

Detecting small changes in spectral fingerprints at multiple wavelength bands simultaneously is challenging for many spectroscopic techniques. Because power variations, drift, and thermal fluctuations can affect such measurements on different timescales, high speed lock-in detection is the preferred method, however this is typically a single channel (wavelength) technique. Here, a way to achieve multichannel (multi-wavelength) lock-in vibrational spectroscopy is reported, using acousto-optic modulators to convert nanosecond periodic temporal perturbations into spatially distinct spectra. This simultaneously resolves perturbed and reference spectra, by projecting them onto different locations of the spectrometer image. As an example, we apply this multichannel time-resolved methodology to detect molecular frequency upconversion in plasmonic nanocavities from the perturbed Raman scattering at different wavelengths. Our phase-sensitive detection scheme can be applied to any spectroscopy throughout the visible and near-infrared wavelength ranges. Extracting perturbed spectra for measurements on nanosecond timescales allows for capturing many processes, such as semiconductor optoelectronics, high-speed spectro-electrochemistry, catalysis, redox chemistry, molecular electronics, or atomic diffusion across materials.

Oblique plane microscopy, OPM, is a form of lightsheet microscopy that permits volumetric imaging of biological samples at high temporal and spatial resolution. However, the imaging geometry of OPM, and related variants of light sheet microscopy, distorts the coordinate frame of the presented image sections with respect to the real space coordinate frame in which the sample is moved. This makes live viewing and practical operation of such microscopes difficult. We present an open-source software package that utilises GPU acceleration and multiprocessing to transform the display of OPM imaging data in real time to produce a live extended depth of field projection. Image stacks can be acquired, processed and plotted at rates of several Hz, making live operation of OPMs, and similar microscopes, more user friendly and intuitive.

We present a number of solutions to the three-dimensional Gross--Pitaevskii equation describing atomic Bose-Einstein condensates. This model supports elaborate patterns, including excited states bearing vorticity. The coherent structures exhibit striking topological features, involving combinations of vortex rings and multiple, possibly bent vortex lines. Although unstable, many of them persist for long times in dynamical simulations. These solutions were identified by a state-of-the-art numerical technique called deflation, which is expected to be applicable to many problems from other areas of physics.

—To analyse and evaluate the physical layer performance of a UK national quantum network (UKQNtel) utilising COW-QKD, in O band, integrated with 500 Gb/s encrypted data, in C band, over 121 km between BT Labs and the University of Cambridge, a theoretical model encompassing COW-QKD and Raman scattering noise is developed and fitted with real-world experimental data. Different physical mechanisms underpinning the link performance are identified and discussed. The model developed in this work also provides a preliminary technical guidance for future UKQNtel upgrade and expansion, as well as potentially useful insights for quantum-secured networks design prior to practical deployment.

Acknowledgements: The authors thank Prof. A. Aurisano for the provision of computing resources at the University of Cincinnati, Dr S. Alonso Monsalve for his helpful comments on the manuscript, and Dr A. Basharina-Freshville for her work on a previous incarnation of the detector simulation., Training deep neural networks using simulations typically requires very large numbers of simulated events. This can be a large computational burden and a limitation in the performance of the deep learning algorithm when insufficient numbers of events can be produced. We investigate the use of transfer learning, where a set of simulated images are used to fine tune a model trained on generic image recognition tasks, to the specific use case of neutrino interaction classification in a liquid argon time projection chamber. A ResNet18, pre-trained on photographic images, was fine-tuned using simulated neutrino images and when trained with one hundred thousand training events reached an F1 score of 0.896$$\,\pm \,$$ ± 0.002 compared to 0.836$$\,\pm \,$$ ± 0.004 from a randomly-initialised network trained with the same training sample. The transfer-learned networks also demonstrate lower bias as a function of energy and more balanced performance across different interaction types.

We summarise the discussions at a virtual Community Workshop on Cold Atoms in Space concerning the status of cold atom technologies, the prospective scientific and societal opportunities offered by their deployment in space, and the developments needed before cold atoms could be operated in space. The cold atom technologies discussed include atomic clocks, quantum gravimeters and accelerometers, and atom interferometers. Prospective applications include metrology, geodesy and measurement of terrestrial mass change due to, e.g., climate change, and fundamental science experiments such as tests of the equivalence principle, searches for dark matter, measurements of gravitational waves and tests of quantum mechanics. We review the current status of cold atom technologies and outline the requirements for their space qualification, including the development paths and the corresponding technical milestones, and identifying possible pathfinder missions to pave the way for missions to exploit the full potential of cold atoms in space. Finally, we present a first draft of a possible road-map for achieving these goals, that we propose for discussion by the interested cold atom, Earth Observation, fundamental physics and other prospective scientific user communities, together with the European Space Agency (ESA) and national space and research funding agencies.

We realise a turbulent cascade of wave excitations in a homogeneous 2D Bose gas, and probe on all relevant time and length scales how it builds up from small to large momenta, until the system reaches a steady state with matching energy injection and dissipation. This all-scales view directly reveals the two theoretically expected cornerstones of turbulence formation -- the emergence of statistical momentum-space isotropy under anisotropic forcing, and the spatiotemporal scaling of the momentum distribution at times before any energy is dissipated.

In understanding the nature of contrast in the emerging field of neutral helium microscopy, it is important to identify if there is an atom-surface scattering distribution that can be expected to apply broadly across a range of sample surfaces. Here we present results acquired in a scanning helium microscope (SHeM) under typical operating conditions, from a range of surfaces in their native state, i.e. without any specialist sample preparation. We observe diffuse scattering, with an approximately cosine distribution centred about the surface normal. The 'cosine-like' distribution is markedly different from those distributions observed from the well-prepared, atomically pristine, surfaces typically studied in helium atom scattering experiments. Knowledge of the typical scattering distribution in SHeM experiments provides a starting basis for interpretation of topographic contrast in images, as well as a reference against which more exotic contrast mechanisms can be compared.

Using a combination of bound-state spectroscopy and loss spectroscopy, we pinpoint eight intrastate Feshbach resonances in $^{39}$K, as well as six previously unexplored interstate ones. We also perform a detailed characterization of four of the intrastate resonances and two of the interstate ones. We carry out coupled-channel scattering calculations and find good agreement with experiment. The combination of experiment and theory provides a faithful map of the scattering length $a$ and permits precision measurements of the signatures of Efimov physics across four intermediate-strength resonances. We measure the modulation of the $a^4$ scaling of the three-body loss coefficient for both $a0$, as well as the many-body loss dynamics at unitarity (where $a$ diverges). The absolute positions of the observed Efimov features confirm a ubiquitous breakdown of Efimov--van-der-Waals universality in $^{39}$K, while their relative positions are in agreement with the universal Efimov ratios. The loss dynamics at the three broadest Feshbach resonances are universal within experimental uncertainties, consistent with observing little variation in the Efimov width parameters., 12 pages, 7 figures (including appendices)

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement, We demonstrate resonant excitation of quantum emitters in gallium nitride (GaN). The emitters are stable under non-resonant excitation and exhibit nearly Fourier-transform-limited lines of ∼250 MHz under coherent excitation, the narrowest reported to date for GaN.

We present a classical induction model to evaluate the three-body ion–water–water (I–W–W) and water–water–water (W–W–W) interactions in aqueous ionic systems. The classical description of the induction energy is based on electrostatic distributed multipoles up to hexadecapole and distributed polarizabilities up to quadrupole–quadrupole on the O and H atoms of water. The monatomic ions were described by a point charge and a dipole–dipole polarizability, while for the polyatomic ions, distributed multipoles up to hexadecapole and distributed polarizabilities up to quadrupole–quadrupole were used. The accuracy of the classical model is benchmarked against an accurate dataset of 936 (I–W–W) and 2184 (W–W–W) three-body terms for 13 different monatomic and polyatomic cation and anion systems. The classical model shows excellent agreement with the reference second order Moller–Plesset and coupled-cluster single double and perturbative triple [CCSD(T)] three-body energies. The Root-Mean-Square-Errors (RMSEs) for monatomic cations, monatomic anions, and polyatomic ions were 0.29, 0.25, and 0.12 kcal/mol, respectively. The corresponding RMSE for 1744 CCSD(T)/aVTZ three-body (W–W–W) energies, used to train MB-pol, was 0.12 kcal/mol. The accuracy of the proposed classical model demonstrates that the three-body term for aqueous ionic systems can be accurately modeled classically. This approach provides a fast, efficient, and as-accurate path toward modeling the three-body term in aqueous ionic systems that is fully transferable across systems with different ions without the need to fit to tens of thousands of ab initio calculations for each ion to extend existing many-body force fields to interactions between water and ions.

PAINT methods that use DNA- or protein- based exchangeable probes have become popular for super-resolution imaging and have been combined with spinning disk confocal microscopy for imaging thicker samples. However, the widely available spinning disks used for routine biological imaging are not optimized for PAINT-based applications and may compromise resolution and imaging speed. Here, we use Drosophila egg chambers in the presence of the actin-binding peptide Lifeact to study the performance of four different spinning disk geometries. We find that disk geometries with higher light collection efficiency perform better for PAINT-based super-resolution imaging due to increased photon numbers and, subsequently, detection of more blinking events.

Certain quantum devices, such as half-wave plates and quarter-wave plates in quantum optics, are bidirectional, meaning that the roles of their input and output ports can be exchanged. Bidirectional devices can be used in a forward mode and a backward mode, corresponding to two opposite choices of the input-output direction. They can also be used in a coherent superposition of the forward and backward modes, giving rise to new operations with indefinite input-output direction. In this work we explore the potential of input-output indefiniteness for the transfer of classical and quantum information through noisy channels. We first formulate a model of communication from a sender to a receiver via a noisy channel used in indefinite input-output direction. Then, we show that indefiniteness of the input-output direction yields advantages over standard communication protocols in which the given noisy channel is used in a fixed input-output direction. These advantages range from a general reduction of noise in bidirectional processes, to heralded noiseless transmission of quantum states, and, in some special cases, to a complete noise removal. The noise reduction due to input-output indefiniteness can be experimentally demonstrated with current photonic technologies, providing a way to investigate the operational consequences of exotic scenarios characterised by coherent quantum superpositions of forward-time and backward-time processes., Comment: 13 + 8 pages, 4 figures

Understanding and classifying nonequilibrium many-body phenomena, analogous to the classification of equilibrium states of matter into universality classes, is an outstanding problem in physics. Any many-body system, from stellar matter to financial markets, can be out of equilibrium in a myriad of ways; since many are also difficult to experiment on, it is a major goal to establish universal principles that apply to different phenomena and physical systems. At the heart of the classification of equilibrium states is the universality seen in the self-similar spatial scaling of systems close to phase transitions. Recent theoretical work, and first experimental evidence, suggest that isolated many-body systems far from equilibrium generically exhibit dynamic (spatiotemporal) self-similar scaling, akin to turbulent cascades and the Family-Vicsek scaling in classical surface growth. Here we observe bidirectional dynamic scaling in an isolated quench-cooled atomic Bose gas; as the gas thermalises and undergoes Bose-Einstein condensation, it shows self-similar net flows of particles towards the infrared (smaller momenta) and energy towards the ultraviolet (smaller lengthscales). For both infrared (IR) and ultraviolet (UV) dynamics we find that the scaling exponents are independent of the strength of the interparticle interactions that drive the thermalisation., 5 pages, 4 figures

The interaction of highly reactive species with solid surfaces can result in modes of adsorption quite distinct from the classic molecular and dissociative events that are usually thought to dominate. For instance, compelling experimental evidence suggests that adsorption of F2 at the Si{001} surface is often initiated by abstraction (and binding at the surface) of just one fluorine atom from the molecule; the second fluorine atom subsequently experiences either a separate atomic adsorption event or ejection from the surface altogether. Molecular dynamics simulations using empirical potentials support this concept but massively overestimate the prevalence of atomic ejection. In this work, we report first-principles molecular dynamics calculations that correctly show atomic ejection to be rare while providing insight into the details of abstractive adsorption. In addition, we also examine the case of F2 adsorption onto a monohydrogenated Si{001} surface, finding evidence for a different type of abstractive adsorption, in which a hydrogen atom may be removed from the surface to form a short-lived HFF intermediate. The latter rapidly decomposes to produce either HF or (via reaction with another surface hydrogen atom) H2.

Large-scale bulk peculiar motions introduce a characteristic length scale, inside which the local kinematics are dominated by peculiar-velocity perturbations rather than by the background Hubble expansion. Regions smaller than the aforementioned critical length, which typically varies between few hundred and several hundred Mpc, can be heavily "contaminated" by the observers' relative motion. For example, at the critical length -- hereafter referred to as the "transition scale", the sign of the locally measured deceleration parameter can change from positive to negative, while the surrounding universe is still decelerating globally. Overall, distant observers can assign very different values to their local deceleration parameters, entirely because of their relative motion. In practice, this suggests that information selected from regions inside and close to the transition scale hold only locally and they should not be readily extrapolated to the global universe. We show that this principle applies to essentially all Friedmann backgrounds, irrespective of their equation of state and spatial curvature. Put another way, the transition scale and the related effects are generic to linear peculiar-velocity perturbations. This study generalises previous work applied, primarily for reasons of mathematical simplicity, to a perturbed Einstein-de Sitter universe., Minor revision, references added. To appear in EPJC

The proliferation of Internet-of-Things has promoted a wide variety of emerging applications that require compact, lightweight, and low-cost optical spectrometers. While substantial progresses have been made in the miniaturization of spectrometers, most of them are with a major focus on the technical side but tend to feature a lower technology readiness level for manufacturability. More importantly, in spite of the advancement in miniaturized spectrometers, their performance and the metrics of real-life applications have seldomly been connected but are highly important. This review paper shows the market trend for chip-scale spectrometers and analyzes the key metrics that are required to adopt miniaturized spectrometers in real-life applications. Recent progress addressing the challenges of miniaturization of spectrometers is summarized, paying a special attention to the CMOS-compatible fabrication platform that shows a clear pathway to massive production. Insights for ways forward are also presented., National Key R&D Program of China (Grant no. 2021YFB2801500), National Natural Science Foundation of China (Grant no. 62105149), Natural Science Foundation of Jiangsu Province (Grant no. BK20210288), Fast Support Program (grant No. 80914010402) and Shuang Chuang Program of Jiangsu Province.

Funder: U.S. National Science Foundation CAREER grant no. DMR-1350237, Funder: RCUK | Engineering and Physical Sciences Research Council (EPSRC); doi: https://doi.org/10.13039/501100000266, Funder: Royal Society; doi: https://doi.org/10.13039/501100000288, Funder: CIFAR as a Fellow of the CIFAR Quantum Materials Research Program, Intermetallic compounds containing f-electron elements have been prototypical materials for investigating strong electron correlations and quantum criticality (QC). Their heavy fermion ground state evoked by the magnetic f-electrons is susceptible to the onset of quantum phases, such as magnetism or superconductivity, due to the enhanced effective mass (m*) and a corresponding decrease of the Fermi temperature. However, the presence of f-electron valence fluctuations to a non-magnetic state is regarded an anathema to QC, as it usually generates a paramagnetic Fermi-liquid state with quasiparticles of moderate m*. Such systems are typically isotropic, with a characteristic energy scale T0 of the order of hundreds of kelvins that require large magnetic fields or pressures to promote a valence or magnetic instability. Here we show the discovery of a quantum critical behaviour and a Lifshitz transition under low magnetic field in an intermediate valence compound α-YbAlB4. The QC origin is attributed to the anisotropic hybridization between the conduction and localized f-electrons. These findings suggest a new route to bypass the large valence energy scale in developing the QC.

We study the Einstein-aether theory in Weyl integrable geometry. The scalar field which defines the Weyl affine connection is introduced in the gravitational field equation. We end up with an Einstein-aether scalar field model where the interaction between the scalar field and the aether field has a geometric origin. The scalar field plays a significant role in the evolution of the gravitational field equations. We focus our study on the case of homogeneous and isotropic background spacetimes and study their dynamical evolution for various cosmological models., 14 pages, 8 compound figures

In this article, we demonstrate that a first-order spin penalty scheme can be efficiently applied to the Slater determinant based Full-CI Quantum Monte Carlo (FCIQMC) algorithm, as a practical route toward spin purification. Two crucial applications are presented to demonstrate the validity and robustness of this scheme: the 1Δg ← 3Σg vertical excitation in O2 and key spin gaps in a [Mn3(IV)O4] cluster. In the absence of a robust spin adaptation/purification technique, both applications would be unattainable by Slater determinant based ground state methods, with any starting wave function collapsing into the higher-spin ground state during the optimization. This strategy can be coupled to other algorithms that use the Slater determinant based FCIQMC algorithm as configuration interaction eigensolver, including the Stochastic Generalized Active Space, the similarity-transformed FCIQMC, the tailored-CC, and second-order perturbation theory approaches. Moreover, in contrast to the GUGA-FCIQMC technique, this strategy features both spin projection and total spin adaptation, making it appealing when solving anisotropic Hamiltonians. It also provides spin-resolved reduced density matrices, important for the investigation of spin-dependent properties in polynuclear transition metal clusters, such as the hyperfine-coupling constants.

We theoretically prove the security of using classical m-psk modulation protocol for the transmission of continuous-variable quantum key distribution and discuss the performance of classical digital communication protocols for CVQKD

Quasi-particles are elementary excitations of condensed matter quantum phases. Demonstrating that they keep quantum coherence while propagating is a fundamental issue for their manipulation for quantum information tasks. Here, we consider anyons, the fractionally charged quasi-particles 20 of the Fractional Quantum Hall Effect occurring in two-dimensional electronic conductors in high magnetic fields. They obey anyonic statistics, intermediate between fermionic and bosonic. Surprisingly, anyons show large quantum coherence when transmitted through the localized states of electronic Fabry-P\'erot interferometers, but almost no quantum interference when transmitted via the propagating states of Mach-Zehnder interferometers. Here, using a novel interferometric 25 approach, we demonstrate that anyons do keep quantum coherence while propagating. Performing two-particle time-domain interference measurements sensitive to the two-particle Hanbury Brown Twiss phase, we find 53% and 60% visibilities for anyons with charges e/5 and e/3. Our results give a positive message for the challenge of performing controlled quantum coherent braiding of anyons., Comment: Main text and supplementary materials, 24 pages, 11 figures

Funder: Engineering and Physical Sciences Research Council; doi: https://doi.org/10.13039/501100000266, Recently published density functional theory results using the PBE functional (Whaley-Baldwin and Needs 2020 New J. Phys. 22 023020) suggest that elemental sulfur does not adopt the simple-cubic (SC) P m 3 ̄ m phase at high pressures, in disagreement with previous works (Rudin and Liu 1999 Phys. Rev. Lett. 83 3049--52; Gavryushkin et al 2017 Phys. Status Solidi B 254 1600857). We carry out an extensive set of calculations using a variety of different exchange–correlation functionals (both local and non-local), and show that even though under LDA and PW91 a high-pressure SC phase does indeed become favourable at the static lattice level, when zero-point energies (ZPEs) are included, the transition to the SC phase is suppressed in every case, owing to the larger ZPE of the SC phase; thus confirming the transition sequence as R 3 ̄ m → BCC, with no intervening SC phase. We reproduce these findings with pseudopotentials that explicitly include core electronic states, and show that even at these high pressures, only the n = 3 valence shell contributes to bonding in sulfur. We then compare our findings against the all-electron code ELK, which is in excellent agreement with our pseudopotential results, and examine the roles of the exchange and correlation contributions to the total energy. We further calculate anharmonic vibrational corrections to the ZPEs of the two phases, and find that such corrections are several orders of magnitude smaller than the ZPEs and are thus negligible. The effect of finite temperatures is also considered, and we show that the P m 3 ̄ m phase becomes even more unfavourable with an increase in temperature. Finally, the experimental consequences of our results on the equation of state of sulfur and its superconducting critical temperature are explicitly calculated.

Calculations of molecular spectral properties, like photodissociation rates and absorption bands, rely on knowledge of the excited state energies of the molecule of interest. Protocols based on the variational quantum eigensolver (VQE) are promising candidates to calculate such energies on emerging noisy intermediate-scale quantum (NISQ) computers. The successful implementation of these protocols on NISQ computers, relies on ansätze that can accurately approximate the molecular states and that can be implemented by shallow quantum circuits. We introduce the excited qubit-excitation-based adaptive (e-QEB-ADAPT)-VQE protocol to calculate molecular-excited-state energies. The e-QEB-ADAPT-VQE constructs efficient problem-tailored ansätze by iteratively appending evolutions of qubit excitation operators. The e-QEB-ADAPT-VQE also improves on previous ADAPT-VQE protocol in that it is designed to be independent on the choice of initial reference state. We perform classical numerical simulations for LiH and BeH2 to benchmark the performance of the e-QEB-ADAPT-VQE. We demonstrate that the e-QEB-ADAPT-VQE can construct highly accurate ansätze that require at least an order of magnitude fewer cnot gates than standard fixed unitary coupled-cluster ansätze, such as the UCCSD and the GUCCSD. We also show that the e-QEB-ADAPT-VQE is more successful in constructing ansätze for excited molecular states than other ADAPT-VQE protocols.

Singlet fission is a photo-physical process that generates two triplet excitons from one singlet exciton and can potentially enhance efficiency in photovoltaic systems. The combination of photovoltaics and singlet fission is a novel field for solar energy conversion when there is much interest in renewable, non-destructive, and continuously available energy sources. Singlet fission can also overcome thermalization losses in photovoltaics, which happens in traditional cells when the incident photon energy is higher than the silicon bandgap energy, using a carrier multiplication mechanism. This thesis will design, construct, and characterize photovoltaic devices incorporating singlet fission materials to study singlet fission in practical application. The research focuses on materials characterization, spin dynamics, and electron transfers between acene and the semiconductor layer in Au/TiO2 ballistic cells, and the incorporation of singlet fission layers on silicon-based cell structures. In detail, a set of investigations was developed and summarized by implementing singlet fission materials into a state-of-the-art ballistic photovoltaic device and silicon-based solar cell. The studies demonstrate proof of concept and rationally explain the process. The first part of the thesis investigates thin films of pentacene, TIPS-pentacene, and tetracene via crystallinity, morphology, absorption, and thickness characterization. Additionally, Au and TiO2 layers in Schottky device structures were optimized to achieve the best performance for energy transfer from an applied dye layer (merbromin). The drop-casted dye layer influences the device performance by increasing short-circuit current and open-circuit voltage, demonstrating the ability of charge transfer between the device and the applied film. This device structure provides a test bed for studying charge and energy transfer from singlet fission films. The latter part of the thesis describes several investigations to understand singlet fission in a thin film using this architecture. Magneto-photoconductivity measurements were primarily used to observe the spin dynamics via photoconductivity under an external magnetic field. Control experiments with bare Au/TiO2 devices showed no observable magneto-photoconductivity signal. In contrast, devices with pentacene and tetracene singlet fission layers showed a strong magnetoconductivity effect caused by ballistic electron transfer from the singlet fission layer into the TiO2 n-type semiconductor through an ultra-thin gold layer inserted between the layers. A qualitatively different behavior is seen between the pentacene and tetracene, which reveals that the energy alignment plays a crucial part in the charge transfer between the singlet fission layer and the device. The last section investigates the application of pentacene and tetracene evaporated thin-films as sensitizer layers to a silicon-based solar cell. The optimized Si cell structure with the annealing treatment improved the cell's performance by increasing short-circuit current and open-circuit voltage. The deposition of pentacene and tetracene as sensitizer layers into the device showed some results but posed several challenges that need to be addressed. As the current-voltage and external quantum efficiency measurements were taken, it was observed that material interfaces need to be designed to fully achieve the singlet fission of the acene layer into the Si devices.

Several theories of modern physics go beyond the standard model of particle physics to describe as of yet unexplained phenomena of the universe. A common method of testing new theories of physics is using spectroscopy to compare transition positions at different times. Non-trivial calculations are required to determine the sensitivity coefficients of transitions to a variation of fundamental constants. These calculations can be done using nuclear motion programs with adequate spectroscopic models. In this work, 27 small molecules with spectroscopic models are evaluated as molecular probes to constrain the variation of the proton-to-electron mass ratio. The diatomic radical CN is used as a case study to develop and explain the construction of spectroscopic models. Over 40,000 experimental transitions from 22 unique sources were validated to generate a network of 8083 interconnected spin-rovibronic energy levels. These empirical energy levels, along with ab initio dipole moment curves have been used to construct and fit a spectroscopic model for the three lowest coupled electronic states of CN in the nuclear motion program Duo. The resultant line list is further refined in a novel hybrid style with the replacement of energy levels from empirical and perturbative sources to produce over 2.2 million transitions up to 60,000 cm-1. A comprehensive high-throughput methodology is developed to calculate the sensitivity coefficients for transitions in CN, 21 other diatomic and 5 small polyatomic molecules of astrophysical relevance. In diatomics, near degenerate vibronic levels and parity transitions within non-singlet-sigma ground states can cause enhanced transition sensitivity. Unfortunately, many of the enhanced transitions, especially those showing anomalously large sensitivities, have extremely low intensities at 100 K. Expanding to polyatomic molecules, tunnelling transitions (a natural progression from parity transitions) show enhanced sensitivity, especially combination rotation-tunnelling transitions. Enhanced transitions are compared against previous calculations, and some previously identified enhanced transitions are excluded from astrophysical consideration based on their very low intensity at 100 K. Selection criteria that consider factors both sensitivity and observability of transitions to be used as molecular probes for a variation in the proton-to-electron mass ratio are considered for both diatomic and polyatomic molecules.

Matsubara dynamics is the classical dynamics which results when imaginary-time path-integrals are smoothed; it conserves the quantum Boltzmann distribution and appears in drastically approximated form in path-integral dynamics methods such as (thermostatted) ring-polymer molecular dynamics (T)RPMD and centroid molecular dynamics (CMD). However, it has never been compared directly with exact quantum dynamics for non-linear operators, because the difficulty of treating the phase has limited the number of Matsubara modes to fewer than 10. Here, we treat up to $\sim$200 Matsubara modes in simulations of a Morse oscillator coupled to a dissipative bath of harmonic oscillators. This is done by expressing the Matsubara equations of motion in the form of a generalised Langevin equation, approximating the noise to be real, and analytically continuing the momenta to convert the Matsubara phase into ring-polymer springs. The resulting equations of motion are stable up to a maximum value of modes which increases with bath coupling strength and decreases with system anharmonicity. The dynamics of the tail of highly oscillatory Matsubara modes is found to be harmonic, and can thus be computed efficiently. For a moderately anharmonic oscillator with a strong but subcritical coupling to the bath, the Matsubara simulations yield non-linear $\large\langle{\hat q^2\hat q^2(t)}\large\rangle$ time-correlation functions in almost perfect agreement with the exact quantum results. Reasonable agreement is also obtained for weaker coupling strengths, where errors arise because of the real-noise approximation. These results give strong evidence that Matsubara dynamics correctly explains how classical dynamics arises in quantum systems which are in thermal equilibrium.

The measurements of quasi-periodic oscillations (QPOs) provide a quite powerful tool to test the nature of astrophysical black hole candidates in the strong gravitational field regime. In this paper, we use QPOs within the relativistic precession model to test a recently proposed family of rotating black hole mimickers, which reduce to the Kerr metric in a limiting case, and can represent traversable wormholes or regular black holes with one or two horizons, depending on the values of the parameters. In particular, assuming that the compact object of GRO J1655-40 is described by a rotating black hole mimicker, we perform a $\chi$-square analysis to fit the parameters of the mimicker with two sets of observed QPO frequencies from GRO J1655-40. Our results indicate that although the metric around the compact object of GRO J1655-40 is consistent with the Kerr metric, a regular black hole with one horizon is favored by the observation data of GRO J1655-40., Comment: v1: 9 pages with 2 figures

Optical networks generate a vast amount of diagnostic, control and performance monitoring data. When information is extracted from this data, reconfigurable network elements and reconfigurable transceivers allow the network to adapt both to changes in the physical infrastructure but also changing traffic conditions. Machine learning is emerging as a disruptive technology for extracting useful information from this raw data to enable enhanced planning, monitoring and dynamic control. We provide a survey of the recent literature and highlight numerous promising avenues for machine learning applied to optical networks, including explainable machine learning, digital twins and approaches in which we embed our knowledge into the machine learning such as physics-informed machine learning for the physical layer and graph-based machine learning for the networking layer.

Single-shot images are the standard readout of experiments with ultracold atoms -- the tarnished looking glass into their many-body physics. The efficient extraction of observables from single-shot images is thus crucial. Here, we demonstrate how artificial neural networks can optimize this extraction. In contrast to standard averaging approaches, machine learning allows both one- and two-particle densities to be accurately obtained from a drastically reduced number of single-shot images. Quantum fluctuations and correlations are directly harnessed to obtain physical observables for bosons in a tilted double-well potential at an unprecedented accuracy. Strikingly, machine learning also enables a reliable extraction of momentum-space observables from real-space single-shot images and vice versa. This obviates the need for a reconfiguration of the experimental setup between in-situ and time-of-flight imaging, thus potentially granting an outstanding reduction in resources., 7+8 pages, 3+8 figures, software available at http://ultracold.org

This work exploits deep learning to develop real-time hologram generation. We propose an original concept of introducing hologram modulators to allow the use of generative models to interpret complex-valued frequency data directly. This new mechanism enables the pre-trained learning model to generate frequency samples with variations in the underlying generative features. To achieve an object-based hologram generation, we also develop a new generative model, named the channeled variational autoencoder (CVAE). The pre-trained CVAE can then interpret and learn the hidden structure of input holograms. It is thus able to generate holograms through the learning of the disentangled latent representations, which can allow us to specify each disentangled feature for a specific object. Additionally, we propose a new technique called hologram super-resolution (HSR) to super-resolve a low-resolution hologram input to a super-resolution hologram output. Combining the proposed CVAE and HSR, we successfully develop a new approach to generate super-resolved, complex-amplitude holograms for 3D scenes.

Classical molecular dynamics (MD) and imaginary-time path-integral dynamics methods underestimate the infrared absorption intensities of overtone and combination bands by typically an order of magnitude. Ple et al. [J. Chem. Phys. 155, 104108 (2021)] have shown that this is because such methods fail to describe the coupling of the centroid to the Matsubara dynamics of the fluctuation modes; classical first-order perturbation theory (PT) applied to the Matsubara dynamics is sufficient to recover most of the lost intensity in simple models and gives identical results to quantum (Rayleigh–Schrodinger) PT. Here, we show numerically that the results of this analysis can be used as post-processing correction factors, which can be applied to realistic (classical MD or path-integral dynamics) simulations of infrared spectra. We find that the correction factors recover most of the lost intensity in the overtone and combination bands of gas-phase water and ammonia and much of it for liquid water. We then re-derive and confirm the earlier PT analysis by applying canonical PT to Matsubara dynamics, which has the advantage of avoiding secular terms and gives a simple picture of the perturbed Matsubara dynamics in terms of action-angle variables. Collectively, these variables “Matsubara heat” the amplitudes of the overtone and combination vibrations of the centroid to what they would be in a classical system with the oscillators (of frequency Ωi) held at their quantum effective temperatures [of ℏΩi coth(βℏΩi/2)/2kB]. Numerical calculations show that a similar neglect of “Matsubara heating” causes path-integral methods to underestimate Fermi resonance splittings.

Typical observers in the universe do not follow the smooth Hubble expansion, but move relative to it. Such bulk peculiar motions introduce a characteristic scale that is closely analogous to the familiar Jeans length. This "peculiar Jeans length" marks the threshold below which relative-motion effects dominate the linear kinematics. There, cosmological measurements can vary considerably between the bulk-flow frame and that of the Hubble expansion, entirely due to the observers' relative motion. When dealing with the deceleration parameter, we find that the peculiar Jeans length varies between few and several hundred Mpc. On these scales, the deceleration parameter measured by the bulk-flow observers can be considerably larger (or smaller) than its Hubble-frame counterpart. This depends on whether the peculiar motion is locally expanding (or contracting), relative to the background expansion. Then, provided expanding and contracting bulk flows are randomly distributed, nearly half of the observers in the universe could be misled to think that their cosmos is over-decelerated. The rest of them, on the other hand, may come to believe that their universe is under-decelerated, or even accelerated in some cases. We make two phenomenological predictions that could in principle support this scenario., Comment: Revised and extended version. References added. Matches published manuscript

Advancing our understanding of non-equilibrium phenomena in quantum many-body systems remains among the greatest challenges in physics. Here, we report on the experimental observation of a paradigmatic many-body problem, namely the non-equilibrium dynamics of a quantum impurity immersed in a bosonic environment. We use an interferometric technique to prepare coherent superposition states of atoms in a Bose-Einstein condensate with a small impurity-state component, and monitor the evolution of such quantum superpositions into polaronic quasiparticles. These results offer a systematic picture of polaron formation from weak to strong impurity interactions. They reveal three distinct regimes of evolution with dynamical transitions that provide a link between few-body processes and many-body dynamics. Our measurements reveal universal dynamical behavior in interacting many-body systems and demonstrate new pathways to study non-equilibrium quantum phenomena., Comment: 15 pages, 9 figures

Funder: Carl-Zeiss-Stiftung; doi: http://dx.doi.org/10.13039/100007569, Funder: German Scholars Organization e.V., We consider quantum stochastic processes and discuss a level 2.5 large deviation formalism providing an explicit and complete characterisation of fluctuations of time-averaged quantities, in the large-time limit. We analyse two classes of quantum stochastic dynamics, within this framework. The first class consists of the quantum jump trajectories related to photon detection; the second is quantum state diffusion related to homodyne detection. For both processes, we present the level 2.5 functional starting from the corresponding quantum stochastic Schrödinger equation and we discuss connections of these functionals to optimal control theory.

Abstract Imaginary-time path-integral or ‘ring-polymer’ methods have been used to simulate quantum (Boltzmann) statistical properties since the 1980s. This article reviews the more recent extension of such methods to simulate quantum dynamics, summarising the chain of approximations that links practical path-integral methods, such as centroid molecular dynamics (CMD) and ring-polymer molecular dynamics (RPMD), to the exact quantum Kubo time-correlation function. We focus on single-surface Born–Oppenheimer dynamics, using the infrared spectrum of water as an illustrative example, but also survey other recent applications and practical techniques, as well as the limitations of current methods and their scope for future development. Graphic abstract

Data availability: Jupyter and Mathematica Notebooks underlying the results presented in this paper are freely available at the GitHub repository: A. L. Trinh and A. Esposito, “Esposito-Lab/BiochemicalResolution,” Zenodo (2021), retrieved https://doi.org/10.5281/zenodo.4483760. Copyright © The Author(s) 2021. A deeper understanding of spatial resolution has led to innovations in microscopy and the disruption of biomedical research, as with super-resolution microscopy. To foster similar advances in time-resolved and spectral imaging, we have previously introduced the concept of ‘biochemical resolving power’ in fluorescence microscopy. Here, we apply those concepts to investigate how the instrument response function (IRF), sampling conditions, and photon-statistics limit the biochemical resolution of fluorescence lifetime microscopy. Using Fisher information analysis and Monte Carlo simulations, we reveal the complex dependencies between photon-statistics and the IRF, permitting us to quantify resolution limits that have been poorly understood (e.g., the minimum resolvable decay time for a given width of the IRF and photon-statistics) or previously underappreciated (e.g., optimization of the IRF for biochemical detection). With this work, we unravel common misunderstandings on the role of the IRF and provide theoretical insights with significant practical implications on the design and use of time-resolved instrumentation. Cancer Research UK (OncoLive, C54674/A27487); Medical Research Council (MC_UU_12022/1, MC_UU_12022/8).

Discontinuous quantum phase transitions and the associated metastability play central roles in diverse areas of physics ranging from ferromagnetism to false vacuum decay in the early universe. Using strongly-interacting ultracold atoms in an optical lattice, we realize a driven many-body system whose quantum phase transition can be tuned from continuous to discontinuous. Resonant shaking of a one-dimensional optical lattice hybridizes the lowest two Bloch bands, driving a novel transition from a Mott insulator to a $\pi$-superfluid, i.e., a superfluid state with staggered phase order. For weak shaking amplitudes, this transition is discontinuous (first-order) and the system can remain frozen in a metastable state, whereas for strong shaking, it undergoes a continuous transition toward a $\pi$-superfluid. Our observations of this metastability and hysteresis are in good quantitative agreement with numerical simulations and pave the way for exploring the crucial role of quantum fluctuations in discontinuous transitions., Comment: 5 pages, 4 figures + Supplementary

Measurement-device-independent quantum key distribution (MDI-QKD) is a technique for quantum-secured communication that eliminates all detector side-channels, although is currently limited by implementation complexity and low secure key rates. Here, we introduce a simple and compact MDI-QKD system design at gigahertz clock rates with enhanced resilience to laser fluctuations—thus enabling free-running semiconductor laser sources to be employed without spectral or phase feedback. This is achieved using direct laser modulation, carefully exploiting gain-switching and injection-locking laser dynamics to encode phase-modulated time-bin bits. Our design enables secure key rates that improve upon the state of the art by an order of magnitude, up to 8 bps at 54 dB channel loss and 2 kbps in the finite-size regime for 30 dB channel loss. This greatly simplified MDI-QKD system design and proof-of-principle demonstration shows that MDI-QKD is a practical, high-performance solution for future quantum communication networks.

We present an experimental demonstration of the feasibility of the first 20 + Mb/s Gaussian modulated coherent state continuous variable quantum key distribution system with a locally generated local oscillator at the receiver (LLO-CVQKD). To increase the signal repetition rate, and hence the potential secure key rate, we equip our system with high-performance, wideband devices and design the components to support high repetition rate operation. We have successfully trialed the signal repetition rate as high as 500 MHz. To reduce the system complexity and correct for any phase shift during transmission, reference pulses are interleaved with quantum signals at Alice. Customized monitoring software has been developed, allowing all parameters to be controlled in real-time without any physical setup modification. We introduce a system-level noise model analysis at high bandwidth and propose a new ‘combined-optimization’ technique to optimize system parameters simultaneously to high precision. We use the measured excess noise, to predict that the system is capable of realizing a record 26.9 Mb/s key generation in the asymptotic regime over a 15 km signal mode fibre. We further demonstrate the potential for an even faster implementation.

Spatial light modulators (SLMs) are key research tools in several contemporary applied optics research domains. In this paper, we present the argument that an open platform for interacting with SLMs would dramatically increase their accessibility to researchers. We introduce HoloBlade, an open-hardware implementation of an SLM driver-stack, and provide a detailed exposition of HoloBlade’s architecture, key components, and detailed design. An optical verification rig is constructed to demonstrate that HoloBlade can provide Fourier imaging capability in a 4f system. Finally, we discuss HoloBlade’s future development roadmap and the opportunities that it presents as a research tool for applied optics.

Miniaturized ultrafast switchable optical components with an extremely compact size and a high-speed response will be the core of next-generation all-optical devices instead of traditional integrated circuits, which are approaching the bottleneck of Moore’s Law. Metasurfaces have emerged as fascinating subwavelength flat optical components and devices for light focusing and holography applications. However, these devices exhibit a severe limitation due to their natural passive response. Here we introduce an active hybrid metasurface integrated with patterned semiconductor inclusions for all-optical active control of terahertz waves. Ultrafast modulation of polarization states and the beam splitting ratio are experimentally demonstrated on a time scale of 667 ps. This scheme of hybrid metasurfaces could also be extended to the design of various free-space all-optical active devices, such as varifocal planar lenses, switchable vector beam generators, and components for holography in ultrafast imaging, display, and high-fidelity terahertz wireless communication systems., Active metasurfaces: Terahertz control All-optical control and manipulation of terahertz waves is now possible thanks to the development of custom-designed, dynamic reconfigurable metasurfaces. Realized by Longqing Cong and coworkers from Nanyang Technological University in Singapore and Tianjin University in China, the metasurfaces enable ultrafast (sub-nanosecond) polarization switching and beam splitting. They consist of an array of miniature aluminum-coated silicon split-ring resonators on a sapphire substrate. Illumination with short pulses of an infrared “pump beam” causes charge carriers in the silicon patch of the microring to transition from the valence to the conduction band, temporarily changing the photoconductivity and thus switching the transmission of the metasurface between “off” and “on” states for a polarized terahertz wave. Such high-speed switching of polarization is expected to be useful for applications such as data-encoding and multiplexing in a terahertz communications system as well as holography.

Structured illumination microscopy (SIM) has become an important technique for optical super-resolution imaging because it allows a doubling of image resolution at speeds compatible with live-cell imaging. However, the reconstruction of SIM images is often slow, prone to artefacts, and requires multiple parameter adjustments to reflect different hardware or experimental conditions. Here, we introduce a versatile reconstruction method, ML-SIM, which makes use of transfer learning to obtain a parameter-free model that generalises beyond the task of reconstructing data recorded by a specific imaging system for a specific sample type. We demonstrate the generality of the model and the high quality of the obtained reconstructions by application of ML-SIM on raw data obtained for multiple sample types acquired on distinct SIM microscopes. ML-SIM is an end-to-end deep residual neural network that is trained on an auxiliary domain consisting of simulated images, but is transferable to the target task of reconstructing experimental SIM images. By generating the training data to reflect challenging imaging conditions encountered in real systems, ML-SIM becomes robust to noise and irregularities in the illumination patterns of the raw SIM input frames. Since ML-SIM does not require the acquisition of experimental training data, the method can be efficiently adapted to any specific experimental SIM implementation. We compare the reconstruction quality enabled by ML-SIM with current state-of-the-art SIM reconstruction methods and demonstrate advantages in terms of generality and robustness to noise for both simulated and experimental inputs, thus making ML-SIM a useful alternative to traditional methods for challenging imaging conditions. Additionally, reconstruction of a SIM stack is accomplished in less than 200 ms on a modern graphics processing unit, enabling future applications for real-time imaging. Source code and ready-to-use software for the method are available at http://ML-SIM.github.io.

Infrared methods are of great importance in nondestructive testing of artworks, allowing a remote and wide-field imaging of interesting hidden features. Here we discuss a workflow based on thermal imaging in the mid infrared 3-5 micron range for the evaluation of subsurface defects in frescoes. Particular attention is payed to obtaining a high resolution (submillimetric) localization of the defects. The transfer of diagnostics techniques into real world applications, is discussed through the proof of concept of the proposed workflow on frescoes at the Sforza Castle (Milan, Italy).

Stimulated emission depletion (STED) microscopy enables the three-dimensional (3D) visualization of dynamic nanoscale structures in living cells, offering unique insights into their organization. However, 3D-STED imaging deep inside biological tissue is obstructed by optical aberrations and light scattering. We present a STED system that overcomes these challenges. Through the combination of two-photon excitation, adaptive optics, red-emitting organic dyes, and a long-working-distance water-immersion objective lens, our system achieves aberration-corrected 3D super-resolution imaging, which we demonstrate 164 µm deep in fixed mouse brain tissue and 76 µm deep in the brain of a living mouse.