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The average ionization state is a critical parameter in plasma models for charged particle transport, equation of state, and optical response. The dynamical or nonadiabatic Born effective charge (NBEC), calculated via first principles time-dependent density functional theory, provides exact ionic partitioning of bulk electron response for both metallic and insulating materials. The NBEC can be trivially transformed into a ''group conductivity", that is, the electron conductivity ascribed to a subset of ions. We show that for disordered metallic systems, such as warm dense matter (WDM) and hot dense plasma, the static limit of the NBEC is different from the average ionization state, but that the ionization state can be extracted from the group conductivity even in mixed systems. We demonstrate this approach using a set of archetypical examples, including cold and warm aluminium, low- and high- density WDM carbon, and a WDM carbon-beryllium-hydrogen mixture., Comment: 7 pages, 3 figures + supplemental material = 11 pages, 5 figures

Dynamic reciprocity imposes stringent performance constraints on nonlinear optical devices such as isolators and circulators. The seminal result by Shi et al. establishes that nonlinear optical devices relying on the intensity-dependent refractive index obey dynamic reciprocity for small signals with spectrally distinct fields. However, it has also been recognized that it is possible to violate dynamic reciprocity by exploiting frequency mixing processes. In this paper, we establish a rigorous upper bound on this violation that is independent of device geometry. We demonstrate that this bound captures the parameter scalings of realizable physical systems, and that under some conditions dynamic reciprocity violation can grow unbounded to achieve arbitrary nonlinear isolation. These results provide an analytically robust version of dynamic reciprocity, as well as theoretical guidance for the development of power efficient nonlinear optical isolators and circulators.

Predicting the charged particle transport properties of warm dense matter / hot dense plasma mixtures is a challenge for analytical models. High accuracy ab initio methods are more computationally expensive, but can provide critical insight by explicitly simulating mixtures. In this work, we investigate the transport properties and optical response of warm dense carbon-hydrogen mixtures at varying concentrations under either conserved electronic pressure or mass density at a constant temperature. We compare options for mixing the calculated pure species properties to estimate the results of the mixtures. We find that a combination of the Drude model with the Matthiessen's rule works well for DC electron transport and low frequency optical response. This breaks down at higher frequencies, where a volumetric mix of pure-species AC conductivities works better., Comment: Special Collection: Charged-Particle Transport in High Energy Density Plasmas

Rapid progress in photonics has led to an explosion of integrated devices that promise to deliver the same performance as table-top technology at the nanoscale; heralding the next generation of optical communications, sensing and metrology, and quantum technologies. However, the challenge of co-integrating the multiple components of high-performance laser systems has left application of these nanoscale devices thwarted by bulky laser sources that are orders of magnitude larger than the devices themselves. Here we show that the two main ingredients for high-performance lasers -- noise reduction and isolation -- currently requiring serial combination of incompatible technologies, can be sourced simultaneously from a single, passive, CMOS-compatible nanophotonic device. To do this, we take advantage of both the long photon lifetime and the nonreciprocal Kerr nonlinearity of a high quality factor silicon nitride ring resonator to self-injection lock a semiconductor laser chip while also providing isolation. Additionally, we identify a previously unappreciated power regime limitation of current on-chip laser architectures which our system overcomes. Using our device, which we term a unified laser stabilizer, we demonstrate an on-chip integrated laser system with built-in isolation and noise reduction that operates with turnkey reliability. This approach departs from efforts to directly miniaturize and integrate traditional laser system components and serves to bridge the gap to fully integrated optical technologies.

Titanium:Sapphire (Ti:Sa) lasers have been essential for advancing fundamental research and technological applications. Ti:Sa lasers are unmatched in bandwidth and tuning range, yet their use is severely restricted due to their large size, cost, and need for high optical pump powers. Here, we demonstrate a monocrystalline Ti:Sa-on-insulator (Ti:SaOI) photonics platform which enables dramatic miniaturization, cost-reduction, and scalability of Ti:Sa technology. First, through fabrication of low-loss whispering gallery mode resonators, we realize a Ti:Sa laser operating with an ultra-low lasing threshold of 290 $\mu$W. Then, through orders-of-magnitude improvement in mode confinement in Ti:SaOI waveguides, we realize the first integrated solid-state (i.e., non-semiconductor) optical amplifier operating below 1 $\mu$m, with an ultra-wide bandwidth of 700 - 950 nm and peak gain of 64 dB/cm. We demonstrate unprecedented 17 dB distortion-free amplification of picosecond pulses to up to 2.3 nJ pulse energy, corresponding to a peak power of 1.0 kW. Finally, we demonstrate the first tunable integrated Ti:Sa laser, featuring narrow linewidths and a 24.7 THz tuning range, which, for the first time, can be pumped with low-cost, miniature, off-the-shelf green laser diodes. This opens doors to new modalities of Ti:Sa lasers (now occupying a footprint less than 0.15 mm$^2$), such as massively-scalable Ti:Sa laser array systems for a variety of applications. As a proof-of-concept demonstration, we employ a Ti:SaOI laser array as the sole optical control for a cavity quantum electrodynamics experiment with artificial atoms in silicon carbide. This work is a key step towards the democratization of Ti:Sa technology through a three orders-of-magnitude reduction in cost and footprint, as well as the introduction of solid-state broadband amplification of sub-micron wavelength light.

Automation can transform productivity in research activities that use liquid handling, such as organic synthesis, but it has made less impact in materials laboratories, which require sample preparation steps and a range of solid-state characterization techniques. For example, powder X-ray diffraction (PXRD) is a key method in materials and pharmaceutical chemistry, but its end-to-end automation is challenging because it involves solid powder handling and sample processing. Here we present a fully autonomous solid-state workflow for PXRD experiments that can match or even surpass manual data quality. The workflow involves 12 steps performed by a team of three multipurpose robots, illustrating the power of flexible, modular automation to integrate complex, multitask laboratories.

Efficient nanophotonic devices are essential for applications in quantum networking, optical information processing, sensing, and nonlinear optics. Extensive research efforts have focused on integrating two-dimensional (2D) materials into photonic structures, but this integration is often limited by size and material quality. Here, we use hexagonal boron nitride (hBN), a benchmark choice for encapsulating atomically thin materials, as a waveguiding layer while simultaneously improving the optical quality of the embedded films. When combined with photonic inverse design, it becomes a complete nanophotonic platform to interface with optically active 2D materials. Grating couplers and low-loss waveguides provide optical interfacing and routing, tunable cavities provide a large exciton-photon coupling to transition metal dichalcogenides (TMD) monolayers through Purcell enhancement, and metasurfaces enable the efficient detection of TMD dark excitons. This work paves the way for advanced 2D-material nanophotonic structures for classical and quantum nonlinear optics.

Spatial modes of light have become highly attractive to increase the dimension and, thereby, security and information capacity in quantum key distribution (QKD). So far, only transverse electric field components have been considered, while longitudinal polarization components have remained neglected. Here, we present an approach to include all three spatial dimensions of electric field oscillation in QKD by implementing our tunable, on-a-chip vector beam decoder (VBD). This inversely designed device pioneers the "preparation" and "measurement" of three-dimensionally polarized mutually unbiased basis states for high-dimensional (HD) QKD and paves the way for the integration of HD QKD with spatial modes in multifunctional on-a-chip photonics platforms., Comment: 10 pages, 3 figures. Corrected typos & added reference

Stochastic and mixed stochastic-deterministic density functional theory (DFT) are promising new approaches for the calculation of the equation-of-state and transport properties in materials under extreme conditions. In the intermediate warm dense matter regime, a state between correlated condensed matter and kinetic plasma, electrons can range from being highly localized around nuclei to delocalized over the whole simulation cell. The plane-wave basis pseudo-potential approach is thus the typical tool of choice for modeling such systems at the DFT level. Unfortunately, the stochastic DFT methods scale as the square of the maximum plane-wave energy in this basis. To reduce the effect of this scaling, and improve the overall description of the electrons within the pseudo-potential approximation, we present stochastic and mixed DFT developed and implemented within the projector augmented wave formalism. We compare results between the different DFT approaches for both single-point and molecular dynamics trajectories and present calculations of self-diffusion coefficients of solid density carbon from 1 to 50 eV.

Many attractive photonics platforms still lack integrated photodetectors due to inherent material incompatibilities and lack of process scalability, preventing their widespread deployment. Here we address the problem of scalably integrating photodetectors in a photonic platform-independent manner. Using a thermal evaporation and deposition technique developed for nanoelectronics, we show that tellurium (Te), a quasi-2D semi-conductive element, can be evaporated at low temperature directly onto photonic chips to form air-stable, high-responsivity, high-speed, ultrawide-band photodetectors. We demonstrate detection at visible, telecom, and mid-infrared wavelengths, a bandwidth of more than 40 GHz, and platform-independent scalable integration with photonic structures in silicon, silicon nitride and lithium niobate.

Fiber and bulk-optical isolators are widely used to stabilize laser cavities by preventing unwanted feedback. However, their integrated counterparts have been slow to be adopted. While several strategies for on-chip optical isolation have been realized, these rely on either integration of magneto-optic materials or high frequency modulation with acousto-optic or electro-optic modulators. Here, we demonstrate an integrated approach for passively isolating a continuous wave laser using the intrinsically non-reciprocal Kerr nonlinearity in ring resonators. Using silicon nitride as a model platform, we achieve single ring isolation of 17-23dB with 1.8-5.5dB insertion loss, and a cascaded ring isolation of 35dB with 5dB insertion loss. Employing these devices, we demonstrate hybrid integration and isolation with a semi-conductor laser chip.

Vortex beams are stable solutions of Maxwell's equations that carry phase singularities and orbital angular momentum, unique properties that give rise to many applications in the basic sciences, optical communications, and quantum technologies. Scalable integration and fabrication of vortex beam emitters will allow these applications to flourish and enable new applications not possible with traditional optics. Here we present a general framework to generate integrated vortex beam emitters using photonic inverse design. We experimentally demonstrate generation of vortex beams with angular momentum spanning -3$\hbar$ to 3$\hbar$. We show the generality of this design procedure by designing a vortex beam multiplexer capable of exciting a custom vortex beam fiber. Finally, we produce foundry-fabricated beam emitters with wide-bandwidths and high-efficiencies that take advantage of a multi-layer heterogeneous integration.

The inner operations of the human brain as a biological processing system remain largely a mystery. Inspired by the function of the human brain and based on the analysis of simple neural network systems in other species, such as Drosophila, neuromorphic computing systems have attracted considerable interest. In cellular-level connectomics research, we can identify the characteristics of biological neural network, called population, which constitute not only recurrent fullyconnection in network, also an external-stimulus and selfconnection in each neuron. Relying on low data bandwidth of spike transmission in network and input data, Spiking Neural Networks exhibit low-latency and low-power design. In this study, we proposed a configurable population-based digital spiking neuromorphic processor in 180nm process technology with two configurable hierarchy populations. Also, these neurons in the processor can be configured as novel models, integer quadratic integrate-and-fire neuron models, which contain an unsigned 8-bit membrane potential value. The processor can implement intelligent decision making for avoidance in real-time. Moreover, the proposed approach enables the developments of biomimetic neuromorphic system and various low-power, and low-latency inference processing applications.

Warm dense matter (WMD) describes an intermediate phase, between condensed matter and classical plasmas, found in natural and man-made systems. In a laboratory setting, WDM needs to be created dynamically. It is typically laser or pulse-power generated and can be difficult to characterize experimentally. Measuring the energy loss of high energy ions, caused by a WDM target, is both a promising diagnostic and of fundamental importance to inertial confinement fusion research. However, electron coupling, degeneracy, and quantum effects limit the accuracy of easily calculable kinetic models for stopping power, while high temperatures make the traditional tools of condensed matter, e.g. Time-Dependent Density Functional Theory (TD-DFT), often intractable. We have developed a mixed stochastic-deterministic approach to TD-DFT which provides more efficient computation while maintaining the required precision for model discrimination. Recently, this approach showed significant improvement compared to models when compared to experimental energy loss measurements in WDM carbon. Here, we describe this approach and demonstrate its application to warm dense carbon stopping acr

Recent advances in the design and fabrication of on-chip optical microresonators has greatly expanded their applications in photonics, enabling metrology, communications, and on-chip lasers. Designs for these applications require fine control of dispersion, bandwidth and high optical quality factors. Co-engineering these figures of merit remains a significant technological challenge due to design strategies being largely limited to analytical tuning of cross-sectional geometry. Here, we show that photonic inverse-design facilitates and expands the functionality of on-chip microresonators; theoretically and experimentally demonstrating flexible dispersion engineering, quality factor beyond 2 million on the silicon-on-insulator platform with single mode operation, and selective wavelength-band operation.

Superradiance is the enhanced emission of photons from quantum emitters collectively coupling to the same optical mode. However, disorder in the resonant frequencies of the quantum emitters can perturb this effect. In this paper, we study the interplay between superradiance and spectral disorder in a dynamically modulated Tavis-Cummings model. Through numerical simulations and analytical calculations, we show that the effective cooperativity of the superradiant mode, which is always formed over an extensive number of emitters, can be multiplicatively enhanced with a quantum control protocol modulating the resonant frequency of the optical mode. Our results are relevant to experimental demonstration of superradiant effects in solid-state quantum optical systems, wherein the spectral disorder is a significant technological impediment towards achieving photon-mediated emitter-emitter couplings.

Modern microelectronic processors have migrated towards parallel computing architectures with many-core processors. However, such expansion comes with diminishing returns exacted by the high cost of data movement between individual processors. The use of optical interconnects has burgeoned as a promising technology that can address the limits of this data transfer. While recent pushes to enhance optical communication have focused on developing wavelength-division multiplexing technology, this approach will eventually saturate the usable bandwidth, and new dimensions of data transfer will be paramount to fulfill the ever-growing need for speed. Here we demonstrate an integrated intra- and inter-chip multi-dimensional communication scheme enabled by photonic inverse design. Using inverse-designed mode-division multiplexers, we combine wavelength- and mode- multiplexing and send massively parallel data through nano-photonic waveguides and optical fibres. Crucially, as we take advantage of an orthogonal optical basis, our approach is inherently scalable to a multiplicative enhancement over the current state of the art., Comment: Fig.2-4 present new experimental results -- (i) demonstration of a broadband, low cross-talk multiplexer, (ii) a silicon photonic mode-division multiplexing with a chip-scale soliton microcomb source, and (iii) a chip-to-chip optical interconnect using a multimode-matched fibre and inverse-designed beam couplers

We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a classical trajectory of the nuclei. Using this Hamiltonian we derive equations of motion for the electronic occupation numbers and for the nuclear coordinates and momenta. We show that in the limit when the number of nuclear degrees of freedom coupled to a given electronic transition is sufficiently high (i.e., the strong decoherence limit), the equations of motion for the electronic occupation numbers become Markovian. Furthermore the transition rates in these (rate) equations are asymmetric with respect to the lower-to-higher energy transitions and vice versa. In thermal equilibrium such asymmetry corresponds to the detailed balance condition. We also study the equations for the electronic occupations in non-Markovian regime and develop a surface hopping algorithm based on our formalism. To treat the decoherence effects we introduce additional "virtual" nuclear wavepackets whose interference with the "real" (physical) wavepackets leads to the reduction in coupling between the electronic states (i.e., decoherence) as well as to the phase shifts that improve the accuracy of the numerical approach. Remarkably, the same phase shifts lead to the detailed balance condition in the strong decoherence limit., Comment: 14 pages, 5 figures

Understanding many processes, e.g. fusion experiments, planetary interiors and dwarf stars, depends strongly on microscopic physics modeling of warm dense matter (WDM) and hot dense plasma. This complex state of matter consists of a transient mixture of degenerate and nearly-free electrons, molecules, and ions. This regime challenges both experiment and analytical modeling, necessitating predictive \emph{ab initio} atomistic computation, typically based on quantum mechanical Kohn-Sham Density Functional Theory (KS-DFT). However, cubic computational scaling with temperature and system size prohibits the use of DFT through much of the WDM regime. A recently-developed stochastic approach to KS-DFT can be used at high temperatures, with the exact same accuracy as the deterministic approach, but the stochastic error can converge slowly and it remains expensive for intermediate temperatures (<50 eV). We have developed a universal mixed stochastic-deterministic algorithm for DFT at any temperature. This approach leverages the physics of KS-DFT to seamlessly integrate the best aspects of these different approaches. We demonstrate that this method significantly accelerated self-consistent field calculations for temperatures from 3 to 50 eV, while producing stable molecular dynamics and accurate diffusion coefficients.

The ability to shape photon emission facilitates strong photon-mediated interactions between disparate physical systems, thereby enabling applications in quantum information processing, simulation and communication. Spectral control in solid state platforms such as color centers, rare earth ions, and quantum dots is particularly attractive for realizing such applications on-chip. Here we propose the use of frequency-modulated optical transitions for spectral engineering of single photon emission. Using a scattering-matrix formalism, we find that a two-level system, when modulated faster than its optical lifetime, can be treated as a single-photon source with a widely reconfigurable photon spectrum that is amenable to standard numerical optimization techniques. To enable the experimental demonstration of this spectral control scheme, we investigate the Stark tuning properties of the silicon vacancy in silicon carbide, a color center with promise for optical quantum information processing technologies. We find that the silicon vacancy possesses excellent spectral stability and tuning characteristics, allowing us to probe its fast modulation regime, observe the theoretically-predicted two-photon correlations, and demonstrate spectral engineering. Our results suggest that frequency modulation is a powerful technique for the generation of new light states with unprecedented control over the spectral and temporal properties of single photons., Comment: 9 pages, 6 figures; Supplementary Information

Complex plasma mixtures with three or more components are often encountered in astrophysics or in inertial confinement fusion (ICF) experiments. For mixtures containing species with large differences in atomic number Z, the modeling needs to consider at the same time the kinetic theory for low-Z elements combined with the theory of strongly coupled plasma for high-Z elements, as well as all the intermediate situations that can appear in multi-component systems. For such cases, we study the pair distribution functions, self-diffusions, mutual diffusion and viscosity for ternary mixtures at extreme conditions. These quantities can be produced from first principles using orbital free molecular dynamics at the computational expense of very intensive simulations to reach good statistics. Utilizing the first-principles results as reference data, we assess the merit of a global analytic model for transport coefficients, Pseudo-Ions in Jellium (PIJ), based on an iso-electronic assumption ( iso-n e ). With a multi-component hypernetted-chain integral equation, we verify the quality of the iso-n e prescription for describing the static structure of the mixtures. This semi-analytical modeling compares well with the simulation results and allows one to consider plasma mixtures not accessible to simulations. Applications are given for the mix of materials in ICF experiments. A reduction of a multicomponent mixture to an effective binary mixture is also established in the hydrodynamic limit and compared with PIJ estimations for ICF relevant mixtures., Comment: 17 pages, 10 Figures

Mixed quantum-classical mechanics descriptions are critical to modeling coupled electron-nuclear dynamics, i.e. non-adiabatic molecular dynamics, relevant to photochemical and photophysical processes. We argue that, for polyatomic molecules, such mixed dynamics can not be efficiently described in terms of a matrix gauge potential and develop the concept of a `length gauge' effective Hamiltonian, which helps clarifying certain aspects for the popular non-adiabatic computational approaches. In particular, within such an effective Hamiltonain formalism one readily derives the momentum rescaling boundary condition, used in the surface hopping algorithms. Furthermore, using the new formalism, we introduce a coupled Gaussian wavepacket parameterization of the nuclear wavefunction, which generalizes the Ehrenfest approach to account for electron-nuclei correlations. We test this new approach, Ehrenfest-Plus, on the standard set of model problems that probe electron-nuclear correlation in non-adiabatic transitions. The high accuracy of our approach, combined with mixed-quantum classical efficiency, opens a path for improved simulation of non-adiabatic molecular dynamics in realistic molecular systems.

We investigate the plasma enhancement of nuclear reactions in the intermediate coupling regime using orbital free molecular dynamics (OFMD) simulations. Mixtures of H-Cu and H-Ag serve as prototypes of simultaneous weak and strong couplings due to the charge asymmetry. Of particular importance is the partial ionization of Cu and Ag and the free electron polarization captured by OFMD simulations. By comparing a series of OFMD simulations at various concentrations and constant pressure to multi-component hyper netted chain (MCHNC) calculations of effective binary ionic mixtures (BIM), we set a general procedure for computing enhancement factors. The MCHNC procedure allows extension to very low concentrations (5% or less) and to very high temperatures (few keV) unreachable by the simulations. Enhancement factors for nuclear reactions rates extracted from the MCHNC approach are compared with the Salpeter theory in the weak and strong coupling regimes, and a new interpolation is proposed., Comment: 14 pages 9 figures 2 Tables