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Topological photonics is an emergent research discipline which interlinks fundamental aspects of photonics, information processing and solid-state physics. Exciton-polaritons are a specifically interesting platform to study topological phenomena, since the coherent light matter coupling enables new degrees of freedom such as tunable non-linearities, chiralities and dissipation. Room-temperature operation of such exciton-polaritons relies on materials comprising both, large exciton binding energies and oscillator strength. We harness widely spectrally tunable, room temperature exciton-polaritons based on a WS2 monolayer in an open optical cavity to realize a polariton potential landscape which emulates the Su-Schrieffer-Heeger (SSH) Hamiltonian. It comprises a domain boundary hosting a topological, exponentially localized mode at the interface between two lattices characterized by different Zak-phases which features a spectral tunability over a range as large as 80 meV. Moreover, we utilize the unique tilt-tunability of our implementation, to transform the SSH-lattice into a Stark-ladder. This transformation couples the topologically protected defect mode to propagating lattice modes, and effectively changes the symmetry of the system. Furthermore, it allows us to directly quantify the Zak-phase difference $\Delta_{Zak}=(1.13\pm 0.11)\pi$ between the two topological phases. Our work comprises an important step towards in-situ tuning topological lattices to control and guide light on non-linear chips.

We propose a scheme for quantum-light generation in a nonlinear cavity hybridized with a 2-level system and theoretically show that, when excited by a series of controlled pump pulses, the hybrid source generates Fock states with high probabilities. E.g., 1- and 2-photon states can be generated near-on-demand, and Fock states with up to $7$ photons with a probability above $50\%$. The tailorable nature of the nonlinear cavity allows for generating Fock states with arbitrary frequencies, even with a fixed 2-level system, creating fundamentally new opportunities in all areas of quantum technologies.

Large language models (LLMs) have gained widespread interest due to their ability to process human language and perform tasks on which they have not been explicitly trained. However, we possess only a limited systematic understanding of the chemical capabilities of LLMs, which would be required to improve models and mitigate potential harm. Here, we introduce "ChemBench," an automated framework for evaluating the chemical knowledge and reasoning abilities of state-of-the-art LLMs against the expertise of chemists. We curated more than 2,700 question-answer pairs, evaluated leading open- and closed-source LLMs, and found that the best models outperformed the best human chemists in our study on average. However, the models struggle with some basic tasks and provide overconfident predictions. These findings reveal LLMs' impressive chemical capabilities while emphasizing the need for further research to improve their safety and usefulness. They also suggest adapting chemistry education and show the value of benchmarking frameworks for evaluating LLMs in specific domains.

One-dimensional models with topological non-trivial band structures are a simple and effective way to study novel and exciting concepts in topological photonics. In this work we are studying the propagation of light-matter quasi-particles, so called exciton-polaritons, in waveguide arrays. Specifically, we are investigating topological states at the interface between dimer chains, characterized by a non-zero winding number. In order to exercise precise control over the polariton propagation, we study non-resonant laser excitation as well as resonant excitation in transmission geometry. The results highlight a new platform for the study of quantum fluids of light and non-linear optical propagation effects in coupled semiconductor waveguides.

With a seminal work of Raghu and Haldane in 2008, concepts of topology have been successfully introduced in a wide range of optical systems, emulating specific lattice Hamiltonians. Certainly, one of the most promising routes to an application of topological photonics in an actual device are topological lasers, where efficient and highly coherent lasing from a topologically non-trivial mode is achieved. While some attempts have been made to excite such structures electrically, the majority of published fundamental experiments use a form of laser excitation. In this paper, we use a lattice of vertical resonator polariton micropillars to form an exponentially localized topological Su-Schrieffer-Heeger defect. Upon electrical excitation of the p-i-n doped structure, the system unequivocally shows polariton lasing from the topological defect using a carefully placed gold contact. Despite the presence of doping and electrical contacts, the polariton band structure clearly preserves its topological properties. At high excitation power the Mott density is exceeded leading to highly efficient lasing in the weak coupling regime. This work is an important step towards applied topological lasers using vertical resonator microcavity structures., Comment: 21 pages, 7 figures

High-order harmonic generation (HHG) in solids is profoundly influenced by the dephasing of the coherent electron-hole motion driven by an external laser field. The exact physical mechanisms underlying this dephasing, crucial for accurately understanding and modelling HHG spectra, have remained elusive and controversial, often regarded more as an empirical observation than a firmly established principle. In this work, we present comprehensive experimental findings on the wavelength-dependency of HHG in both single-atomic-layer and bulk semiconductors. These findings are further corroborated by rigorous numerical simulations, employing ab initio real-time, real-space time-dependent density functional theory and semiconductor Bloch equations. Our experimental observations necessitate the introduction of a novel concept: a momentum-dependent dephasing time in HHG. Through detailed analysis, we pinpoint momentum-dependent electron-phonon scattering as the predominant mechanism driving dephasing. This insight significantly advances the understanding of dephasing phenomena in solids, addressing a long-standing debate in the field. Furthermore, our findings pave the way for a novel, all-optical measurement technique to determine electron-phonon scattering rates and establish fundamental limits to the efficiency of HHG in condensed matter.

Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length-scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance., Comment: 22 pages, 4 figures, typos corrected in the updated version

We investigate the spatial characteristics of high-order harmonic radiation generated in argon, and observe cross-like patterns in the far field. An analytical model describing harmonics from an astigmatic driving beam reveals that these patterns result from the order and generation position dependent divergence of harmonics. Even small amounts of driving field astigmatism may result in cross-like patterns, coming from the superposition of individual harmonics with spatial profiles elongated in different directions. By correcting the aberrations using a deformable mirror, we show that fine-tuning the driving wavefront is essential for optimal spatial quality of the harmonics.

X-ray absorption spectroscopy (XAS) is an element-specific materials characterization technique that is sensitive to structural and electronic properties. First-principles simulated XAS has been widely used as a powerful tool to interpret experimental spectra and draw physical insights. Recently, there has also been growing interest in building computational XAS databases to enable data analytics and machine learning applications. However, there are non-trivial differences among commonly used XAS simulation codes, both in underlying theoretical formalism and in technical implementation. Reliable and reproducible computational XAS databases require systematic benchmark studies. In this work, we benchmarked Ti K-edge XAS simulations of ten representative Ti-O binary compounds, which we refer to as the Ti-O-10 dataset, using three state-of-the-art codes: xspectra, ocean and exciting. We systematically studied the convergence behavior with respect to the input parameters and developed a workflow to automate and standardize the calculations to ensure converged spectra. Our benchmark comparison shows: (1) the two Bethe-Salpeter equation (BSE) codes (ocean and exciting) have excellent agreement in the energy range studied (up to 35 eV above the onset) with an average Spearman's rank correlation score of 0.998; (2) good agreement is obtained between the core-hole potential code (xspectra) and BSE codes (ocean and exciting) with an average Spearman's rank correlation score of 0.990. Our benchmark study provides important standards for first-principles XAS simulations with broad impact in data-driven XAS analysis., Comment: 32 pages, 11 figures and 7 tables

Attosecond pulses created by high-order harmonic generation in gases often exhibit strong chromatic aberrations, arising from the broad bandwidth and wavelength-dependent nonlinear light-matter interaction. When the driving laser intensity varies spatially, as for Gaussian driving beams, the apparent source position of the harmonics differs significantly from one order to the next, thus affecting the achievable intensity and duration of the attosecond pulses when they are focused on a target. We show that these chromatic aberrations can be reduced by spatially shaping the fundamental beam to generate high-order harmonics with a driver having a flat-top profile inside the gas medium. By measuring both the intensity profile and wavefront for each harmonic in a plane, we access the extreme ultra-violet (XUV) beam properties and investigate these properties near focus. We observe that controlling chromatic aberrations by flat-top spatial shaping strongly reduces the variation of the XUV spectrum on the beam axis during propagation and, in return, the longitudinal sensitivity of both the temporal profiles and the temporal shifts of the focused attosecond pulses., Comment: 12 pages, 8 figures + supplementary material: 10 pages, 13 figures

We investigate the generation of higher-order harmonics from a quantum optics perspective via the interaction of a semiconductor with a coherent pump field focusing on the regime where strong-field intraband excitations dominate. The related Schr\"odinger equation for the system is solved approximately and the classical and quantum characteristics of the fundamental light mode as well as the higher frequency modes are analyzed. We find intricate but sufficiently mild modifications of the fundamental mode and coherent displacements depending on the position quadrature component of the driving laser field for the harmonic modes within our approximations due to the intricate induced nonlinear interactions. Similar to high-harmonic generation in atoms, all radiation field modes are entangled, allowing for potential novel protocols for quantum information processing with high photon numbers over a large range of frequencies., Comment: 6 pages, 2 figures, more concise presentation of section 2, improved plots

Tailoring the emission of plasmonic nanowire-based lasers represents one of the major challenges in the field of nanoplasmonics, given the envisaged integration of such devices into on-chip all-optical circuits. In this study, we proposed a mode selection scheme based on distributed feedback, achieved via the external coupling of single zinc oxide nanowires to an aluminum grating, which enabled a quasi-single mode lasing action. The nano-manipulation of a single nanowire allowed for a reliable comparison of the lasing emission characteristics in both planar (i.e. nanowire on the metallic substrate) and on-grating configurations. We found that, by varying the orientation of the nanowire on the grating, only when the nano-cavity was perpendicular to the ridge direction, an additional peak emerged in the emission spectrum on the low-energy side of the gain envelope. As a consequence of the fulfillment of the Bragg condition, such a peak was attributed to a hybrid mode dominating the mode competition. Simulation results showed that the hybrid mode could be efficiently waveguided along the nanowire cavity and supported by localized plasmon polaritons building up at the raised features ("fences") on top of the metal grating ridges. Moreover, the hybrid mode was found to experience an extra reflectance of nearly 50% across the grating periods, in addition to that provided by the nanowire end facets.

Semiconductor nanowire lasers can be subject to modifications of their lasing threshold resulting from a variation of their environment. A promising choice is to use metallic substrates to gain access to low-volume Surface-Plasmon-Polariton (SPP) modes. We introduce a simple, yet quantitatively precise model that can serve to describe mode competition in nanowire lasers on metallic substrates. We show that an aluminum substrate can decrease the lasing threshold for ZnO nanowire lasers while for a silver substrate, the threshold increases compared with a dielectric substrate. Generalizing from these findings, we make predictions describing the interaction between planar metals and semiconductor nanowires, which allow to guide future improvements of highly-integrated laser sources.

The phasing problem of heterodyne-detected nonlinear spectroscopy states that the relative time delay between the exciting pulses and a local oscillator must be known with subcycle precision to separate absorptive and dispersive contributions. Here, a solution to this problem is presented which is the time-domain analogue of holographic interferometry, in which the comparison of two holograms reveals changes of an objects size and position with interferometric precision (i.e. to fractions of a wavelength of light). The introduced method, called nonlinear polarization holography, provides equivalent information as attosecond nonlinear polarization spectroscopy but has the advantage of being all-optical instead of using an attosecond streak camera. Nonlinear polarization holography is used here to retrieve the time-domain nonlinear response of a nanoscale iridium film to an ultrashort femtosecond pulse. Using density matrix calculations it is shown that the knowledge of the nonlinear response with subcycle precision allows to distinguish excitation and relaxation mechanisms of low-energetic electrons that depend on the nanoscale structure of the iridium film.

First-principles computational spectroscopy is a critical tool for interpreting experiment, performing structure refinement, and developing new physical understanding. Systematically setting up input files for different simulation codes and a diverse class of materials is a challenging task with a very high barrier-to-entry, given the complexities and nuances of each individual simulation package. This task is non-trivial even for experts in the electronic structure field and nearly formidable for non-expert researchers. Lightshow solves this problem by providing a uniform abstraction for writing computational x-ray spectroscopy input files for multiple popular codes, including FEFF, VASP, OCEAN, EXCITING and XSPECTRA. Its extendable framework will also allow the community to easily add new functions and to incorporate new simulation codes., Comment: 3 pages, 1 figure, software can be found open source under the BSD-3-clause license at https://github.com/AI-multimodal/Lightshow

Efficient modeling of dispersive materials via time-domain simulations of the Maxwell equations relies on the technique of auxiliary differential equations. In this approach, a material's frequency-dependent permittivity is represented via a sum of rational functions, e.g. Lorentz-poles, and the associated free parameters are determined by fitting to experimental data. In the present work, we present a modified approach for plasmonic materials that requires considerably fewer fit parameters than traditional approaches. Specifically, we consider the underlying microscopic theory and, in the frequency domain, separate the hydrodynamic contributions of the quasi-free electrons in partially filled bands from the interband transitions. As an illustration, we apply our approach to gold and demonstrate how to treat the interband transitions within the effective model via connecting to the underlying electronic bandstructure, thereby assigning physical meaning to the remaining fit parameters. Finally, we show how to utilize this approach within the technique of auxiliary differential equations. Our approach can be extended to other plasmonic materials and leads to efficient time-domain simulations of plasmonic structures for frequency ranges where interband transitions have to be considered., Comment: 9 pages, 3 figures, 1 table

We discuss the semi-classical transverse trapping of waves by means of an inhomogeneous gauge field. In the proposed scheme a temporally-periodic perturbation is shifted in time, the imparted delay being dependent on the transverse direction. We show that, due to the Kapitza effect, an effective potential proportional to the square of the transverse derivative of the delay arises. On a more physical ground, the delay induces a transversely-varying periodic force acting on the wave, in turn providing a phase delay owing to the local modulation of the kinetic energy. Our results are quite generic and can find application in several fields, ranging from cold atoms to optics: accordingly, an experimental proof-of-principle is provided using an optical set-up based upon fiber loops., Comment: 15 pages, 11 figures

The Thomas--Reiche--Kuhn sum rule is used to form an effective potential that is added to the time-dependent configuration interaction singles (TDCIS) equations of motion in velocity gauge. The purpose of the effective potential is to include virtual coupling from singles to doubles, which is required for size-consistent velocity gauge TDCIS results. The proposed method is compared to length gauge TDCIS results for laser-assisted photoionization. Finally, a novel dynamical interference effect controlled by two-color fields is predicted for atomic targets.

We study resonant two-photon ionization of helium atoms via the $1s3p$, $1s4p$ and $1s5p^1$P$_1$ states using the 15$^\mathrm{th}$ harmonic of a titanium-sapphire laser for the excitation and a weak fraction of the laser field for the ionization. The phase of the photoelectron wavepackets is measured by an attosecond interferometric technique, using the 17$^\mathrm{th}$ harmonic. We perform experiments with angular resolution using a velocity map imaging spectrometer and with high energy resolution using a magnetic bottle electron spectrometer. Our results are compared to calculations using the two-photon random phase approximation with exchange to account for electron correlation effects. We give an interpretation for the multiple $\pi$-rad phase jumps observed, both at and away from resonance, as well as their dependence on the emission angle.