arXiv subjects

Christian Schäfer

Publications and source records attributed to Christian Schäfer.

At least 19 recordsLinked to original sources

arXiv2026

A Hierarchical Approach to Quantum Many-Body Systems in Non-Markovian Environments

Quantum many-body systems in cavities combine the rich physics of condensed matter systems or quantum chemistry with strong coupling to the surrounding electromagnetic field. In these systems, large Hilbert spaces, many-body interactions and strong system-environment coupling are all fundamental, posing a significant barrier for established methods in quantum optics and condensed matter physics. Here we propose a novel method based on a combination of the Bogoliubov-Born-Green-Kirkwood-Yvon (BBGKY) hierarchy and the Hierarchical Equations of Motion (HEOM) to achieve a rigorous description of open many-body systems in contact with structured photonic and phononic baths. We rationalize that this stacked hierarchy accounts for spin-squeezing and superradiant emission despite its applicability to arbitrarily many emitters. The potential of BBGKY-HEOM is then demonstrated for many-body electronic systems embedded in host materials (e.g. molecules in organic crystals). We show that the impact of phononic coupling and charge noise can be as relevant as electronic correlation. Our work establishes an accessible, yet rigorous, route between condensed matter and quantum optics, fostering the growth of a new domain at their interface.

quant-ph↗

arXiv2026

Aromatic molecular emitters in a hexagonal boron nitride stack

Single polycyclic aromatic hydrocarbon molecules embedded in organic matrices have proven to be an excellent family of narrow-linewidth quantum emitters. Extending this host-guest setting to van der Waals materials offers the opportunity to combine the preeminent properties of molecular emitters with the access to the versatility of two-dimensional hetero-structures and devices. In this work, we incorporate perylene molecules into multi-layered hexagonal boron nitride stacks and observe gigahertz-narrow zero-phonon-line transitions at cryogenic temperatures. We unambiguously verify the origins of photon emission through vibronic spectra analysis. By combining hyperspectral localization measurements with quantum chemistry calculations, we examine the insertion mechanisms of perylene molecules in the hexagonal boron nitride stacks, and conclude that pristine hBN layers tend to expel molecules from the sandwich, while extended morphological defects, hydroxyl groups and unpassivated boron and nitrogen atoms assist to stabilize molecular bindings to hBN. Our work provides valuable insight for future work to deterministically integrate narrow-linewidth molecular emitters into van der Waals devices.

physics.optics↗

arXiv2026

Vibrationally Induced Resonances in Lasing

Optical circuits and light sources, such as lasers, undergo continuous miniaturization. In its extreme, nanolasers might be comprised of only a few molecules confined in plasmonic nanoresonators. Few-emitter lasers promise low energy requirements and fast responses in a footprint that can be inserted into any device or biological tissue. Utilizing the recently developed stacked hierarchy approach, informed from first principles, we demonstrate the impact of vibrational structure on lasing, using the example of few-molecule lasing in plasmonic cavities. Explicitly accounting for the entire vibrational manifold unveils resonances in the laser intensity that depend on the Stokes shift, drive strength, and the number of emitters. Our work identifies the limits of the omnipresent "incoherent drive"-approximation and paves the way for the understanding of nanolasers at the molecular scale.

quant-ph↗

arXiv2026

Secure Data Bridging in Industry 4.0: An OPC UA Aggregation Approach for Including Insecure Legacy Systems

The increased connectivity of industrial networks has led to a surge in cyberattacks, emphasizing the need for cybersecurity measures tailored to the specific requirements of industrial systems. Modern Industry 4.0 technologies, such as OPC UA, offer enhanced resilience against these threats. However, widespread adoption remains limited due to long installation times, proprietary technology, restricted flexibility, and formal process requirements (e.g. safety certifications). Consequently, many systems do not yet implement these technologies, or only partially. This leads to the challenge of dealing with so-called brownfield systems, which are often placed in isolated security zones to mitigate risks. However, the need for data exchange between secure and insecure zones persists. This paper reviews existing solutions to address this challenge by analysing their approaches, advantages, and limitations. Building on these insights, we identify three key concepts, evaluate their suitability and compatibility, and ultimately introduce the SigmaServer, a novel TCP-level aggregation method. The developed proof-of-principle implementation is evaluated in an operational technology (OT) testbed, demonstrating its applicability and effectiveness in bridging secure and insecure zones.

cs.CR↗

arXiv2025

Prediction of Molecular Single-Photon Emitters: A Materials-Modelling Approach

Interfacing light with quantum systems is an integral part of quantum technology, with the most essential building block being single-photon emitters. Although various platforms exist, each with its individual strengths, molecular emitters boast a unique advantage -- namely the flexibility to tailor their design to fit the requirements of a specific task. However, the characteristics of the vast space of possible molecular configurations are challenging to understand and explore. Here, we present a theoretical and computational framework to initiate exploration of this vast potential by integrating database analysis with microscopic predictions. Using a model system of dibenzoterrylene in an anthracene host as benchmark, our approach identifies promising new candidates, among them a chiral molecular emitter. Future extensions of our approach integrated with machine learning routines hold the promise of ultimately unlocking the full potential of molecular quantum light-matter interfaces.

quant-ph↗

arXiv2025

Frustrated Frustration of Arrays with Four-Terminal Nb-Pt-Nb Josephson Junctions

We study the frustration pattern of a square lattice with in-situ fabricated Nb-Pt-Nb four-terminal Josephson junctions. The four-terminal geometry gives rise to a checker board pattern of alternating fluxes f, f' piercing the plaquettes, which stabilizes the Berezinskii-Kosterlitz-Thouless transition even at irrational flux quanta per plaquette, due to an unequal repartition of integer flux sum f+f' into alternating plaquettes. This type of frustrated frustration manifests as a beating pattern of the dc resistance, with state configurations at the resistance dips gradually changing between the conventional zero-flux and half-flux states. Hence, the four-terminal Josephson junction array offers a promising platform to study previously unexplored flux and vortex configurations, and provides an estimate on the spatial expansion of the four-terminal Josephson junction central weak link area.

cond-mat.supr-con↗

arXiv2025

Effective Equilibrium Theory of Quantum Light-Matter Interaction in Cavities: Extended Systems and the Long Wavelength Approximation

When light and matter interact strongly, the resulting hybrid system inherits properties from both constituents, allowing one to modify material behavior by engineering the surrounding electromagnetic environment. This concept underlies the emerging paradigm of cavity materials engineering, which aims at the control of material properties via tailored vacuum fluctuations of dark photonic environments. The theoretical description of such systems is challenging due to the combined complexity of extended electronic states and quantum electromagnetic fields. Here, we derive an effective, non-perturbative theory for low-dimensional crystals embedded in a Fabry-Pérot resonator, within the long-wavelength limit. Our approach incorporates the multimode and dispersive nature of the cavity field and reduces it to an effective single-mode description by imposing the condition of negligible momentum transfer from light to matter. Importantly, the resulting effective mode is characterized by a finite mode volume-even in the limit of extended cavities-which is directly linked to realistic cavity parameters. This ensures that the light-matter coupling remains finite in bulk systems. By explicitly accounting for the finite reflectivity of cavity mirrors, our theory also avoids double counting the contribution from free-space light-matter coupling. Overall, our results provide a robust and realistic framework for describing cavity-matter interactions at the Hamiltonian level, incorporating the electromagnetic environment beyond the idealized perfect-mirror approximation.

cond-mat.mes-hall↗

arXiv2025

The Role of Dark States on Azopyrrole Photoisomerization Reaction by Varying the Coupling Strength of Light-Matter Interaction

Strong light-matter interactions are gaining importance in controlling the photoswitching behavior of molecules exhibiting bistability. Here, we used the strategy of electronic strong coupling of both the E and Z-isomers of azopyrrole photoswitches to a single cavity mode, thereby tuning the conditions from strong to weak coupling in an on-the-go photoisomerization process. This allows in situ monitoring of apparent rates of forward and backward reactions. Very interestingly, the kinetics follow a non-linear trend with a sharp switch in the kinetic slope at the intermediate coupling regime. At this condition, pumping at the upper polaritonic state and the uncoupled population shows an acceleration of the photoisomerization process mediated by the dark state manifold. On the other hand, an opposite effect is observed while exciting the lower polaritonic state. Performing the same experiment in the ultra-strong coupling regime shows no dynamic change over time but further emphasizes the outstanding role of the lower polaritonic states. Our experimental and theoretical findings underline the importance of collective strong coupling in tailoring energy transfer to control photoisomerization dynamically.

physics.chem-ph↗

arXiv2024

AsIf: Asset Interface Analysis of Industrial Automation Devices

As Industry 4.0 and the Industrial Internet of Things continue to advance, industrial control systems are increasingly adopting IT solutions, including communication standards and protocols. As these systems become more decentralized and interconnected, a critical need for enhanced security measures arises. Threat modeling is traditionally performed in structured brainstorming sessions involving domain and security experts. Such sessions, however, often fail to provide an exhaustive identification of assets and interfaces due to the lack of a systematic approach. This is a major issue, as it leads to poor threat modeling, resulting in insufficient mitigation strategies and, lastly, a flawed security architecture. We propose a method for the analysis of assets in industrial systems, with special focus on physical threats. Inspired by the ISO/OSI reference model, a systematic approach is introduced to help identify and classify asset interfaces. This results in an enriched system model of the asset, offering a comprehensive overview visually represented as an interface tree, thereby laying the foundation for subsequent threat modeling steps. To demonstrate the proposed method, the results of its application to a programmable logic controller (PLC) are presented. In support of this, a study involving a group of 12 security experts was conducted. Additionally, the study offers valuable insights into the experts' general perspectives and workflows on threat modeling.

cs.CR↗

arXiv2024

Quantized Embedding Approaches for Collective Strong Coupling -- Connecting ab initio and macroscopic QED to Simple Models in Polaritonics

Collective light-matter interactions have been used to control chemistry and energy transfer, yet accessible approaches that combine ab initio methodology with large many-body quantum optical systems are missing due to the fast increase in computational cost for explicit simulations. We introduce an accessible ab initio quantum embedding concept for many-body quantum optical systems that allows to treat the collective coupling of molecular many-body systems effectively in the spirit of macroscopic QED while keeping the rigor of ab initio quantum chemistry for the molecular structure. Our approach fully includes the quantum fluctuations of the polaritonic field and yet remains much simpler and more intuitive than complex embedding approaches such as dynamical mean-field theory. We illustrate the underlying assumptions by comparison to the Tavis--Cummings model. The intuitive application of the quantized embedding approach and its transparent limitations offer a practical framework for the field of ab initio polaritonic chemistry to describe collective effects in realistic molecular ensembles.

quant-ph↗

arXiv2024

Controlling Plasmonic Catalysis via Strong Coupling with Electromagnetic Resonators

Plasmonic excitations decay within femtoseconds, leaving non-thermal (often referred to as "hot") charge carriers behind that can be injected into molecular structures to trigger chemical reactions that are otherwise out of reach -- a process known as plasmonic catalysis. In this Letter, we demonstrate that strong coupling between resonator structures and plasmonic nanoparticles can be used to control the spectral overlap between the plasmonic excitation energy and the charge injection energy into nearby molecules. Our atomistic description couples real-time density-functional theory self-consistently to Maxwell's equations via the radiation-reaction potential. Control over the resonator provides then an additional knob for non-intrusively enhancing plasmonic catalysis and dynamically reacting to deterioration of the catalyst -- a new facet of modern catalysis.

cond-mat.mtrl-sci↗

arXiv2024

GPAW: An open Python package for electronic-structure calculations

We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE) providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe-Salpeter Equation (BSE), variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn-Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support of GPU acceleration has been achieved with minor modifications of the GPAW code thanks to the CuPy library. We end the review with an outlook describing some future plans for GPAW.

cond-mat.mtrl-sci↗

arXiv2024

Optimizing Variational Quantum Algorithms with qBang: Efficiently Interweaving Metric and Momentum to Navigate Flat Energy Landscapes

Variational quantum algorithms (VQAs) represent a promising approach to utilizing current quantum computing infrastructures. VQAs are based on a parameterized quantum circuit optimized in a closed loop via a classical algorithm. This hybrid approach reduces the quantum processing unit load but comes at the cost of a classical optimization that can feature a flat energy landscape. Existing optimization techniques, including either imaginary time-propagation, natural gradient, or momentum-based approaches, are promising candidates but place either a significant burden on the quantum device or suffer frequently from slow convergence. In this work, we propose the quantum Broyden adaptive natural gradient (qBang) approach, a novel optimizer that aims to distill the best aspects of existing approaches. By employing the Broyden approach to approximate updates in the Fisher information matrix and combining it with a momentum-based algorithm, qBang reduces quantum-resource requirements while performing better than more resource-demanding alternatives. Benchmarks for the barren plateau, quantum chemistry, and the max-cut problem demonstrate an overall stable performance with a clear improvement over existing techniques in the case of flat (but not exponentially flat) optimization landscapes. qBang introduces a new development strategy for gradient-based VQAs with a plethora of possible improvements.

quant-ph↗

arXiv2024

Tensorial properties via the neuroevolution potential framework: Fast simulation of infrared and Raman spectra

Infrared and Raman spectroscopy are widely used for the characterization of gases, liquids, and solids, as the spectra contain a wealth of information concerning in particular the dynamics of these systems. Atomic scale simulations can be used to predict such spectra but are often severely limited due to high computational cost or the need for strong approximations that limit application range and reliability. Here, we introduce a machine learning (ML) accelerated approach that addresses these shortcomings and provides a significant performance boost in terms of data and computational efficiency compared to earlier ML schemes. To this end, we generalize the neuroevolution potential approach to enable the prediction of rank one and two tensors to obtain the tensorial neuroevolution potential (TNEP) scheme. We apply the resulting framework to construct models for the dipole moment, polarizability, and susceptibility of molecules, liquids, and solids, and show that our approach compares favorably with several ML models from the literature with respect to accuracy and computational efficiency. Finally, we demonstrate the application of the TNEP approach to the prediction of infrared and Raman spectra of liquid water, a molecule (PTAF-), and a prototypical perovskite with strong anharmonicity (BaZrO3). The TNEP approach is implemented in the free and open source software package GPUMD, which makes this methodology readily available to the scientific community.

cond-mat.mes-hall↗

arXiv2024

Machine Learning for Polaritonic Chemistry: Accessing chemical kinetics

Altering chemical reactivity and material structure in confined optical environments is on the rise, and yet, a conclusive understanding of the microscopic mechanisms remains elusive. This originates mostly from the fact that accurately predicting vibrational and reactive dynamics for soluted ensembles of realistic molecules is no small endeavor, and adding (collective) strong light-matter interaction does not simplify matters. Here, we establish a framework based on a combination of machine learning (ML) models, trained using density-functional theory calculations, and molecular dynamics to accelerate such simulations. We then apply this approach to evaluate strong coupling, changes in reaction rate constant, and their influence on enthalpy and entropy for the deprotection reaction of 1-phenyl-2-trimethylsilylacetylene, which has been studied previously both experimentally and using ab initio simulations. While we find qualitative agreement with critical experimental observations, especially with regard to the changes in kinetics, we also find differences in comparison with previous theoretical predictions. The features for which the ML-accelerated and ab initio simulations agree show the experimentally estimated kinetic behavior. Conflicting features indicate that a contribution of dynamic electronic polarization to the reaction process is more relevant then currently believed. Our work demonstrates the practical use of ML for polaritonic chemistry, discusses limitations of common approximations and paves the way for a more holistic description of polaritonic chemistry.

physics.chem-ph↗

arXiv2023

Collective Strong Coupling Modifies Aggregation and Solvation

Intermolecular interactions are pivotal for aggregation, solvation, and crystallization. We demonstrate that the collective strong coupling of several molecules to a single optical mode results in notable changes in the molecular excitations around an impurity, e.g., in the first aggregation or solvation shell. A competition between short-range Coulombic and long-range photonic correlation inverts the local transition density in a polaritonic state, suggesting notable changes in the polarizability of the solvation shell. Our results provide an alternative perspective on recent work in polaritonic chemistry and pave the way for the rigorous treatment of cooperative effects in aggregation, solvation, and crystallization.

quant-ph↗

arXiv2023

Chiral Polaritonics: Analytic Solutions, Intuition and its Use

Preferential selection of a given enantiomer over its chiral counterpart becomes increasingly relevant in the advent of the next era of medical drug design. In parallel, cavity quantum electrodynamics has grown into a solid framework to control energy transfer and chemical reactivity. In this work, we derive an analytical solution to a system of many chiral emitters interacting with a chiral cavity -- in analogy to the widely used Tavis-Cummings and Hopfield models of quantum optics. We are able to estimate the discriminating strength of chiral polaritonics, discuss possible future development directions, exciting applications such as elucidating homochirality, and deliver much needed intuition to foster the freshly flourishing field of chiral polaritonics.

quant-ph↗

arXiv2022

Towards chiral polaritons

Coupling between light and material excitations underlies a wide range of optical phenomena. Polaritons are eigenstates of a coupled system with hybridized wave function. Owing to their hybrid composition, polaritons exhibit at the same time properties typical for photonic and electronic excitations, thus offering new ways for controlling electronic transport and even chemical kinetics. While most theoretical and experimental efforts have been focused on polaritons with electric-dipole coupling between light and matter, in chiral quantum emitters, electronic transitions are characterized by simultaneously nonzero electric and magnetic dipole moments. Geometrical chirality affects the optical properties of materials in a profound way and enables phenomena that underlie our ability to discriminate enantiomers of chiral molecules. Thus, it is natural to wonder what kinds of novel effects chirality may enable in the realm of strong light-matter coupling. Right now, this field located at the intersection of nanophotonics, quantum optics, and chemistry is in its infancy. In this Perspective, we offer our view towards chiral polaritons. We review basic physical concepts underlying chirality of matter and electromagnetic field, discuss the main theoretical and experimental challenges that need to be solved, and consider novel effects that could be enabled by strong coupling between chiral light and matter.

physics.optics↗