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Kai Müller

Publications and source records attributed to Kai Müller.

At least 19 recordsLinked to original sources

Dual-Trigger of Series Nanowire Detector for Event-Based Photon Number Assignment

Photon-number-resolving (PNR) detectors are essential components of photonic quantum technologies. However, conventional single-channel edge-triggered readout struggles to resolve the photon number $n$ in real time or to characterize how timing jitter depends on $n$. In this work, we use a dual-trigger method on a three-pixel series-connected superconducting nanowire single-photon detector (SNSPD) that triggers on both the rising and falling edges of the detection pulse. By doing so, we preserve the precise arrival time of the detection event while mapping the photon number onto the time interval between the rising and falling edges, allowing clear separation of the events. Using this technique, we assign each detection event to $n = 1, 2,$ or 3 photons with $99\,\%$ posterior confidence across all three classes. The timing jitter decreases as $n$ increases, reaching values below $41\, \text{ps}$ for $n \geq 2$. Comparing edge-triggering with constant-fraction discrimination (CFD) for arrival-time extraction, we find that CFD yields lower jitter for single-photon events and a nearly constant mean arrival time. Altogether, our results establish dual-triggering as a robust, low-latency readout scheme for PNR detectors, while revealing a photon-number dependence of the timing jitter relevant to timing precision achievable in heralded photonic quantum applications.

quant-ph

Temperature-Dependent Emission Spectroscopy of Quantum Emitters in Hexagonal Boron Nitride

Color centers in hexagonal boron nitride (hBN) have attracted significant interest due to their potential applications in future optical quantum technologies. For most applications, scalable on-demand fabrication is a key requirement. Recent advances using localized electron irradiation have demonstrated near-identical emitters in the blue and yellow spectral regions. While the blue emitters have been demonstrated in cryogenic temperatures, the yellow emitters remain uncharacterized under such conditions. In this work, we therefore extended the study of yellow emitters to cryogenic temperatures. Initially, multiple spectral features were observed, prompting a systematic investigation that led to the identification of a defect emission centered around 547.5 nm with high brightness and excellent photostability. By tuning the excitation wavelength, we are able to distinguish Raman scattering peaks from the emitter emission. Further analysis of the vibronic emissions allowed us to identify an optical phonon mode, whose contribution becomes increasingly dominant at elevated temperatures. Photoluminescence excitation spectroscopy (PLE) reveals excitation through this phonon mode enhances the emission by almost 5-fold in cryogenic temperature. Temperature-dependent studies further elucidate the role of phonons in the emission process. These observations deepen our understanding of the nature of the emitters, opening new avenues for precise tuning of quantum light sources.

physics.optics

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

Tunable g-Factors of Hybridized Orbitals in a Quantum Dot Molecule

The ability to control the $g$-factors of orbital spin states in optically active quantum dot molecules (QDMs) is a prerequisite for the high-fidelity generation of multi-photonic cluster states with higher-dimensional entanglement structure. Protocols that rely on two coupled spins require knowledge of the $g$-factor and its dependence on external control parameters. Mismatches in the $g$-factor between tunnel-coupled dots introduce unwanted dephasing of coupled spin-states, making precise characterization and voltage control essential. Here, we measure the gate voltage dependence of the electron and hole $g$-factors of negatively charged trions $X^{-}$ in a single InGaAs QDM using polarization-resolved magneto-photoluminescence spectroscopy. The electron $g$-factor exhibits a pronounced step-like change at the tunneling resonance, shifting from $g_\mathrm{e} = -0.336\pm 0.008$ to $g_\mathrm{e} = -0.389\pm 0.003$, providing a direct spectroscopic fingerprint of molecular orbital formation and a shift of the wavefunction localization from the lower to the upper dot. In contrast, the hole $g$-factor remains nearly constant at $g_\mathrm{h} \approx 0.094 \pm 0.007$, exhibiting a weak modulation near the anticrossing voltages attributed to Coulomb-mediated deformation of the wavefunction by the tunneling electron. Our results are quantitatively reproduced by an eight-band $\mathbf{k}{\cdot}\mathbf{p}$ model, establishing electric-field control of the trion $g$-factors as a practical tool for independently tuning the Zeeman splitting of individual dots and opening new pathways towards the deterministic generation of two-dimensional photonic cluster states.

cond-mat.mes-hall

On-site interactions in quantum thermal machines: efficiency, rectification and entanglement beyond local and global master equations

Advances in experimental techniques have opened new routes for harnessing non-equilibrium dynamics in mesoscopic quantum systems. In this context, we study the impact of on-site interactions on the transport properties of a continuous quantum thermal machine composed of two coupled oscillators connected to two thermal reservoirs. In the weak system-reservoir coupling regime, where a long-standing debate concerns which reduced description should be preferred, we first show that the Redfield master equation (RME) provides an accurate and unifying framework that interpolates between two well-known limits: the \textit{local} and \textit{global} master equations. By relying on the Hierarchy of Pure States (HOPS), a numerically exact stochastic method, we then explore the full parameter space and show that interactions can be leveraged to tune the efficiency of the thermal machine at high temperatures (while leaving it essentially unchanged at low temperatures), induce non-reciprocal transport under asymmetric reservoir couplings, and generate steady-state entanglement within the junction. We derive expressions for system-bath correlators, such as heat and particle currents, consistently across different frameworks. Our work features on-site interactions to enhance the versatility of quantum thermodynamic junctions and clarifies the role of non-Markovianity and non-linearities in quantum transport.

quant-ph

Fibonacci Steady-States and Persistent Oscillations in an Ordered Multimode Dicke Model

Ultracold atoms in multimode optical cavities provide a rich testbed for many-body phenomena enabled by light-mediated interactions. Recent experiments include realizations of spin glasses and associative memories, as described by multimode Dicke models with disordered couplings. However, the properties of multimode Dicke models with ordered coupling geometries remain largely unexplored. In this work, we investigate the stable steady-states of the multimode Dicke model with an ordered nearest-neighbor coupling geometry, where $n_c$ atomic clusters are coupled via $n_c-1$ cavity modes. We show that the number of mean-field stable steady-states in the superradiant phase exhibits Fibonacci scaling with the number of atomic clusters, and that a subset of these steady-states exhibit persistent oscillations. Using both the truncated Wigner approximation and the numerically-exact hierarchy of pure states, we further demonstrate that these features of the stable steady-state solutions persist for finite cluster sizes. Ordered multimode Dicke models, such as the nearest-neighbor coupling geometry considered here, are accessible with current experimental technologies and point toward a broader class of strongly interacting dissipative systems with similarly rich behavior.

quant-ph

Optical probing of phononic properties of a tin-vacancy color center in diamond

The coherence characteristics of a tin-vacancy color center (SnV) in diamond are investigated through optical means, including linewidth broadening effects and coherent population trapping (CPT) between the ground state orbital levels. Spectral analysis is required as due to the large spin-orbit splitting of the orbital ground states, thermalization between the ground states occurs at rates that are impractical to measure directly in the time domain. First, by implementing a temperature-dependent linewidth broadening measurement, including the challenging-to-measure D transition, phononic coupling coefficients are determined. These measurements are performed on an emitter with a lifetime-limited linewidth and atom-like properties, making the measurement representative for high-quality SnVs. Next, a CPT-type experiment is carried out to independently analyze thermal decoherence processes at 4 K. The spectral information is transformed into its conjugate variable time, providing picosecond resolution and revealing an orbital depolarization timescale of ${\sim30{\rm~ps}}$. Consequences of the investigated dynamics are then used to estimate spin dephasing times limited by thermal effects.

quant-ph

Impact of Stoichiometry of MoSi Thin Films for Enhanced Sensitivity of Superconducting Nanowire Single-Photon Detectors

We report on the impact of the stoichiometry of superconducting MoSi thin films on the performance of superconducting nanowire single-photon detectors (SNSPDs). Specifically, we investigate the relation between the film parameters critical temperature Tc , sheet resistance Rs and superconductor thickness d and observe a universal scaling behavior. To benchmark the performance of SNSPDs fabricated from films having different stoichiometry, we measure the bias dependent count rate curves, while the detector is illuminated with wavelengths between 780 nm and 1550 nm. The detector performance as a function photon energy for different nanowire widths reveals a linear relation between the detection current and the photon energy. Furthermore, we determine the interfacial thermal boundary conductance $β$ between the superconducting thin film and the substrate, by measuring the return current of the SNSPD and find an increase of $β$ with increasing Mo concentration. The highest sensitivity amongst all compared devices is achieved for Mo$_{0.53}$Si$_{0.47}$, with low Tc (4.1 K) and high Rs (397$Ω$/sq) at a film thickness of 5.4 nm.

cond-mat.supr-con

One-to-one correspondence between Hierarchical Equations of Motion and Pseudomodes for Open Quantum System Dynamics

We unite two of the most widely used approaches for strongly damped, non-Markovian open quantum dynamics, the Hierarchical Equations of Motion (HEOM) and the pseudomode method by proving two statements: First, every physical bath correlation function (BCF) that can be written as a sum of $N$ exponential terms can be obtained from a physical model with $N$ interacting pseudomodes which are damped in Lindblad form. Second, for every such BCF there exists a non-unitary, linear transformation which mirrors the evolution of the system-pseudomode state onto the HEOM hierarchy, and vice versa. Our proofs are constructive and we give explicit expressions for the mirror transformation as well as for the pseudomode Lindbladian corresponding to a given exponential BCF. This approach also gives insight and provides elegant derivations of the corresponding Hierarchy of stochastic Pure States (HOPS) method and its nearly-unitary version, nuHOPS. Our result opens several avenues for further optimization of non-Markovian open quantum system dynamics methods.

quant-ph

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

Molecular beam epitaxy of wafer-scale O-band InAs/InGaAs quantum dots on GaAs for quantum photonics

We report a scalable molecular beam epitaxy strategy to achieve a low density of O-band electrically tunable InAs/InGaAs quantum dots (QDs) on GaAs(001) substrates. Our approach is based on a gradient deposition of InAs in the sub-ML regime and subsequent capping with an InGaA strain-reducing layer to redshift the emission wavelength. For different growth conditions, we investigate the optical properties of the dots using photoluminescence mapping and correlate with structural properties determined by scanning transmission electron microscopy. Using a surface roughness modulation technique and synchronizing InAs sub-monolayer deposition cycles with substrate rotation, we control the dot density and position low-density regions (< 1 QD per um^2) on the substrate. Hyperspectral imaging is used to map the spatial and spectral characteristics of many individual dots in the low-density region, confirming that our approach is universally applicable to conventional MBE growth on (001) surfaces. Finally, we tune the QD emission wavelength within the O-band using electric fields and demonstrate single-photon emission with g(2)(0) = 0.020(14).

cond-mat.mtrl-sci

Ultra-slow orbital and spin dynamics in an electrically tunable quantum dot molecule

Tunnel-coupled optically active quantum dot molecules (QDMs), have the potential to operate as spin-photon-interfaces with coupled spins that interact with two different photon frequencies at the same time. A prerequisite is to deterministically prepare two (electron or hole) spins in the QDM and be able to electrically tune the orbital state couplings. Here, we demonstrate the sequential optical charging of a single QDM with two electron spins while simultaneously maintaining the ability to widely tune orbital couplings using static electric fields and optically drive the system for quantum light generation. We optically prepare one- and two-spin states, initialize via optical pumping and explore orbital and spin relaxation dynamics for one and two-spin states as a function of the energy detuning and hybridization of orbital states. For two-spin states, remarkably long S-T relaxation times are observed extending beyond $\sim 100μs$ with strong dependence on the relative energy of ground and excited two-spin states. Qualitative agreement is observed with $\mathbf{k \cdot p}$ calculations of phonon-mediated spin-relaxation. Our results provide new quantitative understanding of the dynamics of one and two-spin states and confirm their suitability of QDMs for creating multidimensional photonic cluster states by exploiting tunable spin-spin exchange couplings at zero magnetic fields combined with optical driving.

cond-mat.mes-hall

Practical quantum tokens: challenges and perspectives

The concept of quantum tokens dates back alongside quantum cryptography to Stephen Wiesner's seminal work in 1983[1]. Already this initial work proposes society-relevant applications such as secure quantum banknotes, which can be exchanged between a bank and a customer. This quantum currency is based on various physical states that can be easily verified but is protected from being copied by the fundamental quantum laws. Four decades later, these ideas have flourished in the field of quantum information, and the concept of quantum banknotes has not only adopted many varying names, such as quantum money, quantum coins, quantum-digital payments, and quantum tokens, but also reached its first experimental demonstrations. In this perspective article, we discuss the current state-of-the-art of quantum tokens in the field of quantum information, as well as their future perspectives. We present a number of physical realizations of quantum tokens with integrated quantum memories and their applicability scenarios in detail. Finally, we discuss how quantum tokens fit into the information security ecosystem and consider their relationship to post-quantum cryptography.

quant-ph

Optical Spectroscopy of Waveguide coupled Er$^{3+}$ ensembles in CaWO$_4$ and YVO$_4$

We present an optical study of near-surface Er$^{3+}$ ensembles in waveguide-integrated CaWO$_4$ and YVO$_4$, investigating how nanophotonic coupling modifies rare-earth spectroscopy. In particular, we compare bulk excitation with evanescently coupled TE and TM waveguide modes. In Er$^{3+}$:CaWO$_4$, we observe a pronounced polarization-dependent surface effect. TE-coupled spectra closely reproduce bulk behavior. In contrast, TM coupling induces strong inhomogeneous broadening and an asymmetric low-energy shoulder of the site S1 Y1Z1 transition, with linewidths exceeding those of the bulk by more than a factor of four. Temperature-dependent measurements and surface termination studies indicate that surface charges are the dominant mechanism. Er$^{3+}$:YVO$_4$ remains largely unaffected by mode polarization, and surface termination leads only to minor spectral shifts. These observations suggest that non-charge-neutral rare-earth systems are more susceptible to surface-induced decoherence sources than charge-neutral hosts.

cond-mat.mtrl-sci

Mitigating the Transition of SiV$^-$ in Diamond to an Optically Dark State

Negatively charged silicon vacancy centers in diamond (SiV$^-$) are promising for quantum photonic technologies. However, when subject to resonant optical excitation, they can inadvertently transfer into a zero-spin optically dark state. We show that this unwanted change of charge state can be quickly reversed by the resonant laser itself in combination with static electric fields. By defining interdigitated metallic contacts on the diamond surface, we increase the steady-state SiV$^-$ photoluminescence under resonant excitation by a factor $\ge3$ for most emitters, making it practically constant for certain individual emitters. We electrically activate single \sivs near the positively biased electrode, which are entirely dark without applying local electric fields. Using time-resolved 3-color experiments, we show that the resonant laser not only excites the SiV$^-$, but also creates free holes that convert SiV$^{2-}$ to SiV$^-$ on a timescale of milliseconds. Through analysis of several individual emitters, our results show that the degree of electrical charge state controllability differs between individual emitters, indicating that their local environment plays a key role. Our proposed electric-field-based stabilization scheme enhances deterministic charge state control in group-IV color centers and improves its understanding, offering a scalable path toward quantum applications such as entanglement generation and quantum key distribution.

quant-ph

Inverse-Designed Grating Couplers with Tunable Wavelength via Scaling and Biasing

Photonic integrated circuits are heavily researched devices for telecommunication, biosensing, and quantum technologies. Wafer-scale fabrication and testing are crucial for reducing costs and enabling large-scale deployment. Grating couplers allow non-invasive measurements before packaging, but classical designs rely on long tapers and narrow bandwidths. In this work, we present compact, inverse-designed grating couplers with broadband transmission. We optimized and fabricated arrays of devices and characterized them with a 4f-scanning setup. The nominal design reached simulated efficiencies of 52 %, while measurements confirmed robust performance with up to 32 % efficiency at the target 1540 nm wavelength and 46 % at shifted wavelengths. Without scaling and contour biasing, the measured efficiency at the target wavelength drops to only 4.4 %. Thus, a key finding is that systematic scaling and edge biasing recover up to an eightfold improvement in efficiency. These inverse-designed grating couplers can be efficiently corrected post-design, enabling reliable performance despite fabrication deviations. This approach allows simple layout adjustments to compensate for process-induced variations, supporting wafer-scale testing, cryogenic photonic applications, and rapid design wavelength tuning.

physics.optics

Second-order Stark shifts exceeding 10$\,$GHz in electrically contacted SiV$^-$ centers in diamond

Negatively charged silicon vacancy centers (SiV$^-$) in diamond exhibit excellent spin coherence and optical properties, making them promising candidates for quantum technologies. However, the strain-induced inhomogeneous distribution of optical transition frequencies poses a challenge for scalability. We demonstrate electrical tuning of the SiV$^-$ center zero-phonon lines using in-plane contacts to apply moderate electric fields up to 45$\,$MV/m. The second-order Stark shift exceeds 10$\,$GHz, which is of the same order of magnitude as the 15$\,$GHz inhomogeneous distribution of SiV$^-$ observed in emitters embedded in optical nanostructures such as photonic crystal nanocavities. Analysis of individual SiV$^-$ centers shows significant variation in polarizabilities between defects indicating that the polarizability strongly depends on local parameters like strain. The observed polarizabilities are 3-25 times larger than those of tin vacancy centers, which we attribute to valence band resonances that delocalize the $e_u$ wavefunctions. Photoluminescence excitation measurements reveal that optical linewidths increase moderately with applied electric field strength. Our results demonstrate that large electrical Stark shifts can overcome the inhomogeneous distribution of transition frequencies, representing a significant step toward scalable SiV$^-$-based quantum technologies such as quantum repeaters.

quant-ph

Zeeman Spectroscopy of Vacancy-Charge-Compensated Er3+ Sites in CaWO4 under Vector Magnetic Fields

We present polarization-resolved optical absorption measurements on Er3+ ions in CaWO4 under vector magnetic fields, focusing on charge-compensated sites arising from local Ca2+ vacancies. While the known axial Er3+ site displays a single symmetric Zeeman-split transition pattern consistent with S4 symmetry, two additional sites exhibit more complex spectral behavior, including sets of transitions that interchange under 90° crystal rotations-evidence of reduced, rhombic-like symmetry. From these polarization- and temperature-dependent spectra, we extract effective g-factors. Our findings are corroborated by electron paramagnetic resonance measurements and support a model of multiple inequivalent Ca2+ vacancies around Er3+ sites in the host lattice. This detailed characterization contributes to understanding defect-engineered rare-earth sites for quantum information applications.

cond-mat.mtrl-sci