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Thomas Unden

Publications and source records attributed to Thomas Unden.

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PIQC: Scalable Distributed Quantum Computing via Photonic Integration of Designed Molecular Quantum Nodes

There is a growing consensus that large-scale, fault-tolerant quantum computing (FTQC) necessitates high-fidelity photonic interconnects to overcome the scaling limits of monolithic architectures. However, most current platforms were not originally designed for native photonic connectivity and require significant engineering overhead. To overcome these fundamental hardware limitations, we recently introduced a rationally designed organic molecule that serves as an ideal quantum node, featuring a robust qubit-photon interface (QPI) and a long-lived nuclear-spin register. In this work, we present PIQC (Photonic Integrated Quantum Circuits), a distributed architecture designed to scale these molecular nodes into a functional quantum computer. The PIQC framework integrates five mutually reinforcing innovations: (i) Designer molecular qubits, i.e. carbene molecules in an isosteric host that provide millisecond-coherence electron spins with high spectral stability and spin-dependent optical emission, (ii) deterministic nuclear registers made of synthetically placed $^{13}$C or $^{14}$N labels that enable fast ($\sim 1~\mu$s), high-fidelity electron-nuclear gates, (iii) hybrid photonic integration, which allows molecular films to seamlessly integrate with existing mature fabrication technologies, e.g. thin-film lithium niobate (TFLN), (iv) heralded entanglement protocols that can tolerate up to 70% photon loss, and (v) stairway Floquetification, i.e. high-rate quantum low-density parity-check (qLDPC) codes that are converted into Floquet codes, reducing syndrome extraction to weight-two Bell-pair measurements that match PIQC's networked hardware. PIQC offers a hardware-efficient, commercially viable pathway toward a utility-scale quantum computer based on distributed FTQC.

quant-ph

A Single-Molecule Spin-Photon Interface

Optical interfaces that connect long-lived spin qubits to photons are a central requirement for quantum networking and distributed quantum information processing. Currently, solid-state atomic defects are leading candidates due to their inherent spin and optical coherence. Building on these advancements, synthetically tailored molecular systems represent a fundamental change in the field, utilizing precise atomic control and consistent bottom-up assembly. However, the lack of a robust spin-photon interface combining bright fluorescence, high spectral stability, and the persistent spin lifetimes inherent to ground-state systems has prohibited the detection of individual molecular qubits. Here we show that a triplet ground state carbene molecule, embedded within a structurally matched host crystal, functions as a robust spin-photon interface with single-molecule addressability. The system exhibits narrow zero-phonon lines, spectral stability over more than an hour, spin-selective optical transitions and single-molecule optically detected magnetic resonance. Coherent control yields millisecond-scale dynamical-decoupling coherence and tens-of-milliseconds spin relaxation at a temperature of 4.5 K. These results establish molecular qubits as a viable platform for single-emitter quantum optics while preserving the advantages of bottom-up chemical design and processable materials.

quant-ph

Hierarchical Maximum Likelihood Estimation for Time-Resolved NMR Data

Metabolic monitoring and reaction rate estimation using hyperpolarized NMR technology requires accurate quantitative analysis of multidimensional data scenarios. Currently, this analysis is often performed in a two-stage procedure, which is prone to errors in uncertainty propagation and estimation. We propose an approach derived from a Bayesian hierarchical model that intrinsically propagates uncertainties and operates on the full data to maximize the precision at minimal uncertainty. In an analytic treatment, we reduce the estimation procedure to a least-squares optimization problem which can be understood as an extension of the Variable Projection (VarPro) approach for data scenarios with two predictors. We investigate the method's efficacy in two experiments with hyperpolarized metabolites recorded with conventional high-field NMR devices and a micronscale NMR setup using Nitrogen-Vacancy centers in diamond for detection, respectively. In both examples, the new approach improves estimates compared to Fourier methods and proves operational advantages over a two-stage procedure employing VarPro. While the approach presented is motivated by NMR analysis, it is straightforwardly applicable to further estimation scenarios with similar data structure, such as time-resolved photospectroscopy.

q-bio.QM

Quantum Memory Enhanced Multipoint Correlation Spectroscopy for Statistically Polarized NMR

Nuclear magnetic resonance spectroscopy with solid-state spin sensors is a promising pathway for the detection of nuclear spins at the micro- and nanoscale. Although many nanoscale experiments rely on a single sensor spin for the detection of the signal, leveraging spin ensembles can enhance sensitivity, particularly in cases in which the signal merely originates from statistically polarized nuclear spins. In this work, we introduce multipoint correlation spectroscopy, that combines the advantages of two well-established methods -- correlation spectroscopy and quantum heterodyne detection -- to enable temporally efficient measurements of statistically polarized samples at the nanoscale with spin ensembles. We present a theoretical framework for this approach and demonstrate an experimental proof of concept with a nitrogen vacancy center in diamond. We achieve single hertz uncertainty in the estimated signal frequency, highlighting the potential applications of the technique for nanoscale nuclear magnetic resonance.

quant-ph

Power-law scaling of correlations in statistically polarised nano-NMR

Diffusion noise is a major source of spectral line broadening in liquid state nano-scale nuclear magnetic resonance with shallow nitrogen-vacancy centres, whose main consequence is a limited spectral resolution. This limitation arises by virtue of the widely accepted assumption that nuclear spin signal correlations decay exponentially in nano-NMR. However, a more accurate analysis of diffusion shows that correlations survive for a longer time due to a power-law scaling, yielding the possibility for improved resolution and altering our understanding of diffusion at the nano-scale. Nevertheless, such behaviour remains to be demonstrated in experiments. Using three different experimental setups and disparate measurement techniques, we present overwhelming evidence of power-law decay of correlations. These result in sharp-peaked spectral lines, for which diffusion broadening need not be a limitation to resolution.

quant-ph

Revealing the emergence of classicality in nitrogen-vacancy centers

The origin of classical reality in our quantum world is a long-standing mystery. Here, we examine a nitrogen vacancy center evolving naturally in the presence of its environment to study quantum Darwinism - the proliferation of information about preferred quantum states throughout the world via the environment. This redundantly imprinted information accounts for the perception of objective reality, as it is independently accessible by many without perturbing the system of interest. To observe the emergence of redundant information, we implement a novel dynamical decoupling scheme that enables the measurement/control of several nuclear spins (the environment E) interacting with a nitrogen vacancy (the system S). In addition to showing how to create entangled SE states relevant to quantum metrology, we demonstrate that under the decoherence of S, redundant information is imprinted onto E, giving rise to classical objectivity - a consensus of the nuclear spins about the state of S. This provides the first laboratory verification of the objective classical world emerging from the underlying quantum substrate.

quant-ph

Coherent control of solid state nuclear spin nano-ensembles

Detecting and controlling nuclear spin nano-ensembles is crucial for the further development of nuclear magnetic resonance (NMR) spectroscopy and for the emerging solid state quantum technology. Here we present the fabrication of a $\approx$ 1 nanometre thick diamond layer consisting of $^{13}$C nuclear spins doped with Nitrogen-Vacancy centres (NV) embedded in a spin-free $^{12}$C crystal matrix. A single NV in the vicinity of the layer is used for polarization of the $^{13}$C spins and the readout of their magnetization. We demonstrate a method for coherent control of few tens of nuclear spins by using radio frequency pulses and show the basic coherent control experiments - Rabi oscillations, Ramsey spectroscopy and Hahn echo, though any NMR pulse sequence can be implemented. The results shown present a first steps towards the realization of a nuclear spin based quantum simulator.

quant-ph

Controllable Non-Markovianity for a Spin Qubit in Diamond

We present a flexible scheme to realize non-artificial non-Markovian dynamics of an electronic spin qubit, using a nitrogen-vacancy center in diamond where the inherent nitrogen spin serves as a regulator of the dynamics. By changing the population of the nitrogen spin, we show that we can smoothly tune the non-Markovianity of the electron spin's dynamic. Furthermore, we examine the decoherence dynamics induced by the spin bath to exclude other sources of non-Markovianity. The amount of collected measurement data is kept at a minimum by employing Bayesian data analysis. This allows for a precise quantification of the parameters involved in the description of the dynamics and a prediction of so far unobserved data points.

quant-ph

Narrow-bandwidth sensing of high-frequency fields with continuous dynamical decoupling

State-of-the-art methods for sensing weak AC fields are only efficient in the low frequency domain (< 10 MHz). The inefficiency of sensing high frequency signals is due to the lack of ability to use dynamical decoupling. In this paper we show that dynamical decoupling can be incorporated into high frequency sensing schemes and by this we demonstrate that the high sensitivity achieved for low frequency can be extended to the whole spectrum. While our scheme is general and suitable to a variety of atomic and solid-state systems, we experimentally demonstrate it with the nitrogen-vacancy center in diamond. For a diamond with natural abundance of $^{13}$C we achieve coherence times up to 1.43 ms resulting in a smallest detectable magnetic field strength of 4 nT at 1.6 GHz. Attributed to the inherent nature of our scheme, we observe an additional increase in coherence time due to the signal itself.

quant-ph

Sub-millihertz magnetic spectroscopy with a nanoscale quantum sensor

Precise timekeeping is critical to metrology, forming the basis by which standards of time, length and fundamental constants are determined. Stable clocks are particularly valuable in spectroscopy as they define the ultimate frequency precision that can be reached. In quantum metrology, where the phase of a qubit is used to detect external fields, the clock stability is defined by the qubit coherence time, which determines the spectral linewidth and frequency precision. Here we demonstrate a quantum sensing protocol where the spectral precision goes beyond the sensor coherence time and is limited by the stability of a classical clock. Using this technique, we observe a precision in frequency estimation scaling in time $T$, as $T^{-3/2}$ for classical oscillating fields. The narrow linewidth magnetometer based on single spins in diamond is used to sense nanoscale magnetic fields with an intrinsic frequency resolution of 607 $\mu$Hz, 8 orders of magnitude narrower than the qubit coherence time.

quant-ph

Autonomous Calibration of Single Spin Qubit Operations

Fully autonomous precise control of qubits is crucial for quantum information processing, quantum communication, and quantum sensing applications. It requires minimal human intervention on the ability to model, to predict and to anticipate the quantum dynamics [1,2], as well as to precisely control and calibrate single qubit operations. Here, we demonstrate single qubit autonomous calibrations via closed-loop optimisations of electron spin quantum operations in diamond. The operations are examined by quantum state and process tomographic measurements at room temperature, and their performances against systematic errors are iteratively rectified by an optimal pulse engineering algorithm. We achieve an autonomous calibrated fidelity up to 1.00 on a time scale of minutes for a spin population inversion and up to 0.98 on a time scale of hours for a Hadamard gate within the experimental error of 2%. These results manifest a full potential for versatile quantum nanotechnologies.

quant-ph

Protecting a nuclear spin from a noisy electron spin in diamond

Although a nuclear spin is weakly coupled to its environment, due to its small gyromagnetic ratio, its coherence time is limited by the hyperfine coupling to a nearby noisy electron. Here, we propose to utilize continuous dynamical decoupling to refocus the coupling to the electron. If the random phase accumulated by the nuclear spin through the reduced coupling terms is sufficient small, we can increase the nuclear coherence time. Initially, we demonstrate this on a simple case with a two-level electron spin, while taking all relevant hyperfine coupling terms and noise terms into account. We then extend the analysis to a nitrogen-vacancy center in diamond having a three level structure.

quant-ph

Qudi: a modular python suite for experiment control and data processing

Qudi is a general, modular, multi-operating system suite written in Python 3 for controlling laboratory experiments. It provides a structured environment by separating functionality into hardware abstraction, experiment logic and user interface layers. The core feature set comprises a graphical user interface, live data visualization, distributed execution over networks, rapid prototyping via Jupyter notebooks, configuration management, and data recording. Currently, the included modules are focused on confocal microscopy, quantum optics and quantum information experiments, but an expansion into other fields is possible and encouraged. Qudi is available from https://github.com/Ulm-IQO/qudi and is freely useable under the GNU General Public Licence.

quant-ph

Quantum metrology enhanced by repetitive quantum error correction

The accumulation of quantum phase in response to a signal is the central mechanism of quantum sensing, as such, loss of phase information presents a fundamental limitation. For this reason approaches to extend quantum coherence in the presence of noise are actively being explored. Here we experimentally protect a room-temperature hybrid spin register against environmental decoherence by performing repeated quantum error correction whilst maintaining sensitivity to signal fields. We use a long-lived nuclear spin to correct multiple phase errors on a sensitive electron spin in diamond and realize magnetic field sensing beyond the timescales set by natural decoherence. The universal extension of sensing time, robust to noise at any frequency, demonstrates the definitive advantage entangled multi-qubit systems provide for quantum sensing and offers an important complement to quantum control techniques. In particular, our work opens the door for detecting minute signals in the presence of high frequency noise, where standard protocols reach their limits.

quant-ph