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F. Joseph Heremans

Publications and source records attributed to F. Joseph Heremans.

At least 19 recordsLinked to original sources

A Si-on-SiC Platform for Interfacing with Vanadium Dopants in the Telecom O-Band

Vanadium color centers in silicon carbide (SiC) offer telecom O-band emission, sub-microsecond optical lifetimes, and second-scale spin relaxation times, rendering them promising candidates for quantum network nodes. However, efficient photon extraction from the high-refractive-index SiC host remains challenging. Here, we introduce a silicon-on-SiC heterogeneous photonic platform in which silicon nanocavities evanescently couple to shallow vanadium dopants in commercial 4H-SiC, enabling efficient zero-phonon line (ZPL) collection under resonant excitation. In as-grown ensembles, we observe Purcell-enhanced photoluminescence with transient spectral hole burning linewidths of 50 MHz on microsecond timescales. In dilute implanted samples, we isolate individual vanadium centers with high-purity single photon emission and a Purcell-enhanced lifetime of 109 ns. The entire optical interface operates through a single lensed fiber, including a 905 nm repump laser that recovers the vanadium charge state with 95% efficiency. These results establish Si-on-SiC as a scalable, foundry-compatible platform for telecom-wavelength spin-photon interfaces.

cond-mat.mtrl-sci↗

Optical decoherence in Er$^{3+}$-doped CeO$_2$ spin qubit platforms

Erbium ions (Er$^{3+}$) in cerium dioxide (CeO$_2$) represent a promising spin-photon interface for quantum communication, but the mechanisms limiting their optical coherence remain poorly understood. Using periodic hybrid density functional theory calculations with finite-size corrections, we identify Ce$^{3+}$ polarons and their complexes with oxygen vacancies and Er$^{3+}$ dopants as likely sources of optical decoherence. These defects exhibit finite photoionization cross-sections at 0.8 eV, coinciding with both the laser excitation energy used experimentally and the emission energy of Er$^{3+}$. This resonance enables photoionization of the polarons and photoluminescence quenching of Er$^{3+}$, leading to the broadening of optical linewidths, shortening of excited-state lifetimes, and introduction of charge noise. Our concentration-dependent photocurrent measurements in Er$^{3+}$-doped CeO$_2$ films under 0.8 eV illumination validate the predicted decoherence pathway. Our combined computational and experimental results identify a concrete defect-engineering target for improving the Er$^{3+}$-doped CeO$_2$ platform, and point to a decoherence mechanism likely relevant to other Er$^{3+}$-doped multivalent-oxide quantum platforms.

cond-mat.mtrl-sci↗

Minute-long quantum coherence enabled by electrical depletion of magnetic noise

Integrating solid-state spin defects into classical electronic devices can enable new opportunities for quantum information processing that benefit from existing semiconductor technology. Here, we investigate the impact of bias control of an isotopically purified silicon carbide (SiC) p-i-n diode on the coherence of embedded spins. We show that the diode allows for the depletion of not only the electrical, but also the magnetic noise sources. This results in extended relaxation and coherence times of individual electronic and nuclear spins, with Hahn echo times exceeding values reported for single spins in any platform (> 100 seconds). These results demonstrate the importance of materials control and electronic device integration to create highly coherent solid-state quantum technology.

quant-ph↗

A nanoscale magnetic spectrum analyzer based on qubit dressed states

Magnetic field fluctuations on nanometer length scales manifest in a diverse range of phenomena -- electron and spin dynamics in materials and devices, quantum many-body systems, and molecular chemistry. Measuring these phenomena requires sensors with a challenging combination of broad spectral bandwidth, high sensitivity, and nanoscale spatial resolution. Nitrogen-vacancy (NV) centers, atom-like quantum sensors in diamond, possess the requisite sensitivity and nanoscale sensing volume, but are typically limited in bandwidth by the practical speed of the applied quantum control sequence. Here, we overcome this limitation by exposing the NV qubit to a microwave dressing field during a dynamical decoupling sequence, which both amplifies and frequency-mixes target signals at arbitrary frequencies into the detection band of the dynamical decoupling protocol. We demonstrate this approach by using NV centers to detect both coherent and noisy nanoscale spin wave dynamics in a magnetic yttrium-iron-garnet (YIG) thin film over a broad frequency range. Our technique generalizes to other qubit platforms, providing a versatile framework for nanoscale spectroscopy across diverse physical and chemical systems.

cond-mat.mes-hall↗

Spin Dynamics from Atomistic Quantum Simulations

Optically active solid-state spin defects are promising candidates for quantum applications, however a unified theoretical framework to predict their spin dynamics at high temperatures is not yet available. Here, using Kubo linear--response theory, we derive expressions of spin-lattice and decoherence times \(T_1\) and \(T_2\) in terms of correlation functions of spin--lattice couplings. We then evaluate \(T_1\) and \(T_2\) from molecular dynamics and spin--lattice interaction time--series generated by state--of--the--art machine learning models trained on {\it ab--initio} data. Finally we measure \(T_1\) times for the NV center in diamond and compare experimental and theoretical results, showing excellent agreement.

cond-mat.mtrl-sci↗

The Role of Defect Geometry in Localized Emission from Monolayer Tungsten Dichalcogenides

Understanding the mechanism of single photon emission (SPE) in two-dimensional (2D) material is an unsolved problem important for quantum optical materials and the development of quantum information applications. In 2D transition metal dichalcogenides (TMDs) such as tungsten diselenide (WSe2), quantum emission has been broadly attributed to exciton localization from atomic point defects, yet the precise microscopic origins are not fully understood. This work introduces an empirically grounded computational framework that explains both the origins of facile SPE in WSe2 and its relative scarcity in related TMD, tungsten disulfide. High resolution microscopy identifies native defect geometries existing in monolayer WSe2 lattices providing the ingredients necessary to build a realistic model. The qualitative effects of chalcogen type, defect geometry, and mechanical strain on the electronic structure are then individually assessed using density functional theory, from which a specific divacancy configuration emerges as the candidate for localized single-electron transitions that match observed spectral energies. Spectroscopy and photon correlation measurements further validate this model, establishing a self-consistent link between defect geometry, electronic structure, and quantum emission. By isolating the distinct roles of chalcogen type, defect configuration, and mechanical strain, this work provides a thorough investigation of exciton localization and optical behavior, contributing to a clearer picture of the physical drivers of single photon emission in tungsten-based TMDs.

cond-mat.mtrl-sci↗

Heterogeneously Integrated Diamond-on-Lithium Niobate Quantum Photonic Platform

Diamond photonics has enabled efficient interfaces for quantum memories and is predicted to be a critical component of quantum networks. However, scalable network architectures require spatial, temporal, and spectral control of photons, which relies on nonlinear and electro-optic functionalities that diamond alone cannot provide. Here, we demonstrate heterogeneous integration of a thin-film lithium niobate (TFLN) platform, which has strong chi-2 nonlinearity and electro-optic effects, with thin diamond films. We demonstrate high-Q diamond photonic crystal cavities (Q factors exceeding 5x10^4 at 735 nm) that are lithographically aligned with TFLN photonic backbone and critically coupled to it. This allows us to realize low-loss diamond-TFLN "escalators" (loss ~1 dB/coupler) that support efficient light transfer between them. At cryogenic temperatures (5K), we can collect photons emitted from silicon vacancies (SiVs) embedded within the diamond structure via the TFLN photonic circuit. This approach establishes a scalable route toward integrated photonic circuits for practical quantum networking and other technologies.

physics.optics↗

Valley Splitting Correlations Across a Silicon Quantum Well Containing Germanium

Quantum dots in SiGe/Si/SiGe heterostructures host coherent electron spin qubits, which are promising for future quantum computers. The silicon quantum well hosts near-degenerate electron valley states, creating a low-lying excited state that is known to reduce spin qubit readout and control fidelity. The valley energy splitting is dominated by the microscopic disorder in the SiGe alloy and at the Si/SiGe interfaces, and while Si devices are compatible with large-scale semiconductor manufacturing, achieving a uniformly large valley splitting energy across a many-qubit device spanning mesoscopic distances is an outstanding challenge. In this work we study valley splitting variations in a 1D quantum dot array, formed in a Si$_{0.972}$Ge$_{0.028}$ quantum well, manufactured by Intel. We observe correlations in valley splitting, at both sub-100nm (single gate) and >1$μ$m (device) lengthscales, that are consistent with alloy disorder-dominated theory and simulation. Our results develop the mesoscopic understanding of Si/SiGe heterostructures necessary for scalable device design.

cond-mat.mes-hall↗

Spin decoherence dynamics of Er$^{3+}$ in CeO$_2$ film

Developing telecom-compatible spin-photon interfaces is essential towards scalable quantum networks. Erbium ions (Er$^{3+}$) exhibit a unique combination of a telecom (1.5 $μ$m) optical transition and an effective spin-$1/2$ ground state, but identifying a host that enables heterogeneous device integration while preserving long optical and spin coherence remains an open challenge. We explore a new platform of Er$^{3+}$:CeO$_2$ films on silicon, offering low nuclear spin density and the potential for on-chip integration. We demonstrate a 38.8 $μ$s spin coherence, which can be extended to 176.4\nobreakspace $μ$s with dynamical decoupling. Pairing experiments with cluster correlation expansion calculations, we identify spectral diffusion-induced Er$^{3+}$ spin flips as the dominant decoherence mechanism and provide pathways to millisecond-scale coherence.

quant-ph↗

First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation

Optically active spin defects in solids are promising platforms for quantum technologies. Here, we present a first-principles framework to investigate intersystem crossing processes, which represent crucial steps in the optical spin-polarization cycle used to address spin defects. Considering the nitrogen-vacancy center in diamond as a case study, we demonstrate that our framework effectively captures electron correlation effects in the calculation of many-body electronic states and their spin-orbit coupling and electron-phonon interactions, while systematically addressing finite-size effects. We validate our predictions by carrying out measurements of fluorescence lifetimes, finding excellent agreement between theory and experiments. The framework presented here provides a versatile and robust tool for exploring the optical cycle of varied spin defects entirely from first principles.

cond-mat.mtrl-sci↗

High-throughput spin-bath characterization of spin-defects in semiconductors

Detailed knowledge of the local environments of spin-defects in semiconductors, such as nitrogen vacancy (NV) centers in diamond or divacancies in silicon carbide, is crucial for optimizing control and entanglement protocols in quantum sensing and information applications. However, a direct experimental characterization of individual defect environments is not scalable, as spin bath measurements are extremely time consuming. In this work, we address the ill-posed inverse problem of recovering the atomic positions and hyperfine couplings of random nuclei surrounding spin-defects from sparse experimental coherence signals, which can be obtained in hours. To address the challenge to determine the number of isotopic nuclear spins along with their hyperfine couplings, we employ a trans-dimensional Bayesian approach that incorporates ab initio data. This approach provides posterior distributions of the numbers, hyperfine couplings, and locations of nuclear spins present in the sample. In addition to enabling high-throughput screening of spin-defects, we demonstrate how this trans-dimensional Bayesian approach can guide experimental design for dynamical decoupling experiments to detect nuclear spins within targeted hyperfine coupling regimes. While the primary focus is on accelerating spin-defect characterization, this Bayesian approach also lays the foundation for digital twin studies of spin-defects, where a virtual model of the spin-defect system evolves in real time with ongoing experimental measurements. Together, the set of tools we designed and applied paves the way for scalable deployment of spin-defects in semiconductors for quantum sensing and information applications.

quant-ph↗

Emergent anisotropic three-phase order in critically doped superconducting diamond films

Two decades since its discovery, superconducting heavily boron-doped diamond (HBDD) still presents unresolved fundamental questions whose resolution is relevant to the development of this material for quantum technologies. We use electrical magnetotransport measurements of critically-doped homoepitaxial single crystal HBDD films to reveal signatures of intrinsic (electronic) granular superconductivity. By studying the dependence of electrical resistivity on temperature and magnetic field vector, we infer that this granularity arises from electron correlations. This is revealed by a striking three-phase anisotropy in the magnetoresistance, accompanied by a spontaneous transverse voltage (Hall anomaly). Our findings indicate an emergent magnetically tunable intrinsic order in an otherwise isotropic three dimensional single crystal HBDD film, offering new insights into the mechanism of superconductivity in this quantum material.

cond-mat.supr-con↗

Atomic-scale imaging and charge state manipulation of NV centers by scanning tunneling microscopy

Nitrogen-vacancy (NV) centers in diamond are among the most promising solid-state qubit candidates, owing to their exceptionally long spin coherence times, efficient spin-photon coupling, room-temperature operation, and steadily advancing fabrication and integration techniques. Despite significant progress in the field, atomic-scale characterization and control of individual NV centers have remained elusive. In this work, we present a novel approach utilizing a conductive graphene capping layer to enable direct imaging and manipulation of $NV^{-}$ defects via scanning tunneling microscopy (STM). By investigating over 40 individual $NV^{-}$ centers, we identify their spectroscopic signatures and spatial configurations. Our dI/dV conductance spectra reveal the ground state approximately 300 meV below the Fermi level. Additionally, density-of-states mapping uncovers a two-lobed wavefunction aligned along the [111] crystallographic direction. Remarkably, we demonstrate the ability to manipulate the charge state of the NV centers from $NV^{-}$ to $NV^{0}$ through STM tip-induced gating. This work represents a significant advancement in the atomic-scale understanding and engineering of NV centers, paving the way for future quantum device development.

quant-ph↗

Purcell-enhanced emissions from diamond color centers in slow light photonic crystal waveguides

Quantum memories based on emitters with optically addressable spins rely on efficient photonic interfaces, often implemented as nanophotonic cavities with ideally narrow spectral linewidths and small mode volumes. However, these approaches require nearly perfect spectral and spatial overlap between the cavity mode and quantum emitter, which can be challenging. This is especially true in the case of solid-state quantum emitters that are often randomly positioned and can suffer from significant inhomogeneous broadening. An alternative approach to mitigate these challenges is to use slow-light waveguides that can enhance light-matter interaction across large optical bandwidths and large areas. Here, we demonstrate diamond slow light photonic crystal (PhC) waveguides that enable broadband optical coupling to embedded silicon-vacancy (SiV) color centers. We take advantage of the recently demonstrated thin-film diamond photonic platform to fabricate fully suspended two-dimensional PhC waveguides. Using this approach, we demonstrate waveguide modes with high group indices up to 70 and observe Purcell-enhanced emissions of the SiVs coupled to the waveguide mode. Our approach represents a practical diamond platform for robust spin-photon interfaces with color centers.

quant-ph↗

Nuclear Spin Engineering for Quantum Information Science

Semiconductors are the backbone of modern technology, garnering decades of investment in high quality materials and devices. Electron spin systems in semiconductors, including atomic defects and quantum dots, have been demonstrated in the last two decades to host quantum coherent spin qubits, often with coherent spin-photon interfaces and proximal nuclear spins. These systems are at the center of developing quantum technology. However, new material challenges arise when considering the isotopic composition of host and qubit systems. The isotopic composition governs the nature and concentration of nuclear spins, which naturally occur in leading host materials. These spins generate magnetic noise -- detrimental to qubit coherence -- but also show promise as local quantum memories and processors, necessitating careful engineering dependent on the targeted application. Reviewing recent experimental and theoretical progress towards understanding local nuclear spin environments in semiconductors, we show this aspect of material engineering as critical to quantum information technology.

quant-ph↗

Practical hybrid PQC-QKD protocols with enhanced security and performance

Quantum resistance is vital for emerging cryptographic systems as quantum technologies continue to advance towards large-scale, fault-tolerant quantum computers. Resistance may be offered by quantum key distribution (QKD), which provides information-theoretic security using quantum states of photons, but may be limited by transmission loss at long distances. An alternative approach uses classical means and is conjectured to be resistant to quantum attacks, so-called post-quantum cryptography (PQC), but it is yet to be rigorously proven, and its current implementations are computationally expensive. To overcome the security and performance challenges present in each, here we develop hybrid protocols by which QKD and PQC inter-operate within a joint quantum-classical network. In particular, we consider different hybrid designs that may offer enhanced speed and/or security over the individual performance of either approach. Furthermore, we present a method for analyzing the security of hybrid protocols in key distribution networks. Our hybrid approach paves the way for joint quantum-classical communication networks, which leverage the advantages of both QKD and PQC and can be tailored to the requirements of various practical networks.

quant-ph↗

Towards efficient and secure quantum-classical communication networks

The rapid advancement of quantum technologies calls for the design and deployment of quantum-safe cryptographic protocols and communication networks. There are two primary approaches to achieving quantum-resistant security: quantum key distribution (QKD) and post-quantum cryptography (PQC). While each offers unique advantages, both have drawbacks in practical implementation. In this work, we introduce the pros and cons of these protocols and explore how they can be combined to achieve a higher level of security and/or improved performance in key distribution. We hope our discussion inspires further research into the design of hybrid cryptographic protocols for quantum-classical communication networks.

quant-ph↗

Quantifying the limits of controllability for the nitrogen-vacancy electron spin defect

Solid-state electron spin qubits, like the nitrogen-vacancy center in diamond, rely on control sequences of population inversion to enhance sensitivity and improve device coherence. But even for this paradigmatic system, the fundamental limits of population inversion and potential impacts on applications like quantum sensing have not been assessed quantitatively. Here, we perform high accuracy simulations beyond the rotating wave approximation, including explicit unitary simulation of neighboring nuclear spins. Using quantum optimal control, we identify analytical pulses for the control of a qubit subspace within the spin-1 ground state and quantify the relationship between pulse complexity, control duration, and fidelity. We find exponentially increasing amplitude and bandwidth requirements with reduced control duration and further quantify the emergence of non-Markovian effects for multipulse sequences using sub-nanosecond population inversion. From this, we determine that the reduced fidelity and non-Markovianity is due to coherent interactions of the electron spin with the nuclear spin environment. Ultimately, we identify a potentially realizable regime of nanosecond control duration for high-fidelity multipulse sequences. These results provide key insights into the fundamental limits of quantum information processing using electron spin defects in diamond.

quant-ph↗