arXiv subjects

Alexander A. High

Publications and source records attributed to Alexander A. High.

At least 19 recordsLinked to original sources

arXiv2026

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↗

arXiv2025

Pump Free Microwave-Optical Quantum Transduction

Distributed quantum computing involves superconducting computation nodes operating at microwave frequencies, which are connected by long-distance transmission lines that transmit photons at optical frequencies. Quantum transduction, which coherently converts between microwave and optical (M-O) photons, is a critical component of such an architecture. Current approaches are hindered by the unavoidable problem of device heating due to the optical pump. In this work, we propose a pump-free scheme based on color centers that generates time-bin encoded M-O Bell pairs. Our scheme first creates spin-photon entanglement and then converts the spin state into a time-bin-encoded microwave photon using a strongly coupled Purcell-enhanced resonator. In our protocol, the microwave retrieval is heralded by detecting the microwave signal with a three-level transmon. We have analyzed the resulting Bell state fidelity and generation probability of this protocol. Our simulation shows that by combining a state-of-the-art spin-optical interface with our proposed strongly-coupled spin-microwave design, the pump-free scheme can generate M-O Bell pairs at a heralding rate exceeding one kilohertz with near-unity fidelity, which establishes the scheme as a promising source for M-O Bell pairs.

quant-ph↗

arXiv2025

Extending exciton and trion lifetimes in MoSe$_{2}$ with a nanoscale plasmonic cavity

Excitons in transition metal dichalcogenides (TMDs) have extremely short, picosecond-scale lifetimes which hinders exciton thermalization, limits the emergence of collective coherence, and reduces exciton transport in optoelectronic devices. In this work, we explore an all-optical pathway to extend exciton lifetimes by placing MoSe$_2$ in a deep-subwavelength Fabry-Perot silver cavity. The cavity structure is designed to suppress radiative recombination from in-plane optical dipoles, such as bright excitons and trions. We observe a consistent decrease in photoluminescence (PL) linewidths of excitons and trions (~1 nm), along with a corresponding lifetime increase (~10 ps). We confirm the experimental observations arise purely from exciton-cavity interactions-etching back the top silver layer returns the PL linewidth and lifetimes return to their original values. Our study offers a pathway to engineer excited state lifetimes in 2D materials which can be utilized for studies of optically dark excitons and have potential applications for novel optoelectronic devices.

cond-mat.mes-hall↗

arXiv2025

Donor-Acceptor Pairs near Silicon Carbide surfaces

Donor-acceptor pairs (DAPs) in wide-bandgap semiconductors are promising platforms for the realization of quantum technologies, due to their optically controllable, long-range dipolar interactions. Specifically, Al-N DAPs in bulk silicon carbide (SiC) have been predicted to enable coherent coupling over distances exceeding 10 nm. However, their practical implementations require an understanding of the properties of these pairs near surfaces and interfaces. Here, using first principles calculations we investigate how the presence of surfaces influence the stability and optical properties of Al-N DAPs in SiC, and we show that they retain favorable optical properties comparable to their bulk counterparts, despite a slight increase in electron-phonon coupling. Furthermore, we introduce the concept of surface-defect pairs (SDPs), where an electron-hole pair is generated between a near-surface defect and an occupied surface state located in the bandgap of the material. We show that vanadium-based SDPs near OH-terminated 4H-SiC surfaces exhibit dipoles naturally aligned perpendicular to the surface, greatly enhancing dipole-dipole coupling between SDPs. Our results also reveal significant polarization-dependent modulation in the stimulated emission and photoionization cross sections of V-based SDPs, which are tunable by two orders of magnitude via the polarization angle of the incident laser light. The near-surface defects investigated here provide novel possibilities for the development of hybrid quantum-classical interfaces, as they can be used to mediate information transfer between quantum nodes and integrated photonic circuits.

physics.comp-ph↗

arXiv2025

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↗

arXiv2024

Molecular optomechanics with atomic antennas

A typical surface-enhanced Raman scattering (SERS) system relies on deeply subwavelength field localization in nanoscale plasmonic cavities to enhance both the excitation and emission of Raman-active molecules. Here, we demonstrate that a germanium-vacancy (GeV) defect in diamond can efficiently mediate the excitation process, by acting as a bright atomic antenna. At low temperatures, the GeV's low dissipation allows it to be efficiently populated by the incident field, resulting in a thousand-fold increase in the efficiency of Raman scattering. We show that atomic antenna-enhanced Raman scattering can be distinguished from conventional SERS by tracing the dependence of Stokes intensity on input power.

quant-ph↗

arXiv2024

Metalens formed by structured arrays of atomic emitters

Arrays of atomic emitters have proven to be a promising platform to manipulate and engineer optical properties, due to their efficient cooperative response to near-resonant light. Here, we theoretically investigate their use as an efficient metalens. We show that, by spatially tailoring the (sub-wavelength) lattice constants of three consecutive two-dimensional arrays of identical atomic emitters, one can realize a large transmission coefficient with arbitrary position-dependent phase shift, whose robustness against losses is enhanced by the collective response. To characterize the efficiency of this atomic metalens, we perform large-scale numerical simulations involving a substantial number of atoms ($N\sim 5\times 10^5$) that is considerably larger than comparable works. Our results suggest that low-loss, robust optical devices with complex functionalities, ranging from metasurfaces to computer-generated holograms, could be potentially assembled from properly engineered arrays of atomic emitters.

quant-ph↗

arXiv2023

Microwave-based quantum control and coherence protection of tin-vacancy spin qubits in a strain-tuned diamond membrane heterostructure

Robust spin-photon interfaces in solids are essential components in quantum networking and sensing technologies. Ideally, these interfaces combine a long-lived spin memory, coherent optical transitions, fast and high-fidelity spin manipulation, and straightforward device integration and scaling. The tin-vacancy center (SnV) in diamond is a promising spin-photon interface with desirable optical and spin properties at 1.7 K. However, the SnV spin lacks efficient microwave control and its spin coherence degrades with higher temperature. In this work, we introduce a new platform that overcomes these challenges - SnV centers in uniformly strained thin diamond membranes. The controlled generation of crystal strain introduces orbital mixing that allows microwave control of the spin state with 99.36(9) % gate fidelity and spin coherence protection beyond a millisecond. Moreover, the presence of crystal strain suppresses temperature dependent dephasing processes, leading to a considerable improvement of the coherence time up to 223(10) $μ$s at 4 K, a widely accessible temperature in common cryogenic systems. Critically, the coherence of optical transitions is unaffected by the elevated temperature, exhibiting nearly lifetime-limited optical linewidths. Combined with the compatibility of diamond membranes with device integration, the demonstrated platform is an ideal spin-photon interface for future quantum technologies.

cond-mat.mes-hall↗

arXiv2023

Direct-bonded diamond membranes for heterogeneous quantum and electronic technologies

Diamond has superlative material properties for a broad range of quantum and electronic technologies. However, heteroepitaxial growth of single crystal diamond remains limited, impeding integration and evolution of diamond-based technologies. Here, we directly bond single-crystal diamond membranes to a wide variety of materials including silicon, fused silica, sapphire, thermal oxide, and lithium niobate. Our bonding process combines customized membrane synthesis, transfer, and dry surface functionalization, allowing for minimal contamination while providing pathways for near unity yield and scalability. We generate bonded crystalline membranes with thickness as low as 10 nm, sub-nm interfacial regions, and nanometer-scale thickness variability over 200 by 200 $\mu m^2$ areas. We measure spin coherence times $T_2$ for nitrogen-vacancy centers in bonded membranes of up to 623(21) $\mu$s, suitable for advanced quantum applications. We demonstrate multiple methods for integrating high quality factor nanophotonic cavities with the diamond heterostructures, highlighting the platform versatility in quantum photonic applications. Furthermore, we show that our ultra-thin diamond membranes are compatible with total internal reflection fluorescence (TIRF) microscopy, which enables interfacing coherent diamond quantum sensors with living cells while rejecting unwanted background luminescence. The processes demonstrated herein provide a full toolkit to synthesize heterogeneous diamond-based hybrid systems for quantum and electronic technologies.

physics.app-ph↗

arXiv2023

The maximum refractive index of an atomic crystal $\unicode{x2013}$ from quantum optics to quantum chemistry

All known optical materials have an index of refraction of order unity. Despite the tremendous implications that an ultrahigh index could have for optical technologies, little research has been done on why the refractive index of materials is universally small, and whether this observation is fundamental. Here, we investigate the index of an ordered arrangement of atoms, as a function of atomic density. At dilute densities, this problem falls into the realm of quantum optics, where atoms do not interact with one another except via the scattering of light. On the other hand, when the lattice constant becomes comparable to the Bohr radius, the electronic orbitals begin to overlap, giving rise to quantum chemistry. We present a minimal model that allows for a unifying theory of index spanning these two regimes. A key aspect is the treatment of multiple light scattering, which can be highly non-perturbative over a large density range, and which is the reason that conventional theories of the index break down. In the quantum optics regime, we show that ideal light-matter interactions can have a single-mode nature, allowing for a purely real refractive index that grows with density as $(N/V)^{1/3}$. At the onset of quantum chemistry, we show how two physical mechanisms (excited electron tunneling dynamics and the buildup of electronic density-density correlations) can open up inelastic or spatial multi-mode light scattering processes, which ultimately reduce the index back to order unity while introducing absorption. Around the onset of chemistry, our theory predicts that ultrahigh index ($n\sim 30$), low-loss materials could in principle be allowed by the laws of nature.

quant-ph↗

arXiv2021

Engineering the Radiative Dynamics of Thermalized Excitons with Metal Interfaces

As a platform for optoelectronic devices based on exciton dynamics, monolayer transition metal dichalcogenides (TMDCs) are often placed near metal interfaces or inside planar cavities. While the radiative properties of point dipoles at metal interfaces has been studied extensively, those of excitons, which are delocalized and exhibit a temperature-dependent momentum distribution, lack a thorough treatment. Here, we analyze the emission properties of excitons in TMDCs near planar metal interfaces and explore their dependence on exciton center-of-mass momentum, transition dipole orientation, and temperature. Defining a characteristic energy scale $k_B T_c = (\hbar k)^2/2m$~($k$ being the radiative wavevector and $m$ the exciton mass), we find that at temperatures $T\gg T_c$ and low densities where the momentum distribution can be characterized by Maxwell-Boltzmann statistics, the modified emission rates~(normalized to free space) behave similarly to point dipoles at temperatures $T\gg T_c$. This similarity in behavior arises due to the broad nature of wavevector components making up the exciton and point dipole emission. On the other hand, the narrow momentum distribution of excitons for $T<T_c$ can result in significantly different emission behavior as compared to point dipoles. These differences can be further amplified by considering excitons with a Bose Einstein distribution at high phase space densities. We find suppression or enhancement of emission relative to the point dipole case by several orders of magnitude. These insights can help optimize the performance of optoelectronic devices that incorporate 2D semiconductors near metal electrodes and can inform future studies of exciton radiative dynamics at low temperatures. Additionally, these studies show that nanoscale optical cavities are a viable pathway to generating long-lifetime exciton states in TMDCs.

cond-mat.mes-hall↗

arXiv2021

Tunable and Transferable Diamond Membranes for Integrated Quantum Technologies

Color centers in diamond are widely explored as qubits in quantum technologies. However, challenges remain in the effective and efficient integration of these diamond-hosted qubits in device heterostructures. Here, nanoscale-thick uniform diamond membranes are synthesized via "smart-cut" and isotopically (12C) purified overgrowth. These membranes have tunable thicknesses (demonstrated 50 nm to 250 nm), are deterministically transferable, have bilaterally atomically flat surfaces (Rq <= 0.3 nm), and bulk-diamond-like crystallinity. Color centers are synthesized via both implantation and in-situ overgrowth incorporation. Within 110 nm thick membranes, individual germanium-vacancy (GeV-) centers exhibit stable photoluminescence at 5.4 K and average optical transition linewidths as low as 125 MHz. The room temperature spin coherence of individual nitrogen-vacancy (NV-) centers shows Ramsey spin dephasing times (T2*) and Hahn echo times (T2) as long as 150 us and 400 us, respectively. This platform enables the straightforward integration of diamond membranes that host coherent color centers into quantum technologies.

physics.app-ph↗

arXiv2021

Optically controllable magnetism in atomically thin semiconductors

Electronic states in two-dimensional layered materials can exhibit a remarkable variety of correlated phases including Wigner-crystals, Mott insulators, charge density waves, and superconductivity. Recent experimental and theoretical research has indicated that ferromagnetic phases can exist in electronically-doped transition metal dichalcogenide (TMD) semiconductors, but a stable magnetic state at zero magnetic field has eluded detection. Here, we experimentally demonstrate that mesoscopic ferromagnetic order can be generated and controlled by local optical pumping in monolayer WSe2 at zero applied magnetic field. In a spatially resolved pump-probe experiment, we use polarization-resolved reflectivity from excitonic states as a probe of charge-carrier spin polarization. When the sample is electron-doped at density $n_e = 10^{12} cm^{-2}$, we observe that a local, circularly-polarized, microwatt-power optical pump breaks the symmetry between equivalent ferromagnetic spin configurations and creates magnetic order which extends over mesoscopic regions as large as 8 um x 5 um, bounded by sample edges and folds in the 2D semiconductor. The experimental signature of magnetic order is circular dichroism (CD) in reflectivity from the excitonic states, with magnitude exceeding 20% at resonant wavelengths. The helicity of the pump determines the orientation of the magnetic state, which can be aligned along the two principle out-of-plane axes. In contrast to previous studies in 2D materials that have required non-local, slowly varying magnetic fields to manipulate magnetic phases, the demonstrated capability to control long-range magnetism and corresponding strong CD with local and tunable optical pumps is highly versatile. This discovery will unlock new TMD-based spin and optical technologies and enable sophisticated control of correlated electron phases in two-dimensional electron gases (2DEGs).

cond-mat.mes-hall↗

arXiv2021

Maximum refractive index of an atomic medium

It is interesting to observe that all optical materials with a positive refractive index have a value of index that is of order unity. Surprisingly, though, a deep understanding of the mechanisms that lead to this universal behavior seems to be lacking. Moreover, this observation is difficult to reconcile with the fact that a single, isolated atom is known to have a giant optical response, as characterized by a resonant scattering cross section that far exceeds its physical size. Here, we theoretically and numerically investigate the evolution of the optical properties of an ensemble of ideal atoms as a function of density, starting from the dilute gas limit, including the effects of multiple scattering and near-field interactions. Interestingly, despite the giant response of an isolated atom, we find that the maximum index does not indefinitely grow with increasing density, but rather reaches a limiting value $n\approx 1.7$. We propose an explanation based upon strong-disorder renormalization group theory, in which the near-field interaction combined with random atomic positions results in an inhomogeneous broadening of atomic resonance frequencies. This mechanism ensures that regardless of the physical atomic density, light at any given frequency only interacts with at most a few near-resonant atoms per cubic wavelength, thus limiting the maximum index attainable. Our work is a promising first step to understand the limits of refractive index from a bottom-up, atomic physics perspective, and also introduces renormalization group as a powerful tool to understand the generally complex problem of multiple scattering of light overall.

quant-ph↗

arXiv2020

High-Q Nanophotonic Resonators on Diamond Membranes using Templated Atomic Layer Deposition of TiO2

Integrating solid-state quantum emitters with nanophotonic resonators is essential for efficient spin-photon interfacing and optical networking applications. While diamond color centers have proven to be excellent candidates for emerging quantum technologies, their integration with optical resonators remains challenging. Conventional approaches based on etching resonators into diamond often negatively impact color center performance and offer low device yield. Here, we developed an integrated photonics platform based on templated atomic layer deposition of TiO2 on diamond membranes. Our fabrication method yields high-performance nanophotonic devices while avoiding etching wavelength-scale features into diamond. Moreover, this technique generates highly reproducible optical resonances and can be iterated on individual diamond samples, a unique processing advantage. Our approach is suitable for a broad range of both wavelengths and substrates and can enable high-cooperativity interfacing between cavity photons and coherent defects in diamond or silicon carbide, rare earth ions, or other material systems.

quant-ph↗

arXiv2018

Electrical control of interlayer exciton dynamics in atomically thin heterostructures

Excitons in semiconductors, bound pairs of excited electrons and holes, can form the basis for new classes of quantum optoelectronic devices. A van der Waals heterostructure built from atomically thin semiconducting transition metal dichalcogenides (TMDs) enables the formation of excitons from electrons and holes in distinct layers, producing interlayer excitons with large binding energy and a long lifetime. Employing heterostructures of monolayer TMDs, we realize optical and electrical generation of long-lived neutral and charged interlayer excitons. We demonstrate the transport of neutral interlayer excitons across the whole sample that can be controlled by excitation power and gate electrodes. We also realize the drift motion of charged interlayer excitons using Ohmic-contacted devices. The electrical generation and control of excitons provides a new route for realizing quantum manipulation of bosonic composite particles with complete electrical tunability.

cond-mat.mes-hall↗

arXiv2017

Atomically thin mirrors made of monolayer semiconductors

Transition metal dichalcogenide monolayers are promising candidates for exploring new electronic and optical phenomena and for realizing atomically thin optoelectronic devices. They host tightly bound electron-hole pairs (excitons) that can be efficiently excited by resonant light fields. Here, we demonstrate that a single monolayer of molybdenum diselenide (MoSe2) can dramatically modify light transmission near the excitonic resonance, acting as an electrically switchable mirror that reflects up to 85% of incident light at cryogenic temperatures. This high reflectance is a direct consequence of the excellent coherence properties of excitons in this atomically thin semiconductor, encapsulated by hexagonal boron nitride. Furthermore, we show that the MoSe2 monolayer exhibits power- and wavelength-dependent nonlinearities that stem from exciton-based lattice heating in the case of continuous-wave excitation and exciton-exciton interactions when fast, pulsed laser excitation is used. These observations open up new possibilities for studying quantum nonlinear optical phenomena and topological photonics, and for miniaturizing optical devices.

cond-mat.mes-hall↗

arXiv2017

Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons

Transition metal dichalcogenide (TMD) monolayers are direct bandgap semiconductors that feature tightly bound excitons, strong spin-orbit coupling, and spin-valley degrees of freedom. Depending on the spin configuration of the electron-hole pairs, intra-valley excitons of TMD monolayers can be either optically bright or dark. Dark excitons involve nominally spin-forbidden optical transitions with zero in-plane transition dipole moment, making their detection with conventional far-field optical techniques challenging. Here, we introduce a new method for probing the optical properties of two-dimensional (2D) materials via near-field coupling to surface plasmon polaritons (SPPs), which selectively enhances optical transitions with dipole moments normal to the 2D plane. We utilize this method to directly detect dark excitons in monolayer TMDs. When a WSe2 monolayer is placed on top of a single-crystal silver film, its emission into near-field-coupled SPPs displays new spectral features whose energies and dipole orientations are consistent with dark neutral and charged excitons. The SPP-based near-field spectroscopy significantly enhances experimental capabilities for probing and manipulating exciton dynamics of atomically thin materials.

cond-mat.mes-hall↗