arXiv subjects

Carlos A. Meriles

Publications and source records attributed to Carlos A. Meriles.

At least 55 records · Page 3Linked to original sources

arXiv2021

Magnetic-field-induced delocalization in hybrid electron-nuclear spin ensembles

We use field-cycling-assisted dynamic nuclear polarization and continuous radio-frequency (RF) driving over a broad spectral range to demonstrate magnetic-field-dependent activation of nuclear spin transport from strongly-hyperfine-coupled 13C sites in diamond. We interpret our observations with the help of a theoretical framework where nuclear spin interactions are mediated by electron spins. In particular, we build on the results from a 4-spin toy model to show how otherwise localized nuclear spins must thermalize as they are brought in contact with a larger ancilla spin network. Further, by probing the system response to a variable driving field amplitude, we witness stark changes in the RF-absorption spectrum, which we interpret as partly due to contributions from heterogeneous multi-spin sets, whose 'zero-quantum' transitions become RF active thanks to the hybrid electron-nuclear nature of the system. These findings could prove relevant in applications to dynamic nuclear polarization, spin-based quantum information processing, and nanoscale sensing.

cond-mat.mes-hall↗

arXiv2021

Nuclear spin temperature reversal via continuous radio-frequency driving

Optical spin pumping of color centers in diamond is presently attracting broad interest as a platform for dynamic nuclear polarization at room temperature, but the mechanisms involved in the generation and transport of polarization within the host crystal are still partly understood. Here we investigate the impact of continuous radio-frequency (RF) excitation on the generation of nuclear magnetization produced by optical illumination. In the presence of RF excitation far removed from the nuclear Larmor frequency, we witness a magnetic-field-dependent sign reversal of the measured nuclear spin signal when the drive is sufficiently strong, a counter-intuitive finding that immediately points to non-trivial spin dynamics. With the help of analytical and numerical modeling, we show our observations indicate a modified form of 'solid effect', down-converted from the microwave to the radio-frequency range through the driving of hybrid transitions involving one (or more) nuclei and two (or more) electron spins. Our results open intriguing opportunities for the manipulation of many-electron spin systems by exploiting hyperfine couplings as a means to access otherwise forbidden intra-band transitions.

physics.app-ph↗

arXiv2021

Spontaneous emission dynamics of $Eu^{ 3+}$ ions coupled to hyperbolic metamaterials

Sub-wavelength nanostructured systems with tunable electromagnetic properties, such as hyperbolic metamaterials (HMMs), provide a useful platform to tailor spontaneous emission processes. Here, we investigate a system comprising $Eu^{ 3+}(NO_{3})_{3}6H_{2}O$ nanocrystals on an HMM structure featuring a hexagonal array of Ag-nanowires in a porous $Al_{2}O_{3}$ matrix. The HMM-coupled $Eu^{ 3+}$ ions exhibit up to a 2.4-fold increase of their decay rate, accompanied by an enhancement of the emission rate of the $^{ 5}D_{0}\rightarrow$ $^{ 7}F_{2}$ transition. Using finite-difference time-domain modeling, we corroborate these observations with the increase in the photonic density of states seen by the $Eu^{ 3+}$ ions in the proximity of the HMM. Our results indicate HMMs can serve as a valuable tool to control the emission from weak transitions, and hence hint at a route towards more practical applications of rare-earth ions in nanoscale optoelectronics and quantum devices.

physics.optics↗

arXiv2020

Probing metastable space-charge potentials in a wide bandgap semiconductor

While the study of space charge potentials has a long history, present models are largely based on the notion of steady state equilibrium, ill-suited to describe wide bandgap semiconductors with moderate to low concentrations of defects. Here we build on color centers in diamond both to locally inject carriers into the crystal and probe their evolution as they propagate in the presence of external and internal potentials. We witness the formation of metastable charge patterns whose shape - and concomitant field - can be engineered through the timing of carrier injection and applied voltages. With the help of previously crafted charge patterns, we unveil a rich interplay between local and extended sources of space charge field, which we then exploit to show space-charge-induced carrier guiding.

cond-mat.mes-hall↗

arXiv2020

Optically pumped spin polarization as a probe of many-body thermalization

The interplay between disorder and transport is a problem central to the understanding of a broad range of physical processes, most notably the ability of a system to reach thermal equilibrium. Disorder and many body interactions are known to compete, with the dominance of one or the other giving rise to fundamentally different dynamical phases. Here we investigate the spin diffusion dynamics of 13C in diamond, which we dynamically polarize at room temperature via optical spin pumping of engineered color centers. We focus on low-abundance, strongly hyperfine-coupled nuclei, whose role in the polarization transport we expose through the integrated impact of variable radio-frequency excitation on the observable bulk 13C magnetic resonance signal. Unexpectedly, we find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength, which we attribute to effective carbon-carbon interactions mediated by the electronic spin ensemble. In particular, observations across the full range of hyperfine couplings indicate the nuclear spin diffusion constant takes values up to two orders of magnitude greater than that expected from homo-nuclear spin couplings. Our results open intriguing opportunities to study the onset of thermalization in a system by controlling the internal interactions within the bath.

quant-ph↗

arXiv2020

Long-term spin state storage using ancilla charge memories

We articulate confocal microscopy and electron spin resonance to implement spin-to-charge conversion in a small ensemble of nitrogen-vacancy (NV) centers in bulk diamond, and demonstrate charge conversion of neighboring defects conditional on the NV spin state. We build on this observation to show time-resolved NV spin manipulation and ancilla-charge-aided NV spin state detection via integrated measurements. Our results hint at intriguing opportunities in the search for enhanced forms of color-center-based metrology and information processing down to the limit of individual point defects.

quant-ph↗

arXiv2019

Room-temperature Single Photon Emitters in Cubic Boron Nitride Nanocrystals

Color centers in wide bandgap semiconductors are attracting broad attention as platforms for quantum technologies relying on room-temperature single-photon emission (SPE), and for nanoscale metrology applications building on the centers' response to electric and magnetic fields. Here, we demonstrate room-temperature SPE from defects in cubic boron nitride (cBN) nanocrystals, which we unambiguously assign to the cubic phase using spectrally resolved Raman imaging. These isolated spots show photoluminescence (PL) spectra with zero-phonon lines (ZPLs) within the visible region (496-700 nm) when subject to sub-bandgap laser excitation. Second-order autocorrelation of the emitted photons reveals antibunching with $g^{2}$ ~ 0.2 and a decay constant of 2.75 ns that is further confirmed through fluorescence lifetime measurements. The results presented herein prove the existence of optically addressable isolated quantum emitters originating from defects in cBN, making this material an interesting platform for opto-electronic devices and quantum applications.

cond-mat.mes-hall↗

arXiv2019

Coupling of deterministically activated quantum emitters in hexagonal boron nitride to plasmonic surface lattice resonances

Cooperative phenomena stemming from radiation-field-mediated coupling between individual quantum emitters are presently attracting broad interest for on-chip photonic quantum memories and long-range entanglement. Common to these applications is the generation of electromagnetic modes over macroscopic distances. Much research, however, is still needed before such systems can be deployed in the form of practical devices, starting with the investigation of alternate physical platforms. Quantum emitters in two-dimensional (2D) systems provide an intriguing route because these materials can be adapted to arbitrarily shaped substrates to form hybrid systems where emitters are near-field-coupled to suitable optical modes. Here, we report a scalable coupling method allowing color center ensembles in a van der Waals material - hexagonal boron nitride - to couple to a delocalized high quality plasmonic surface lattice resonance. This type of architecture is promising for photonic applications, especially given the ability of the hexagonal boron nitride emitters to operate as single-photon sources at room temperature.

physics.optics↗

arXiv2019

Scalable microcavity-coupled emitters in hexagonal boron nitride

Scalable integration of bright emitters in quantum photonic structures is an important step in the broader quest to generate and manipulate single photons via compact solid-state devices. Unfortunately, implementations relying on material platforms that also serve as the emitter host often suffer from a trade-off between the desired emitter properties and the photonic system practicality and performance. Here, we demonstrate 'pick and place' integration of a Silicon Nitride microdisk optical resonator with a bright emitter host in the form of 20nm thick hexagonal boron nitride (hBN).The film folds around the microdisk maximizing contact to ultimately form a composite hBN/Si3N4 structure. The local strain that develops in the hBN film at the resonator circumference deterministically activates a low density of SPEs within the whispering gallery mode volume of the microdisk. These conditions allow us to demonstrate cavity-mediated out-coupling and Purcell enhancement of emission from hBN color centers through the microdisk cavity modes. Our results pave the route toward the development of scalable quantum photonic circuits with independent emitter/resonator optimization for active and passive functionalities.

physics.optics↗

arXiv2019

Two-electron-spin ratchets as a platform for microwave-free dynamic nuclear polarization of arbitrary material targets

Optically-pumped color centers in semiconductor powders can potentially induce high levels of nuclear spin polarization in surrounding solids or fluids at or near ambient conditions, but complications stemming from the random orientation of the particles and the presence of unpolarized paramagnetic defects hinder the flow of polarization beyond the defect's host material. Here, we theoretically study the spin dynamics of interacting nitrogen-vacancy (NV) and substitutional nitrogen (P1) centers in diamond to show that outside protons spin-polarize efficiently upon a magnetic field sweep across the NV-P1 level anti-crossing. The process can be interpreted in terms of an NV-P1 spin ratchet, whose handedness - and hence the sign of the resulting nuclear polarization - depends on the relative timing of the optical excitation pulse. Further, we find that the polarization transfer mechanism is robust to NV misalignment relative to the external magnetic field, and efficient over a broad range of electron-electron and electron-nuclear spin couplings, even if proxy spins feature short coherence or spin-lattice relaxation times. Therefore, these results pave the route towards the dynamic nuclear polarization of arbitrary spin targets brought in proximity with a diamond powder under ambient conditions.

quant-ph↗

arXiv2019

Dynamics of frequency-swept nuclear spin optical pumping in powdered diamond at low magnetic fields

A broad effort is underway to improve the sensitivity of nuclear magnetic resonance through the use of dynamic nuclear polarization. Nitrogen-vacancy (NV) centers in diamond offer an appealing platform because these paramagnetic defects can be optically polarized efficiently at room temperature. However, work thus far has been mainly limited to single crystals because most polarization transfer protocols are sensitive to misalignment between the NV and magnetic field axes. Here we study the spin dynamics of NV-13C pairs in the simultaneous presence of optical excitation and microwave frequency sweeps at low magnetic fields. We show that a subtle interplay between illumination intensity, frequency sweep rate, and hyperfine coupling strength leads to efficient, sweep-direction-dependent 13C spin polarization over a broad range of orientations of the magnetic field. In particular, our results strongly suggest that finely-tuned, moderately coupled nuclear spins are key to the hyperpolarization process, which makes this mechanism distinct from other known dynamic polarization channels. These findings pave the route to applications where powders are intrinsically advantageous, including the hyper-polarization of target fluids in contact with the diamond surface or the use of hyperpolarized particles as contrast agents for in-vivo imaging.

cond-mat.mes-hall↗

arXiv2019

Hyperpolarized relaxometry based nuclear T1 noise spectroscopy in hybrid diamond quantum registers

Understanding the origins of spin lifetimes in hybrid quantum systems is a matter of current importance in several areas of quantum information and sensing. Methods that spectrally map spin relaxation processes provide insight into their origin and can motivate methods to mitigate them. In this paper, using a combination of hyperpolarization and precision field cycling over a wide range (1mT-7T), we map frequency dependent relaxation in a prototypical hybrid system of 13C nuclear spins in diamond coupled to Nitrogen Vacancy centers. Nuclear hyperpolarization through the optically pumped NV electrons allows signal time savings for the measurements exceeding million-fold over conventional methods. We observe that 13C lifetimes show a dramatic field dependence, growing rapidly with field up to 100mT and saturating thereafter. Through a systematic study with increasing substitutional electron (P1 center) concentration as well as 13C enrichment levels, we identify the operational relaxation channels for the nuclei in different field regimes. In particular, we demonstrate the dominant role played by the 13C nuclei coupling to the interacting P1 electronic spin bath. These results pave the way for quantum control techniques for dissipation engineering to boost spin lifetimes in diamond, with applications ranging from engineered quantum memories to hyperpolarized 13C imaging.

quant-ph↗

arXiv2018

Room temperature "Optical Nanodiamond Hyperpolarizer": physics, design and operation

Dynamic Nuclear Polarization (DNP) is a powerful suite of techniques that deliver multifold signal enhancements in NMR and MRI. The generated athermal spin states can also be exploited for quantum sensing and as probes for many-body physics. Typical DNP methods require use of cryogens, large magnetic fields, and high power microwaves, which are expensive and unwieldy. Nanodiamond particles, rich in Nitrogen-Vacancy (NV) centers, have attracted attention as alternative DNP agents because they can potentially be optically hyperpolarized at room temperature. Indeed the realization of a miniature "optical nanodiamond hyperpolarizer", where 13C nuclei are optically hyperpolarized has been a longstanding goal but has been technically challenging to achieve. Here, unravelling new physics underlying an optical DNP mechanism first introduced in [Ajoy et al., Sci. Adv. 4, eaar5492 (2018)], we report the realization of such a device in an ultracompact footprint and working fully at room temperature. Instrumental requirements are very modest: low polarizing fields, extremely low optical and microwave irradiation powers, and convenient frequency ranges that enable device miniaturization. We obtain best reported optical 13C hyperpolarization in diamond particles exceeding 720 times of the thermal 7T value (0.86% bulk polarization), corresponding to a ten-million-fold gain in NMR averaging time. In addition the hyperpolarization signal can be background-suppressed by over two-orders of magnitude and retained for multiple-minute long periods. Besides compelling applications in quantum sensing, and bright-contrast MRI imaging, this work paves the way for low-cost DNP platforms that relay the 13C polarization to liquids in contact with the high surface-area particles. This will ultimately allow development of miniature "quantum-assisted" NMR spectrometers for chemical analysis.

quant-ph↗

arXiv2018

Toward the Identification of Atomic Defects in Hexagonal Boron Nitride: X-Ray Photoelectron Spectroscopy and First-Principles Calculations

Defects in hexagonal boron nitride (hBN) exhibit single-photon emission (SPE) and are thus attracting broad interest as platforms for quantum information and spintronic applications. However, the atomic structure and the specific impact of the local environment on the defect physical properties remain elusive. Here we articulate X-ray photoelectron spectroscopy (XPS) and first-principles calculations to discern the experimentally-observed point defects responsible for the quantum emission observed in hBN. XPS measurements show a broad band, which was deconvolved and then assigned to $N_{B}V_{N}$, $V_{N}$, $C_{B}$, $C_{B}V_{N}$, and $O_{2B}V_{N}$ defect structures using Density Functional Theory (DFT) core-level binding energy (BE) calculations.

cond-mat.mtrl-sci↗

arXiv2018

Spin readout via spin-to-charge conversion in bulk diamond nitrogen-vacancy ensembles

We demonstrate optical readout of ensembles of nitrogen-vacancy(NV) center spins in a bulk diamond sample via spin-to-charge conversion. A high power 594 nm laser is utilized to selectively ionize these paramagnetic defects in the spin state with a contrast of up to 12%. In comparison with the conventional 520 nm spin readout, spin-to-charge-conversion-based readout provides higher signal-to-noise ratio, with tenfold sensing measurement speedup for millisecond long pulse sequences. This level of performance was achieved for an NV- ionization of only 25%, limited by the ionization and readout laser powers. These observations pave the way to a range of high-sensitivity metrology applications where the use of NV- ensembles in bulk diamond has proven useful, including sensing and imaging of target materials overlaid on the diamond surface.

cond-mat.mes-hall↗

arXiv2018

Charge dynamics in near-surface, variable-density ensembles of nitrogen-vacancy centers in diamond

Although the spin properties of superficial shallow nitrogen-vacancy (NV) centers have been the subject of extensive scrutiny, considerably less attention has been devoted to studying the dynamics of NV charge conversion near the diamond surface. Using multi-color confocal microscopy, here we show that near-surface point defects arising from high-density ion implantation dramatically increase the ionization and recombination rates of shallow NVs compared to those in bulk diamond. Further, we find that these rates grow linearly not quadratically with laser intensity, indicative of single-photon processes enabled by NV state mixing with other defect states. Accompanying these findings we observe NV ionization and recombination in the dark, likely the result of charge transfer to neighboring traps. In spite of the altered charge dynamics, we show one can imprint rewritable, long-lasting patterns of charged-initialized, near-surface NVs over large areas, an ability that could be exploited for electrochemical biosensing or to optically store digital data sets with sub-diffraction resolution.

cond-mat.mes-hall↗

arXiv2018

On-Demand Generation of Neutral and Negatively-Charged Silicon-Vacancy Centers in Diamond

Point defects in wide-bandgap semiconductors are emerging as versatile resources for nanoscale sensing and quantum information science but our understanding of the photo-ionization dynamics is presently incomplete. Here we use two-color confocal microscopy to investigate the dynamics of charge in Type 1b diamond hosting nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers. By examining the non-local fluorescence patterns emerging from local laser excitation, we show that in the simultaneous presence of photo-generated electrons and holes, SiV (NV) centers selectively transform into the negative (neutral) charge state. Unlike NVs, 532 nm illumination ionizes SiV- via a single photon process thus hinting at a comparatively shallower ground state. In particular, slower ionization rates at longer wavelengths suggest the latter lies approximately ~1.9 eV below the conduction band minimum. Building on the above observations we demonstrate on-demand SiV and NV charge initialization over large areas via green laser illumination of variable intensity.

cond-mat.mes-hall↗

arXiv2017

Multi-spin-assisted optical pumping of bulk 13C nuclear spin polarization in diamond

One of the most remarkable properties of the nitrogen-vacancy (NV) center in diamond is that optical illumination initializes its electronic spin almost completely, a feature that can be exploited to polarize other spin species in their proximity. Here we use field-cycled nuclear magnetic resonance (NMR) to investigate the mechanisms of spin polarization transfer from NVs to 13C spins in diamond at room temperature. We focus on the dynamics near 51 mT, where a fortuitous combination of energy matching conditions between electron and nuclear spin levels gives rise to alternative polarization transfer channels. By monitoring the 13C spin polarization as a function of the applied magnetic field, we show 13C spin pumping takes place via a multi-spin cross relaxation process involving the NV- spin and the electronic and nuclear spins of neighboring P1 centers. Further, we find that this mechanism is insensitive to the crystal orientation relative to the magnetic field, although the absolute level of 13C polarization - reaching up to ~3% under optimal conditions - can vary substantially depending on the interplay between optical pumping efficiency, photo-generated carriers, and laser-induced heating.

quant-ph↗