arXiv subjects

Harishankar Jayakumar

Publications and source records attributed to Harishankar Jayakumar.

At least 19 recordsLinked to original sources

arXiv2026

Enantiopurity-Controlled Magnetism in a Two-Dimensional Organic-Inorganic Material

Extended solids that combine unpaired electron spin and structural chirality can host unconventional magnetic behaviors with potential for electronic technologies. A versatile strategy for creating chiral solids is incorporation of chiral organic molecules into inorganic crystals. However, such hybrid organic-inorganic materials have so far been examined through the lens of absolute chirality, leaving enantiomeric excess (ee) underexplored as a tuning parameter. Here, we report two-dimensional (2D) intercalation compounds with controllable ee produced by cation exchange of MnPS$_3$ with chiral organic molecules. We show that these materials' magnetism is determined by intercalant ee rather than absolute chirality. Moreover, low-ee materials display thermally activated dynamic magnetism absent from enantiopure analogs. These ee-dependent magnetic behaviors are explained by local ordering of Mn vacancies, directed by correlated vacancy-intercalant electrostatics and confined molecular packing. Together, these results demonstrate a distinctive tuning strategy for molecule-material hybrids and establish design principles for 2D chiral and magnetically dynamic materials.

cond-mat.mtrl-sci↗

arXiv2026

Photoionization in KTN deflectors by light in the near-infrared imaging window

Electro-optical deflectors (EODs) offer unparalleled scanning speed for laser-scanning microscopy and other applications, but suffer from limited deflection range. EODs based on potassium tantalate niobate (KTN) crystals feature some of the highest number of resolvable spots. These deflectors rely on internal electric fields generated by trapped electrons to enable beam scanning. However, visible light induces rapid photoionization of trapped charges, thus KTN-based deflectors are typically continuously recharged with a bias voltage that effectively limits the range of the deflector. Recent work has proposed the use of KTN-based EODs for biological imaging with infrared excitation light, but quantitative data on near-infrared photoionization is lacking. Here, we present quantitative measurements of photoionization in KTN deflectors across the NIR-I and NIR-IIa biological imaging windows (700 - 1300 nm), a range that is particularly important for deep tissue imaging and nonlinear microscopy. Using a two-beam polarization interferometer, we measured trapped charge density as a function of photon fluence. We observed that the photoionization rate decreases dramatically with increasing wavelength. The charge density decay curves exhibit multi-exponential behavior that cannot be explained by a single-trap model without recapture, indicating the presence of multiple trap species or substantial recapture. These measurements provide critical quantitative guidance for selecting operating wavelengths and charge-scan duty cycles for KTN-based EODs in near-infrared imaging applications.

physics.optics↗

arXiv2025

Relayed-loop optical scan amplification

Many modern sensing, processing, and fabrication technologies depend upon the sequential scanning of laser light. Due to inertial, thermal, and electrical limitations, the speed of a typical laser deflector is inversely related to its optical invariant and therefore the number of resolvable spots it can address. Passive optical systems have been developed that can effectively double the optical invariant and maximum throughput of a single deflector. We present a method for increasing the effective optical invariant beyond 2$\times$ by repeated relaying of the deflected beam onto the deflector in an optical loop created within a cavity. We use this Relayed-Loop Optically Amplified Deflection (ReLOAD) approach to accomplish 8$\times$ amplification of electro-optical (EO) deflection, a deflection technology with unparalleled speed, but limited optical invariant. Using ReLOAD, we demonstrate 10 kHz frame rate imaging, 1 MHz line scan rate, and $\mu$s step times across an addressable space well beyond the capabilities of typical electro-optical deflectors.

physics.optics↗

arXiv2022

Room-temperature photo-chromism of silicon vacancy centers in CVD diamond

The silicon-vacancy (SiV) center in diamond is typically found in three stable charge states, SiV0, SiV- and SiV2-, but studying the processes leading to their formation is challenging, especially at room temperature, due to their starkly different photo-luminescence rates. Here, we use confocal fluorescence microscopy to activate and probe charge interconversion between all three charge states under ambient conditions. In particular, we witness the formation of SiV0 via the two-step capture of diffusing, photo-generated holes, a process we expose both through direct SiV0 fluorescence measurements at low temperatures and confocal microscopy observations in the presence of externally applied electric fields. Further, we show that continuous red illumination induces the converse process, first transforming SiV0 into SiV-, then into SiV2-. Our results shed light on the charge dynamics of SiV and promise opportunities for nanoscale sensing and quantum information processing.

cond-mat.mtrl-sci↗

arXiv2022

Spin dynamics of a solid-state qubit in proximity to a superconductor

A broad effort is underway to understand and harness the interaction between superconductors and spin-active color centers with an eye on the realization of hybrid quantum devices and novel imaging modalities of superconducting materials. Most work, however, overlooks the complex interplay between either system and the environment created by the color center host. Here we use an all-diamond scanning probe to investigate the spin dynamics of a single nitrogen-vacancy (NV) center proximal to a high-critical-temperature superconducting film in the presence of a weak magnetic field. We find that the presence of the superconductor increases the NV spin coherence lifetime, a phenomenon we tentatively rationalize as a change in the electric noise due to a superconductor-induced redistribution of charge carriers near the NV site. We build on these findings to demonstrate transverse-relaxation-time-weighted imaging of the superconductor film. These results shed light on the complex surface dynamics governing the spin coherence of shallow NVs while simultaneously paving the route to new forms of noise spectroscopy and imaging of superconductors.

cond-mat.mes-hall↗

arXiv2021

Optical activation and detection of charge transport between individual color centers in room-temperature diamond

Charge control of color centers in semiconductors promises opportunities for novel forms of sensing and quantum information processing. Here, we articulate confocal fluorescence microscopy and magnetic resonance protocols to induce and probe charge transport between discrete sets of engineered nitrogen-vacancy (NV) centers in diamond, down to the level of individual defects. In our experiments, a "source" NV undergoes optically-driven cycles of ionization and recombination to produce a stream of photo-generated carriers, one of which we subsequently capture via a "target" NV several micrometers away. We use a spin-to-charge conversion scheme to encode the spin state of the source color center into the charge state of the target, in the process allowing us to set an upper bound to carrier injection from other background defects. We attribute our observations to the action of unscreened Coulomb potentials producing giant carrier capture cross-sections, orders of magnitude greater than those typically attained in ensemble measurements. Besides their fundamental interest, these results open intriguing prospects in the use of free carriers as a quantum bus to mediate effective interactions between paramagnetic defects in a solid-state chip.

cond-mat.mes-hall↗

arXiv2021

Investigation of photon emitters in Ce-implanted hexagonal boron nitride

Color centers in hexagonal boron nitride (hBN) are presently attracting broad interest as a novel platform for nanoscale sensing and quantum information processing. Unfortunately, their atomic structures remain largely elusive and only a small percentage of the emitters studied thus far has the properties required to serve as optically addressable spin qubits. Here, we use confocal fluorescence microscopy at variable temperature to study a new class of point defects produced via cerium ion implantation in thin hBN flakes. We find that, to a significant fraction, emitters show bright room-temperature emission, and good optical stability suggesting the formation of Ce-based point defects. Using density functional theory (DFT) we calculate the emission properties of candidate emitters, and single out the CeVB center - formed by an interlayer Ce atom adjacent to a boron vacancy - as one possible microscopic model. Our results suggest an intriguing route to defect engineering that simultaneously exploits the singular properties of rare-earth ions and the versatility of two-dimensional material hosts.

cond-mat.mes-hall↗

arXiv2021

Tunable amplification and cooling of a diamond resonator with a microscope

Controlling the dynamics of mechanical resonators is central to many quantum science and metrology applications. Optomechanical control of diamond resonators is attractive owing to diamond's excellent physical properties and its ability to host electronic spins that can be coherently coupled to mechanical motion. Using a confocal microscope, we demonstrate tunable amplification and damping of a diamond nanomechanical resonator's motion. Observation of both normal mode cooling from room temperature to 80K, and amplification into self--oscillations with $60\,μ\text{W}$ of optical power is observed via waveguide optomechanical readout. This system is promising for quantum spin-optomechanics, as it is predicted to enable optical control of stress-spin coupling with rates of $\sim$ 1 MHz (100 THz) to ground (excited) states of diamond nitrogen vacancy centers.

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

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

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↗

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↗

arXiv2017

Near-deterministic activation of room temperature quantum emitters in hexagonal boron nitride

Applications of quantum science to computing, cryptography and imaging are on their way to becoming key next generation technologies. Owing to the high-speed transmission and exceptional noise properties of photons, quantum photonic architectures are likely to play a central role. A long-standing hurdle, however, has been the realization of robust, device-compatible single photon sources that can be activated and controlled on demand. Here we use strain engineering to create large arrays of quantum emitters in two-dimensional hexagonal boron nitride (hBN). The large energy gap inherent to this Van der Waals material stabilizes the emitters at room temperature within nanoscale regions defined by substrate-induced deformation of the flake. Combining analytical and numerical modeling we show that emitter activation is likely the result of carrier trapping in deformation potential wells localized near the points where the hBN flake reaches the highest curvature. These findings, therefore, hint at novel opportunities for the manipulation of single photon sources through the combined control of strain and external electrostatic potentials under ambient conditions.

cond-mat.mes-hall↗

arXiv2016

Long-term data storage in diamond

The negatively-charged nitrogen-vacancy (NV-) center in diamond is the focus of widespread attention for applications ranging from quantum information processing to nanoscale metrology. Although most work so far has focused on the NV- optical and spin properties, control of the charge state promises complementary opportunities. One intriguing possibility is the long-term storage of information, a notion we hereby introduce using NV rich, type-1b diamond. As a proof of principle, we use multi-color optical microscopy to read, write, and reset arbitrary data sets with 2-D binary bit density comparable to present digital-video-disk (DVD) technology. Leveraging on the singular dynamics of NV- ionization, we encode information on different planes of the diamond crystal with no cross talk, hence extending the storage capacity to three dimensions. Further, we correlate the center's charge state and nuclear spin polarization of the nitrogen host, and show that the latter is robust to a cycle of NV- ionization and recharge. In combination with super-resolution microscopy techniques, these observations provide a route towards sub-diffraction NV charge control, a regime where the storage capacity could exceed present technologies.

cond-mat.mes-hall↗

arXiv2016

Optical patterning of trapped charge in nitrogen-doped diamond

The nitrogen-vacancy (NV) centre in diamond is emerging as a promising platform for solid-state quantum information processing and nanoscale metrology. Of interest in these applications is the manipulation of the NV charge, which can be attained by optical excitation. Here we use two-color optical microscopy to investigate the dynamics of NV photo-ionization, charge diffusion, and trapping in type-1b diamond. We combine fixed-point laser excitation and scanning fluorescence imaging to locally alter the concentration of negatively charged NVs, and to subsequently probe the corresponding redistribution of charge. We uncover the formation of spatial patterns of trapped charge, which we qualitatively reproduce via a model of the interplay between photo-excited carriers and atomic defects. Further, by using the NV as a probe, we map the relative fraction of positively charged nitrogen upon localized optical excitation. These observations may prove important to transporting quantum information between NVs or to developing three-dimensional, charge-based memories.

cond-mat.mes-hall↗

arXiv2016

Efficient telecom to visible wavelength conversion in doubly resonant GaP microdisks

Resonant second harmonic generation between 1550 nm and 775 nm with outside efficiency $> 4.4\times10^{-4}\, \text{mW}^{-1}$ is demonstrated in a gallium phosphide microdisk cavity supporting high-$Q$ modes at visible ($Q \sim 10^4$) and infrared ($Q \sim 10^5$) wavelengths. The double resonance condition was satisfied through intracavity photothermal temperature tuning using $\sim 360\,μ$W of 1550 nm light input to a fiber taper and resonantly coupled to the microdisk. Above this pump power efficiency was observed to decrease. The observed behavior is consistent with a simple model for thermal tuning of the double resonance condition.

physics.optics↗