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Hongkun Park

Publications and source records attributed to Hongkun Park.

At least 55 records · Page 3Linked to original sources

Controlling excitons in an atomically thin membrane with a mirror

We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photonic density of states in a controllable and reversible fashion, we show that both the absorption and emission properties of the excitons can be dynamically modulated. This electromechanical control over exciton dynamics in a mechanically flexible, atomically thin semiconductor opens up new avenues in cavity quantum optomechanics, nonlinear quantum optics, and topological photonics.

cond-mat.mes-hall↗

Experimental demonstration of memory-enhanced quantum communication

The ability to communicate quantum information over long distances is of central importance in quantum science and engineering. For example, it enables secure quantum key distribution (QKD) relying on fundamental principles that prohibit the "cloning" of unknown quantum states. While QKD is being successfully deployed, its range is currently limited by photon losses and cannot be extended using straightforward measure-and-repeat strategies without compromising its unconditional security. Alternatively, quantum repeaters, which utilize intermediate quantum memory nodes and error correction techniques, can extend the range of quantum channels. However, their implementation remains an outstanding challenge, requiring a combination of efficient and high-fidelity quantum memories, gate operations, and measurements. Here we report the experimental realization of memory-enhanced quantum communication. We use a single solid-state spin memory integrated in a nanophotonic diamond resonator to implement asynchronous Bell-state measurements. This enables a four-fold increase in the secret key rate of measurement device independent (MDI)-QKD over the loss-equivalent direct-transmission method while operating megahertz clock rates. Our results represent a significant step towards practical quantum repeaters and large-scale quantum networks.

quant-ph↗

Single crystals of the layered dichalcogenides MoS2 and WS2 grown by liquid phase transport

The growth of single crystals of MoS2 and WS2 by materials transport through a liquid salt flux made from a low melting mixture of NaCl and CsCl is described. The crystals are characterized by single crystal X-ray diffraction, which reveals that they are 2H-MoS2 with a small percentage (about 3%) of 3R intergrowths. The 2H-WS2 crystals display less than 1% of 3R intergrowths. Photoluminescence spectra of exfoliated monolayers suggest that MoS2 grown by this method has superior crystallinity in comparison to commercially-available MoS2 crystals.

cond-mat.mtrl-sci↗

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↗

Origins of diamond surface noise probed by correlating single spin measurements with surface spectroscopy

The nitrogen vacancy (NV) center in diamond exhibits spin-dependent fluorescence and long spin coherence times under ambient conditions, enabling applications in quantum information processing and sensing. NV centers near the surface can have strong interactions with external materials and spins, enabling new forms of nanoscale spectroscopy. However, NV spin coherence degrades within 100 nanometers of the surface, suggesting that diamond surfaces are plagued with ubiquitous defects. Prior work on characterizing near-surface noise has primarily relied on using NV centers themselves as probes; while this has the advantage of exquisite sensitivity, it provides only indirect information about the origin of the noise. Here we demonstrate that surface spectroscopy methods and single spin measurements can be used as complementary diagnostics to understand sources of noise. We find that surface morphology is crucial for realizing reproducible chemical termination, and use these insights to achieve a highly ordered, oxygen-terminated surface with suppressed noise. We observe NV centers within 10 nm of the surface with coherence times extended by an order of magnitude.

cond-mat.mtrl-sci↗

Hyperpolarization-enhanced NMR spectroscopy with femtomole sensitivity using quantum defects in diamond

Nuclear magnetic resonance (NMR) spectroscopy is a widely used tool for chemical analysis and molecular structure identification. Because it typically relies on the weak magnetic fields produced by a small thermal nuclear spin polarization, NMR suffers from poor molecule-number sensitivity compared to other analytical techniques. Recently, a new class of NMR sensors based on optically-probed nitrogen-vacancy (NV) quantum defects in diamond have allowed molecular spectroscopy from sample volumes several orders of magnitude smaller than the most sensitive inductive detectors. To date, however, NV-NMR spectrometers have only been able to observe signals from pure, highly concentrated samples. To overcome this limitation, we introduce a technique that combines picoliter-scale NV-NMR with fully integrated Overhauser dynamic nuclear polarization (DNP) to perform high-resolution spectroscopy on a variety of small molecules in dilute solution, with femtomole sensitivity. Our technique advances mass-limited NMR spectroscopy for drug and natural product discovery, catalysis research, and single cell studies.

physics.app-ph↗

Photon-mediated interactions between quantum emitters in a diamond nanocavity

Photon-mediated interactions between quantum systems are essential for realizing quantum networks and scalable quantum information processing. We demonstrate such interactions between pairs of silicon-vacancy (SiV) color centers strongly coupled to a diamond nanophotonic cavity. When the optical transitions of the two color centers are tuned into resonance, the coupling to the common cavity mode results in a coherent interaction between them, leading to spectrally-resolved superradiant and subradiant states. We use the electronic spin degrees of freedom of the SiV centers to control these optically-mediated interactions. Our experiments pave the way for implementation of cavity-mediated quantum gates between spin qubits and for realization of scalable quantum network nodes.

quant-ph↗

High Resolution Magnetic Resonance Spectroscopy Using Solid-State Spins

We demonstrate a synchronized readout (SR) technique for spectrally selective detection of oscillating magnetic fields with sub-millihertz resolution, using coherent manipulation of solid state spins. The SR technique is implemented in a sensitive magnetometer (~50 picotesla/Hz^(1/2)) based on nitrogen vacancy (NV) centers in diamond, and used to detect nuclear magnetic resonance (NMR) signals from liquid-state samples. We obtain NMR spectral resolution ~3 Hz, which is nearly two orders of magnitude narrower than previously demonstrated with NV based techniques, using a sample volume of ~1 picoliter. This is the first application of NV-detected NMR to sense Boltzmann-polarized nuclear spin magnetization, and the first to observe chemical shifts and J-couplings.

quant-ph↗

Quantum Nonlinear Optics with a Germanium-Vacancy Color Center in a Nanoscale Diamond Waveguide

We demonstrate a quantum nanophotonics platform based on germanium-vacancy (GeV) color centers in fiber-coupled diamond nanophotonic waveguides. We show that GeV optical transitions have a high quantum efficiency and are nearly lifetime-broadened in such nanophotonic structures. These properties yield an efficient interface between waveguide photons and a single GeV without the use of a cavity or slow-light waveguide. As a result, a single GeV center reduces waveguide transmission by $18 \pm 1\%$ on resonance in a single pass. We use a nanophotonic interferometer to perform homodyne detection of GeV resonance fluorescence. By probing the photon statistics of the output field, we demonstrate that the GeV-waveguide system is nonlinear at the single-photon level.

quant-ph↗

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↗

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↗

Single-Photon Switching and Entanglement of Solid-State Qubits in an Integrated Nanophotonic System

Efficient interfaces between photons and quantum emitters form the basis for quantum networks and enable nonlinear optical devices operating at the single-photon level. We demonstrate an integrated platform for scalable quantum nanophotonics based on silicon-vacancy (SiV) color centers coupled to nanoscale diamond devices. By placing SiV centers inside diamond photonic crystal cavities, we realize a quantum-optical switch controlled by a single color center. We control the switch using SiV metastable orbital states and verify optical switching at the single-photon level by using photon correlation measurements. We use Raman transitions to realize a single-photon source with a tunable frequency and bandwidth in a diamond waveguide. Finally, we create entanglement between two SiV centers by detecting indistinguishable Raman photons emitted into a single waveguide. Entanglement is verified using a novel superradiant feature observed in photon correlation measurements, paving the way for the realization of quantum networks.

quant-ph↗

NMR Technique for Determining the Depth of Shallow Nitrogen-Vacancy Centers in Diamond

We demonstrate a robust experimental method for determining the depth of individual shallow Nitrogen-Vacancy (NV) centers in diamond with $\sim1$ nm uncertainty. We use a confocal microscope to observe single NV centers and detect the proton nuclear magnetic resonance (NMR) signal produced by objective immersion oil, which has well understood nuclear spin properties, on the diamond surface. We determine the NV center depth by analyzing the NV NMR data using a model that describes the interaction of a single NV center with the statistically-polarized proton spin bath. We repeat this procedure for a large number of individual, shallow NV centers and compare the resulting NV depths to the mean value expected from simulations of the ion implantation process used to create the NV centers, with reasonable agreement.

quant-ph↗

Magnetic resonance detection of individual proton spins using a quantum reporter network

We demonstrate a method of magnetic resonance imaging with single nuclear-spin sensitivity under ambient conditions. It employs a network of isolated electronic-spin quantum bits (qubits) that act as quantum reporters on the surface of high purity diamond. The reporter spins are localized with nanometer-scale uncertainty, and their quantum state is coherently manipulated and measured optically via a proximal nitrogen-vacancy (NV) color center located a few nanometers below the diamond surface. The quantum reporter network is then used for sensing, coherent coupling and imaging individual proton spins on the diamond surface with angstrom resolution. This approach may enable direct structural imaging of complex molecules that cannot be accessed from bulk studies. It realizes a new platform for probing novel materials, monitoring chemical reactions, and manipulation of complex systems on surfaces at a quantum level.

quant-ph↗

Nanoscale NMR Spectroscopy and Imaging of Multiple Nuclear Species

Nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are well-established techniques that provide valuable information in a diverse set of disciplines but are currently limited to macroscopic sample volumes. Here we demonstrate nanoscale NMR spectroscopy and imaging under ambient conditions of samples containing multiple nuclear species, using nitrogen-vacancy (NV) colour centres in diamond as sensors. With single, shallow NV centres in a diamond chip and samples placed on the diamond surface, we perform NMR spectroscopy and one-dimensional MRI on few-nanometre-sized samples containing $^1$H and $^{19}$F nuclei. Alternatively, we employ a high-density NV layer near the surface of a diamond chip to demonstrate wide-field optical NMR spectroscopy of nanoscale samples containing $^1$H, $^{19}$F, and $^{31}$P nuclei, as well as multi-species two-dimensional optical MRI with sub-micron resolution. For all diamond samples exposed to air, we identify a ubiquitous $^1$H NMR signal, consistent with a $\sim 1$ nm layer of adsorbed hydrocarbons or water on the diamond surface and below any sample placed on the diamond. This work lays the foundation for nanoscale NMR and MRI applications such as studies of single proteins and functional biological imaging with subcellular resolution, as well as characterization of thin films with sub-nanometre resolution.

quant-ph↗

Multi-color correlative light and electron microscopy using nanoparticle cathodoluminescence

Correlative light and electron microscopy promises to combine molecular specificity with nanoscale imaging resolution. However, there are substantial technical challenges including reliable co-registration of optical and electron images, and rapid optical signal degradation under electron beam irradiation. Here, we introduce a new approach to solve these problems: multi-color imaging of stable optical cathodoluminescence emitted in a scanning electron microscope by nanoparticles with controllable surface chemistry. We demonstrate well-correlated cathodoluminescence and secondary electron images using three species of semiconductor nanoparticles that contain defects providing stable, spectrally-distinguishable cathodoluminescence. We also demonstrate reliable surface functionalization of the particles. The results pave the way for the use of such nanoparticles for targeted labeling of surfaces to provide nanoscale mapping of molecular composition, indicated by cathodoluminescence color, simultaneously acquired with structural electron images in a single instrument.

physics.ins-det↗

Tailoring Light-Matter Interaction with a Nanoscale Plasmon Resonator

We propose and demonstrate a new approach for achieving strong light-matter interactions with quantum emitters. Our approach makes use of a plasmon resonator composed of defect-free, highly crystalline silver nanowires surrounded by patterned dielectric distributed Bragg reflectors (DBRs). These resonators have an effective mode volume (Veff) two orders of magnitude below the diffraction limit and quality factor (Q) approaching 100, enabling enhancement of spontaneous emission rates by a factor exceeding 75 at the cavity resonance. We also show that these resonators can be used to convert a broadband quantum emitter to a narrowband single-photon source with color-selective emission enhancement.

cond-mat.mes-hall↗

Deterministic coupling of a single nitrogen vacancy center to a photonic crystal cavity

We describe and experimentally demonstrate a technique for deterministic coupling between a photonic crystal (PC) nanocavity and single emitters. The technique is based on in-situ scanning of a PC cavity over a sample and allows the positioning of the cavity over a desired emitter with nanoscale resolution. The power of the technique, which we term a Scanning Cavity Microscope (SCM), is demonstrated by coupling the PC nanocavity to a single nitrogen vacancy (NV) center in diamond, an emitter system that provides optically accessible electron and nuclear spin qubits.

quant-ph↗