arXiv subjects

Jennifer A. Dionne

Publications and source records attributed to Jennifer A. Dionne.

At least 37 records · Page 2Linked to original sources

arXiv2023

Millimeter-scale exfoliation of hBN with tunable flake thickness

As a two-dimensional (2D) dielectric material, hexagonal boron nitride (hBN) is in high demand for applications in photonics, nonlinear optics, and nanoelectronics. Unfortunately, the high-throughput preparation of macroscopic-scale, high-quality hBN flakes with controlled thickness is an ongoing challenge, limiting device fabrication and technological integration. Here, we present a metal thin-film exfoliation method to prepare hBN flakes with millimeter-scale dimension, near-unity yields, and tunable flake thickness distribution from 1-7 layers, a substantial improvement over scotch tape exfoliation. The single crystallinity and high quality of the exfoliated hBN are demonstrated with optical microscopy, atomic force microscopy, Raman spectroscopy, and second harmonic generation. We further explore a possible mechanism for the effectiveness and selectivity based on thin-film residual stress measurements, density functional theory calculations, and transmission electron microscopy imaging of the deposited metal films. We find that the magnitude of the residual tensile stress induced by thin film deposition plays a key role in determining exfoliated flake thickness in a manner which closely resembles 3D semiconductor spalling. Lastly, we demonstrate that our exfoliated, large-area hBN flakes can be readily incorporated as encapsulating layers for other 2D monolayers. Altogether, this method brings us one step closer to the high throughput, mass production of hBN-based 2D photonic, optoelectronic, and quantum devices.

cond-mat.mtrl-sci↗

arXiv2023

Achiral dielectric metasurfaces for spectral and polarization control of valley specific light emission from monolayer MoS2

Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically accessed and manipulated for quantum information processing. Here, we integrate MoS2 with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface Mie modes, the intensity and lifetime of the emission of neutral excitons, trions and defect bound excitons can be enhanced, while the spectral shape can be modified. Additionally, we demonstrate the symmetric enhancement of the degree-of-polarization (DOP) of neutral exciton and trions via valley-resolved PL measurements, and find that the DOP can be as high as 24% for exciton emission and 34% for trion emission at 100K. These results can be understood by analyzing the near-field impact of metasurface resonators on both the chiral absorption of MoS2 emitters as well as the enhanced emission from the Purcell effect. Combining Si-compatible photonic design with large-scale (mm-scale) 2D materials integration, our work makes an important step towards on-chip valleytronic applications approaching room-temperature operation.

physics.optics↗

arXiv2023

Solution-phase single-particle spectroscopy for probing multi-polaronic dynamics in quantum emitters at femtosecond resolution

The development of many optical quantum technologies depends on the availability of solid-state single quantum emitters with near-perfect optical coherence. However, a standing issue that limits systematic improvement is the significant sample heterogeneity and lack of mechanistic understanding of microscopic energy flow at the single emitter level and ultrafast timescales. Here we develop solution-phase single-particle pump-probe spectroscopy with photon correlation detection that captures sample-averaged dynamics in single molecules and/or defect states with unprecedented clarity at femtosecond resolution. We apply this technique to single quantum emitters in two-dimensional hexagonal boron nitride, which suffers from significant heterogeneity and low quantum efficiency. From millisecond to nanosecond timescales, the translation diffusion, metastable-state-related bunching shoulders, rotational dynamics, and antibunching features are disentangled by their distinct photon-correlation timescales, which collectively quantify the normalized two-photon emission quantum yield. Leveraging its femtosecond resolution, spectral selectivity and ultralow noise (two orders of magnitude improvement over solid-state methods), we visualize electron-phonon coupling in the time domain at the single defect level, and discover the acceleration of polaronic formation driven by multi-electron excitation. Corroborated with results from a theoretical polaron model, we show how this translates to sample-averaged photon fidelity characterization of cascaded emission efficiency and optical decoherence time. Our work provides a framework for ultrafast spectroscopy in single emitters, molecules, or defects prone to photoluminescence intermittency and heterogeneity, opening new avenues of extreme-scale characterization and synthetic improvements for quantum information applications.

cond-mat.mes-hall↗

arXiv2023

Combining acoustic bioprinting with AI-assisted Raman spectroscopy for high-throughput identification of bacteria in blood

Identifying pathogens in complex samples such as blood, urine, and wastewater is critical to detect infection and inform optimal treatment. Surface-enhanced Raman spectroscopy (SERS) and machine learning (ML) can distinguish among multiple pathogen species, but processing complex fluid samples to sensitively and specifically detect pathogens remains an outstanding challenge. Here, we develop an acoustic bioprinter to digitize samples into millions of droplets, each containing just a few cells, which are identified with SERS and ML. We demonstrate rapid printing of 2 pL droplets from solutions containing S. epidermidis, E. coli, and blood; when mixed with gold nanorods (GNRs), SERS enhancements of up to 1500x are achieved.We then train a ML model and achieve >=99% classification accuracy from cellularly-pure samples, and >=87% accuracy from cellularly-mixed samples. We also obtain >=90% accuracy from droplets with pathogen:blood cell ratios <1. Our combined bioprinting and SERS platform could accelerate rapid, sensitive pathogen detection in clinical, environmental, and industrial settings.

physics.bio-ph↗

arXiv2022

Accelerating quantum materials development with advances in transmission electron microscopy

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, quantum dots, color center hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the materials detailed atomic scale structure, including atomic defects, dopants, and lattice stacking. In this review, after introduction of different classes of quantum materials and quantum excitations, we describe how progress in the field of electron microscopy, including in situ and in operando EM, can accelerate advances in quantum materials. Our review describes EM methods including: i) principles and operation modes of EM, ii) EM spectroscopies, such as electron energy loss spectroscopy, cathodoluminescence, and electron energy gain spectroscopy, iii) 4D scanning transmission electron microscopy, iv) dynamic and ultrafast EM, v) complimentary ultrafast spectroscopies, and vi) atomic electron tomography. We discuss how these methods inform structure function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable high resolution manipulation of quantum materials. Among numerous results, our review highlights how EM has enabled identification of the 3D structure of quantum defects, measuring reversible and metastable dynamics of quantum excitations, mapping exciton states and single photon emission, measuring nanoscale thermal transport and coupled excitation dynamics, and measuring the internal electric field of quantum heterointerfaces, all at the quantum materials intrinsic atomic and near atomic-length scale.

cond-mat.mtrl-sci↗

arXiv2022

Rapid genetic screening with high quality factor metasurfaces

Genetic analysis methods are foundational to advancing personalized and preventative medicine, accelerating disease diagnostics, and monitoring the health of organisms and ecosystems. Current nucleic acid technologies such as polymerase chain reaction (PCR), next-generation sequencing (NGS), and DNA microarrays rely on fluorescence and absorbance, necessitating sample amplification or replication and leading to increased processing time and cost. Here, we introduce a label-free genetic screening platform based on high quality (high-Q) factor silicon nanoantennas functionalized with monolayers of nucleic acid fragments. Each nanoantenna exhibits substantial electromagnetic field enhancements with sufficiently localized fields to ensure isolation from neighboring resonators, enabling dense biosensor integration. We quantitatively detect complementary target sequences using DNA hybridization simultaneously for arrays of sensing elements patterned at densities of 160,000 pixels per cm$^2$. In physiological buffer, our nanoantennas exhibit average resonant quality factors of 2,200, allowing detection of two gene fragments, SARS-CoV-2 envelope (E) and open reading frame 1b (ORF1b), down to femtomolar concentrations. We also demonstrate high specificity sensing in clinical nasopharyngeal eluates within 5 minutes of sample introduction. Combined with advances in biomarker isolation from complex samples (e.g., mucus, blood, wastewater), our work provides a foundation for rapid, compact, amplification-free and high throughput multiplexed genetic screening assays spanning medical diagnostics to environmental monitoring.

physics.optics↗

arXiv2022

High quality factor silicon-on-lithium niobate metasurfaces for electro-optically reconfigurable wavefront shaping

Dynamically reconfigurable metasurfaces promise compact and lightweight spatial light modulation for many applications, including LiDAR, AR/VR, and LiFi systems. Here, we design and computationally investigate high quality factor silicon-on-lithium niobate metasurfaces with electrically-driven, independent control of its constituent nanobars for full phase tunability with high tuning efficiency. Free-space light couples to guided modes within each nanobar via periodic perturbations, generating quality factors exceeding 30,000, while maintaining bar spacing <$λ$/1.5. We achieve nearly 2$π$ phase variation with an applied bias not exceeding $\pm$ 25 V, maintaining reflection efficiency above 91%. Using full-field simulations, we demonstrate a high angle, 51°, switchable beamsplitter with a diffracted efficiency of 93%, and an angle-tunable beamsteerer, spanning 18-31°, with up to 86% efficiency, all using the same metasurface device. Our platform provides a foundation for highly efficient wavefront shaping devices with a wide dynamic tuning range capable of generating nearly any transfer function.

physics.optics↗

arXiv2022

Nanodiamond grain boundaries and lattice expansion drive Silicon vacancy emission heterogeneity

Silicon-vacancy (SiV$^-$) centers in diamond are promising candidates as sources of single-photons in quantum networks due to their minimal phonon coupling and narrow optical linewidths. Correlating SiV$^-$ emission with the defect's atomic-scale structure is important for controlling and optimizing quantum emission, but remains an outstanding challenge. Here, we use cathodoluminescence imaging in a scanning transmission electron microscope (STEM) to elucidate the structural sources of non-ideality in the SiV$^-$ emission from nanodiamonds with sub-nanometer-scale resolution. We show that different crystalline domains of a nanodiamond exhibit distinct zero-phonon line (ZPL) energies and differences in brightness, while near-surface SiV$^-$ emitters remain bright. We correlate these changes with local lattice expansion using 4D STEM and diffraction, and show that associated blue shifts from the ZPL are due to defect density heterogeneity, while red shifts are due to lattice distortions.

physics.app-ph↗

arXiv2021

Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in nanocrystals are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in semiconductor nanocrystals. Investigation of the excitation energy dependence shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap result in transient lattice heating that occurs on a much longer 200 ps timescale, governed by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.

cond-mat.mes-hall↗

arXiv2020

Fluorescence-Detected Circular Dichroism of a Chiral Molecular Monolayer with Dielectric Metasurfaces

Strong enhancement of molecular circular dichroism has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost circular dichroism. We use fluorescence-detected circular dichroism spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk arrays. Importantly, the molecules and nanodisk antennas have spectrally-coincident resonances, and our fluorescence technique allows us to deconvolute absorption in the nanodisks from the molecules. We find that enhanced fluorescence-detected circular dichroism signals depend on nanophotonic resonances in good agreement with simulated differential absorption and optical chirality density, while no signal is detected from molecules adsorbed on featureless silicon surfaces. These results verify the potential of nanophotonic platforms to be used for asymmetric photolysis with lower energy requirements

physics.optics↗

arXiv2020

Electron and Light Induced Stimulated Raman Spectroscopy for Nanoscale Molecular Mapping

We propose and theoretically analyze a new vibrational spectroscopy, termed electron- and light-induced stimulated Raman (ELISR) scattering, that combines the high spatial resolution of electron microscopy with the molecular sensitivity of surface-enhanced Raman spectroscopy. With ELISR, electron-beam excitation of plasmonic nanoparticles is utilized as a spectrally-broadband but spatially-confined Stokes beam in the presence of a diffraction-limited pump laser. To characterize this technique, we develop a numerical model and conduct full-field electromagnetic simulations to investigate two distinct nanoparticle geometries, nanorods and nanospheres, coated with a Raman-active material. Our results show the significant ($10^6$-$10^7$) stimulated Raman enhancement that is achieved with dual electron and optical excitation of these nanoparticle geometries. Importantly, the spatial resolution of this vibrational spectroscopy for electron microscopy is solely determined by the nanoparticle geometry and the plasmon mode volume. Our results highlight the promise of ELISR for simultaneous high-resolution electron microscopy with sub-diffraction-limited Raman spectroscopy, complementing advances in superresolution microscopy, correlated light and electron microscopy, and vibrational electron energy loss spectroscopy.

physics.optics↗

arXiv2020

Surface-Enhanced Circular Dichroism spectroscopy on periodic dual nanostructures

Increasing the sensitivity of chiral spectroscopic techniques such as circular dichroism (CD) spectroscopy is a current aspiration in the research field of nanophotonics. Enhancing CD spectroscopy depends upon of two complementary requirements: the enhancement of the electromagnetic fields perceived by the molecules under study and the conservation of the helicity of those fields, guaranteed by duality symmetry. In this work, we introduce a systematic method to design nanostructured dual periodic photonic systems capable of enhancing molecular CD spectroscopy resonantly. As an illustration, we engineer a dual 1D silicon nanoparticle array and show that its collective optical modes can be efficiently employed to resonantly enhance by two orders of magnitude the local density of optical chirality and, thus, the CD signal obtained from a given molecular sample on its vicinity.

physics.optics↗

arXiv2018

Bright sub-20 nm cathodoluminescent nanoprobes for multicolor electron microscopy

Electron microscopy (EM) has been instrumental in our understanding of biological systems ranging from subcellular structures to complex organisms. Although EM reveals cellular morphology with nanoscale resolution, it does not provide information on the location of proteins within a cellular context. An EM-based bioimaging technology capable of localizing individual proteins and resolving protein-protein interactions with respect to cellular ultrastructure would provide important insights into the molecular biology of a cell. Here, we report on the development of luminescent nanoprobes potentially suitable for labeling biomolecules in a multicolor EM modality. In this approach, the labels are based on lanthanide-doped nanoparticles that emit light under electron excitation in a process known as cathodoluminescence (CL). Our results suggest that the optimization of nanoparticle composition, synthesis protocols and electron imaging conditions could enable high signal-to-noise localization of biomolecules with a sub-20-nm resolution, limited only by the nanoparticle size. In ensemble measurements, these luminescent labels exhibit narrow spectra of nine distinct colors that are characteristic of the corresponding rare-earth dopant type.

cond-mat.mtrl-sci↗

arXiv2016

Towards nanoscale multiplexing with parity-time symmetric plasmonic coaxial waveguides

We theoretically investigate a nanoscale mode-division multiplexing scheme based on parity-time (PT) symmetric coaxial plasmonic waveguides. Coaxial waveguides support paired degenerate modes corresponding to distinct orbital angular momentum states. PT symmetric inclusions of gain and loss break the degeneracy of the paired modes and create new hybrid modes without orbital angular momentum. This process can be made thresholdless by matching the mode order with the number of gain and loss sections within the coaxial ring. Using both a Hamiltonian formulation and degenerate perturbation theory, we show how the wavevectors and fields evolve with increased loss/gain and derive sufficient conditions for thresholdless transitions. As a multiplexing filter, this PT symmetric coaxial waveguide could help double density rates in on-chip nanophotonic networks.

physics.optics↗

arXiv2015

Photon Upconversion with Hot Carriers in Plasmonic Systems

We propose a novel scheme of photon upconversion based on harnessing the energy of plasmonic hot carriers. Low-energy photons excite hot electrons and hot holes in a plasmonic nanoparticle, which are then injected into an adjacent semiconductor quantum well where they radiatively recombine to emit a photon of higher energy. We theoretically study the proposed upconversion scheme using Fermi-liquid theory and determine the upconversion quantum efficiency to be as high as 25% in 5 nm silver nanocubes. This upconversion scheme is linear in its operation, does not require coherent illumination, offers spectral tunability, and is more efficient than conventional upconverters.

physics.optics↗

arXiv2014

Controlling electric, magnetic, and chiral dipolar emission with PT-symmetric potentials

We investigate the effect of parity-time (PT)-symmetric optical potentials on the radiation of achiral and chiral emitters. Mode coalescence and the appearance of exceptional points lead to orders-of-magnitude enhancements in the emitted dipole power. Further, the emitter can be tuned to behave as a strong optical source or absorber based on the non-Hermiticity parameter. Chiral enantiomers radiating near PT metamaterials exhibit a 4.5-fold difference in their decay rate. The results of this work could enable new atom-cavity interactions for quantum optics, as well as all- optical enantio-specific separation.

physics.optics↗

arXiv2013

PT-Symmetric Plasmonic Metamaterials

We theoretically investigate the optical properties of parity-time (PT)-symmetric three dimensional metamaterials composed of strongly-coupled planar plasmonic waveguides. By tuning the loss-gain balance, we show how the initially isotropic material becomes both asymmetric and unidirectional. The highly tunable optical dispersion of PT -symmetric metamaterials provides a foundation for designing an entirely new class of three-dimensional bulk synthetic media, with applications ranging from sub-diffraction-limited optical lenses to non-reciprocal nanophotonic devices.

physics.optics↗

arXiv2012

Narrow-bandwidth solar upconversion: design principles, efficiency limits, and case studies

We employ a detailed balance approach to model a single-junction solar cell with a realistic narrow-band, non-unity-quantum-yield upconverter. As upconverter bandwidths are increased from 0 to 0.5 eV, maximum cell efficiencies increase from the Shockley-Queisser limit of 30.58% to over 43%. Such efficiency enhancements are calculated for upconverters with near-infrared spectral absorption bands, readily accessible with existing upconverters. While our model shows that current bimolecular and lanthanide-based upconverting materials will improve cell efficiencies by <1%, cell efficiencies can increase by several absolute percent with increased upconverter quantum yield - even without an increased absorption bandwidth. By examining the efficiency limits of a highly realistic solar cell-upconverter system, our model provides a platform for optimizing future solar upconverter designs.

physics.optics↗