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Mark L. Brongersma

Publications and source records attributed to Mark L. Brongersma.

At least 19 recordsLinked to original sources

Nonresonant optomechanical control of structural phases

Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties.

physics.optics↗

Interfacial control of hot-carrier extraction and photostability in two-dimensional materials

Two-dimensional transition metal dichalcogenides (TMDCs) are promising materials for next-generation optoelectronic devices, yet their implementation is hindered by limited sample stability and challenges in forming reliable electrical contacts. Here, by utilizing time-domain THz emission spectroscopy we directly probe charge carrier dynamics in monolayer WS2 on gold (Au) and fused silica (SiO2) as a function of interface morphology. For laser excitation above the band gap of WS2, we independently extract effective transport times for both electrons and holes and find that discontinuous WS2 contacts on rough Au generate larger net photocurrents than uniform, strongly coupled interfaces - a counterintuitive observation attributed to imbalanced electron and hole transfer from WS2 to Au. Crucially, we demonstrate that ultrafast charge extraction and separation suppress recombination-driven energy release and thereby prevent photo-induced degradation under ambient conditions, eliminating the need for encapsulation. These findings redefine interfacial design as a central control parameter for both performance and stability in 2D optoelectronic devices.

cond-mat.mtrl-sci↗

Hybrid-2D Excitonic Metasurfaces for Complex Amplitude Modulation

Dynamic control of visible light is crucial for technologies such as holographic displays and adaptive optics. Passive metasurfaces can shape wavefronts at the subwavelength scale and active metasurfaces promise to extend this functionality into the temporal domain. However, existing metasurfaces for dynamic phase manipulation typically cannot deliver phase modulation across a broad range without causing variations in the scattering amplitude. Here, we use an inverse-design pipeline to numerically demonstrate a hybrid-2D excitonic metasurface platform offering independent amplitude and phase control in the visible regime. Harnessing the gate-tunable excitonic response of monolayer WS2 retrieved from experiments, we design a pi-phase modulator with a uniform amplitude profile. Adding a second tunable monolayer, we achieve independent control of the amplitude and phase over the full 0-2pi phase range, which we leverage for a reconfigurable beam-steering metadevice. Our results demonstrate how hybrid-2D excitonic metasurfaces enable electrically tunable wavefront shaping in the visible regime.

physics.optics↗

Temperature-dependent excitonic light manipulation with atomically-thin optical elements

Monolayer 2D semiconductors, such as WS2, exhibit uniquely strong light-matter interactions due to exciton resonances that enable atomically-thin optical elements. Similar to geometry-dependent plasmon and Mie resonances, these intrinsic material resonances offer coherent and tunable light scattering. Thus far, the impact of the excitons temporal dynamics on the performance of such excitonic metasurfaces remains unexplored. Here, we show how the excitonic decay rates dictate the focusing efficiency of an atomically-thin lens carved directly out of exfoliated monolayer WS2. By isolating the coherent exciton radiation from the incoherent background in the focus of the lens, we obtain a direct measure of the role of exciton radiation in wavefront shaping. Furthermore, we investigate the influence of exciton-phonon scattering by characterizing the focusing efficiency as a function of temperature, demonstrating an increased optical efficiency at cryogenic temperatures. Our results provide valuable insights in the role of excitonic light scattering in 2D nanophotonic devices.

physics.optics↗

Acoustic wave modulation of gap plasmon cavities

The role of metallic nanostructures in nanophotonics is expected to expand if ways to electrically manipulate their optical resonances at high speed can be identified. Here, we capitalize on electrically-driven surface acoustic waves and the extreme light concentration afforded by gap plasmons to achieve this goal. We place gold nanoparticles in a particle-on-mirror configuration with a few-nanometer-thick, compressible polymer spacer. Surface acoustic waves are then used to tune light scattering at speeds approaching the GHz regime. We observe evidence that the surface acoustic waves produce mechanical deformations in the polymer, and that ensuing nonlinear mechanical dynamics lead to unexpectedly large levels of strain and spectral tuning. Our approach provides a design strategy for electrically driven dynamic metasurfaces and fundamental explorations of high-frequency, polymer dynamics in ultra-confined geometries.

physics.optics↗

Apparent Resonance Splitting in Self-Coupled Excitonic Systems

Thin films of high-refractive-index excitonic materials enable self-coupling by simultaneously supporting intrinsic excitonic transitions and optical resonances. These optical resonances take the form of Fabry-Perot resonances in thick films and absorption resonances in ultrathin films placed on metallic substrates. Here, we investigate whether these optical resonances lead to true exciton-photon hybridization. Using far-field reflectance and spectrally resolved photocurrent measurements, we study tungsten disulfide (WS$_2$) flakes on both metallic and dielectric substrates across a range of thicknesses. While reflectance spectra for ultrathin flakes exhibit resonance splitting between excitons and absorption resonances, our photocurrent measurements reveal only excitonic peaks, indicating that no polaritons are formed. In contrast, thicker flakes exhibit Fabry-Perot resonances that strongly couple to excitons, resulting in clear splitting in both reflectance and photocurrent spectra, and providing evidence of polariton formation. We further show that the polariton resonances can be tuned through the reflection phase at the WS$_2$-substrate interface by changing the substrate material. In addition to coupling with the strong A-exciton, we observe polariton formation involving the weaker B-exciton at shorter wavelengths, as well as higher-order hybridization where both excitons interact simultaneously with a single Fabry-Perot resonance. These findings clarify the distinction between apparent and true strong coupling in excitonic materials and demonstrate how reflection phase and flake thickness can be used to engineer light-matter interactions.

physics.optics↗

Roadmap on Nonlocality in Photonic Materials and Metamaterials

Photonic technologies continue to drive the quest for new optical materials with unprecedented responses. A major frontier in this field is the exploration of nonlocal (spatially dispersive) materials, going beyond the local, wavevector-independent assumption traditionally made in optical material modeling. On one end, the growing interest in plasmonic, polaritonic and quantum materials has revealed naturally occurring nonlocalities, emphasizing the need for more accurate models to predict and design their optical responses. This has major implications also for topological, nonreciprocal, and time-varying systems based on these material platforms. Beyond natural materials, artificially structured materials--metamaterials and metasurfaces--can provide even stronger and engineered nonlocal effects, emerging from long-range interactions or multipolar effects. This is a rapidly expanding area in the field of photonic metamaterials, with open frontiers yet to be explored. In the case of metasurfaces, in particular, nonlocality engineering has become a powerful tool for designing strongly wavevector-dependent responses, enabling enhanced wavefront control, spatial compression, multifunctional devices, and wave-based computing. Furthermore, nonlocality and related concepts play a critical role in defining the ultimate limits of what is possible in optics, photonics, and wave physics. This Roadmap aims to survey the most exciting developments in nonlocal photonic materials, highlight new opportunities and open challenges, and chart new pathways that will drive this emerging field forward--toward new scientific discoveries and technological advancements.

cond-mat.mes-hall↗

GHz-speed wavefront shaping metasurface modulators enabled by resonant electro-optic nanoantennas

Electrically tunable metasurfaces that control the amplitude and phase of light through biasing of nanoscale antennas present a route to compact, sub-micron thick modulator devices. However, most platforms face limitations in bandwidth, absolute optical efficiency, and tuning response. Here, we present electro-optically tunable metasurfaces capable of both GHz amplitude modulation and transmissive wavefront shaping in the telecom range. Our resonant electro-optic nanoantenna design consists of a silicon nanobar atop thin-film lithium niobate, with gold electrodes. The silicon nanobar is a periodically perturbed optical waveguide that supports high quality factor (Q $>$ 1000) guided mode resonances excited with free space light. Applying a voltage bias to the lithium niobate tunes its refractive index, modulating the resonant behavior of the silicon nanobar through evanescent mode overlap. We demonstrate an absolute transmittance modulation of 7.1% with $\pm$5 V applied voltage, and show the dependence of this modulation behavior on the resonance quality factor. We additionally study the electrode limitations on modulation bandwidth, demonstrating bandwidths exceeding 800 MHz. Finally, we show how this resonant antenna platform can be used to design wavefront shaping metasurfaces. We demonstrate a beamsplitting metasurface device, whose diffraction efficiency can be modulated with a bandwidth of 1.03 GHz. The high-speed modulation and wavefront control capabilities of this platform provide a foundation for compact, high bandwidth free space communications and sensing devices.

physics.optics↗

Highly efficient, tunable, electro-optic metasurfaces based on quasi-bound states in the continuum

Ultrafast and highly efficient dynamic optical metasurfaces enabling truly spatiotemporal control over optical radiation are poised to revolutionize modern optics and photonics, but their practical realization remains elusive. In this work, we demonstrate highly efficient electro-optic metasurfaces based on quasi-bound states in the continuum (qBIC) operating in reflection that are amenable for ultrafast operation and thereby spatiotemporal control over reflected optical fields. The material configuration consists of a lithium niobate thin film sandwiched between an optically thick gold back-reflector and a grating of gold nanoridges also functioning as control electrodes. Metasurfaces for optical free-space intensity modulation are designed by utilizing the electro-optic Pockels effect in combination with an ultra-narrow qBIC resonance, whose wavelength can be finely tuned by varying the angle of light incidence. The fabricated electro-optic metasurfaces operate at telecom wavelengths with the modulation depth reaching 95 % (modulating thereby 35 % of the total incident power) for a bias voltage of +/-30 V within the electrical bandwidth of 125 MHz. Leveraging the highly angle-dependent qBIC resonance realized, we demonstrate electrically tunable phase contrast imaging using the fabricated metasurface. Moreover, given the potential bandwidth of 39 GHz estimated for the metasurface pixel size of 22 $μ$m, the demonstrated electro-optic metasurfaces promise successful realization of unique optical functions, such as harmonic beam steering and spatiotemporal shaping as well as nonreciprocal operation.

physics.optics↗

High-throughput antibody screening with high-quality factor nanophotonics and bioprinting

Empirical investigation of the quintillion-scale, functionally diverse antibody repertoires that can be generated synthetically or naturally is critical for identifying potential biotherapeutic leads, yet remains burdensome. We present high-throughput nanophotonics- and bioprinter-enabled screening (HT-NaBS), a multiplexed assay for large-scale, sample-efficient, and rapid characterization of antibody libraries. Our platform is built upon independently addressable pixelated nanoantennas exhibiting wavelength-scale mode volumes, high-quality factors (high-Q) exceeding 5000, and pattern densities exceeding one million sensors per square centimeter. Our custom-built acoustic bioprinter enables individual sensor functionalization via the deposition of picoliter droplets from a library of capture antigens at rates up to 25,000 droplets per second. We detect subtle differentiation in the target binding signature through spatially-resolved spectral imaging of hundreds of resonators simultaneously, elucidating antigen-antibody binding kinetic rates, affinity constant, and specificity. We demonstrate HT-NaBS on a panel of antibodies targeting SARS-CoV-2, Influenza A, and Influenza B antigens, with a sub-picomolar limit of detection within 30 minutes. Furthermore, through epitope binning analysis, we demonstrate the competence and diversity of a library of native antibodies targeting functional epitopes on a priority pathogen (H5N1 bird flu) and on glycosylated therapeutic Cetuximab antibodies against epidermal growth factor receptor. With a roadmap to image tens of thousands of sensors simultaneously, this high-throughput, resource-efficient, and label-free platform can rapidly screen for high-affinity and broad epitope coverage, accelerating biotherapeutic discovery and de novo protein design.

physics.optics↗

Routing Light Emission from Monolayer MoS$_2$ by Mie Resonances of Crystalline Silicon Nanospheres

A dielectric Mie-resonant nanoantenna is capable of controlling the directionality of the emission from nearby quantum emitters through the excitation of multiple degenerate Mie resonances. A crystalline silicon nanosphere (Si NS) is a promising candidate for a dielectric nanoantenna because crystalline Si has a large refractive index (3.8 at 650 nm) and the small imaginary part of a complex refractive index (0.015 at 650 nm) as an optical material. In this work, we control the emission directionality of excitons supported by monolayer transition metal dichalcogenides (1L-TMDCs) using a Si NS. We first discuss the condition to extract the emission preferentially towards the Si NS side from the analytical calculations. We then study the photoluminescence (PL) of 1L-TMDCs on which differently sized single Si NSs are placed. We show that the PL spectral shape strongly depends on the emission direction, and that the emission toward the Si NS side (top) with respect to the opposite side (bottom) is the largest at wavelengths between the magnetic dipole and electric dipole Mie resonances of a Si NS. Finally, we quantitatively discuss the spectral shape of the top-to-bottom ratio from numerical simulations.

physics.optics↗

Ion-Assisted Nanoscale Material Engineering in Atomic Layers

Achieving deterministic control over the properties of low-dimensional materials with nanoscale precision is a long-sought goal. Mastering this capability has a transformative impact on the design of multifunctional electrical and optical devices. Here, we present an ion-assisted synthetic technique that enables precise control over the material composition and energy landscape of two-dimensional (2D) atomic crystals. Our method transforms binary transition metal dichalcogenides (TMDs), like MoSe$_2$, into ternary MoS$_{2α}$Se$_{2(1-α})$ alloys with systematically adjustable compositions, $α$. By piecewise assembly of the lateral, compositionally modulated MoS$_{2α}$Se$_{2(1-α)}$ segments within 2D atomic layers, we present a synthetic pathway towards the realization of multi-compositional designer materials. Our technique enables the fabrication of complex structures with arbitrary boundaries, dimensions as small as 30 nm, and fully customizable energy landscapes. Our optical characterizations further showcase the potential for implementing tailored optoelectronics in these engineered 2D crystals.

cond-mat.mtrl-sci↗

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↗

Tunable vector beam decoder by inverse design for high-dimensional quantum key distribution with 3D polarized spatial modes

Spatial modes of light have become highly attractive to increase the dimension and, thereby, security and information capacity in quantum key distribution (QKD). So far, only transverse electric field components have been considered, while longitudinal polarization components have remained neglected. Here, we present an approach to include all three spatial dimensions of electric field oscillation in QKD by implementing our tunable, on-a-chip vector beam decoder (VBD). This inversely designed device pioneers the "preparation" and "measurement" of three-dimensionally polarized mutually unbiased basis states for high-dimensional (HD) QKD and paves the way for the integration of HD QKD with spatial modes in multifunctional on-a-chip photonics platforms.

physics.optics↗

Impact of substrates and quantum effects on exciton line shapes of 2D semiconductors at room temperature

Exciton resonances in monolayer transition-metal dichalcogenides (TMDs) provide exceptionally strong light-matter interaction at room temperature. Their spectral line shape is critical in the design of a myriad of optoelectronic devices, ranging from solar cells to quantum information processing. However, disorder resulting from static inhomogeneities and dynamical fluctuations can significantly impact the line shape. Many recent works experimentally evaluate the optical properties of TMD monolayers placed on a substrate and the line shape is typically linked directly to the material's quality. Here, we highlight that the interference of the substrate and TMD reflections can strongly influence the line shape. We further show how basic, room-temperature reflection measurement allow investigation of the quantum mechanical exciton dynamics by systematically controlling the substrate reflection with index-matching oils. By removing the substrate contribution with a properly chosen oil, we can extract the excitonic decay rates including the quantum mechanical dephasing rate. The results provide valuable guidance for the engineering of exciton line shapes in layered nanophotonic systems.

cond-mat.mes-hall↗

Quantum Analog of Vibration Isolation: From Room Temperature Superfluorescence to High Temperature Superconductivity

The development and the use of quantum technologies are hindered by a fundamental challenge: Quantum materials exhibit macroscopic quantum properties at extremely low temperatures due to the loss of quantum coherence at elevated temperatures. Here, based on our recent discovery of room temperature superfluorescence in perovskites, we present the Quantum Analog of Vibration Isolation, 'QAVI', model and explain how it protects the quantum phase against dephasing at high temperatures. We then postulate the requirements for observation of macroscopic quantum phenomena at practical temperatures and propose a unified model for all macroscopic quantum phase transitions. We further present the general features of the temperature and density phase diagram of macroscopic quantum phase transitions that are mediated by the QAVI process and identify the similarities observed in the phase diagram of high Tc superconductors. Understanding this fundamental quantum coherence protection mechanism is imperative to accelerate the discovery of high temperature macroscopic quantum phenomena, and offers significant potential for developing quantum technologies functioning under practical conditions.

cond-mat.supr-con↗

High-Specific-Power Flexible Transition Metal Dichalcogenide Solar Cells

Semiconducting transition metal dichalcogenides (TMDs) are promising for flexible high-specific-power photovoltaics due to their ultrahigh optical absorption coefficients, desirable band gaps and self-passivated surfaces. However, challenges such as Fermi-level pinning at the metal contact-TMD interface and the inapplicability of traditional doping schemes have prevented most TMD solar cells from exceeding 2% power conversion efficiency (PCE). In addition, fabrication on flexible substrates tends to contaminate or damage TMD interfaces, further reducing performance. Here, we address these fundamental issues by employing: 1) transparent graphene contacts to mitigate Fermi-level pinning, 2) $\rm{MoO}_\it{x}$ capping for doping, passivation and anti-reflection, and 3) a clean, non-damaging direct transfer method to realize devices on lightweight flexible polyimide substrates. These lead to record PCE of 5.1% and record specific power of $\rm{4.4\ W\,g^{-1}}$ for flexible TMD ($\rm{WSe_2}$) solar cells, the latter on par with prevailing thin-film solar technologies cadmium telluride, copper indium gallium selenide, amorphous silicon and III-Vs. We further project that TMD solar cells could achieve specific power up to $\rm{46\ W\,g^{-1}}$, creating unprecedented opportunities in a broad range of industries from aerospace to wearable and implantable electronics.

physics.app-ph↗

Nonlocal metasurfaces for spectrally decoupled wavefront manipulation and eye tracking

Metasurface-based optical elements typically manipulate light waves by imparting space-variant changes in the amplitude and phase with a dense array of scattering nanostructures. The highly-localized and low optical-quality-factor (Q) modes of nanostructures are beneficial for wavefront-shaping as they afford quasi-local control over the electromagnetic fields. However, many emerging imaging, sensing, communication, display, and non-linear optics applications instead require flat, high-Q optical elements that provide notable energy storage and a much higher degree of spectral control over the wavefront. Here, we demonstrate high-Q, nonlocal metasurfaces with atomically-thin metasurface elements that offer notably enhanced light-matter interaction and fully-decoupled optical functions at different wavelengths. We illustrate a possible use of such a flat optic in eye tracking for eye-wear. Here, a metasurface patterned on a regular pair of eye-glasses provides an unperturbed view of the world across the visible spectrum and redirects near-infrared light to a camera to allow imaging of the eye.

physics.optics↗