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Vahagn Mkhitaryan

Publications and source records attributed to Vahagn Mkhitaryan.

18 recordsLinked to original sources

Pathway to Optical-Cycle Dynamic Photonics: Extreme Electron Temperatures in Transparent Conducting Oxides

We theoretically demonstrate that transparent conducting oxides (TCOs) exhibit oscillatory and sign-reversing dynamic modulation in transmittance on the order of a few optical cycles under extreme electron temperatures, providing a possible explanation for TCO dynamics observed in earlier experiments. We present an inverse-designed multilayer cavity incorporating an ultrathin TCO layer, which supports an oscillatory optical response more pronounced than those previously observed experimentally in TCOs. This approach yields transmittance oscillations with a characteristic period of ~20fs, which corresponds to approximately four optical cycles of the 1.431μm probe beam. To achieve a similar oscillatory modulation in Δn, we incorporate a TCO electron-acceptor layer on top of the inverse-designed cavity, enabling thermionic carrier injection at the TCO junction. The resulting acceptor layer exhibits a striking Δn response as fast as 20fs, corresponding to only three optical cycles of the 1.8-2.0μm probe, and can be further tailored into the sub-optical-cycle regime. The findings could both clarify the previously unexplained transient dynamics in TCOs and, for the first time, demonstrate the critical role of electron temperatures in driving oscillatory dynamic responses.

physics.optics

Inverse-Designed Superchiral Hot Spot in Dielectric Meta-Cavity for Ultra-Compact Enantioselective Detection

Chiral nanophotonic structures have garnered considerable interest in recent years due to their potential to enhance the efficacy of chirality-sensitive biomolecular detection. Designing metaplatforms to enhance chiroptical signals under linearly polarized excitation is particularly appealing due to the minimal chiral background and the ease of controlling excitation polarization. Here, a novel two-step inverse design scheme for dielectric lossless metasurfaces with superchiral hot spots is proposed. The method extends the local density of field enhancements for non-chiral fields into the chiral regime and significantly surpasses previous enhancements in super-chiral field generation. It has been demonstrated that by leveraging the excitation of high quality factor modes with small mode volumes, it is theoretically possible to convert linearly polarized plane waves into a superchiral hot spot with record-high enhancement in the near-field optical chirality up to 104. A prototype is successfully implemented using advanced nanofabrication technologies. The optical characterization of the prototype demonstrates a 102-fold enhancement in optical chirality. The findings of this study unveil novel prospects for chiral spectroscopy with ultra-compact devices, underscoring the role of machine learning and physics-based inverse design in the development of cutting-edge, functional photonic structures.

physics.optics

Topology-Optimized Dielectric Cavities for Enhanced Excitonic Light Emission from $\rm WSe_{2}$

Photonic inverse design and, especially, topology optimization, enable dielectric cavities with deeply sub-diffraction mode volumes and high quality factors, thus offering a powerful platform for enhanced light-matter coupling. Here, we design and fabricate arrays of CMOS-compatible silicon cavities on sapphire with extreme subwavelength transverse mode sizes of only 30-40 nm ($\rm V\simλ^3/2500$). These cavities are engineered for deterministic coupling to a monolayer (or few-layer) excitonic material, producing strong near-field localization directly beneath the 2D material. Photoluminescence (PL) measurements show reproducible tenfold enhancements relative to bare silicon, consistent with numerical simulations that account for material absorption and fabrication tolerances. Furthermore, time-resolved PL measurements reveal pronounced lifetime shortening and non-exponential dynamics, indicating cavity-mediated exciton-exciton interactions. The optimized cavity geometry enhances the far-field collection efficiency and supports scalable integration with van der Waals semiconductors. Our results show that the arrays of topology-optimized dielectric cavities are a versatile, scalable platform for controlling excitonic emission and interactions, which creates new opportunities in nonlinear optics, optoelectronics, and quantum photonics.

physics.optics

Atomically thin silver films for enhanced nanoscale nonlinear optics

The inherently weak nonlinear optical response of bulk materials remains a fundamental limitation in advancing photonic technologies. Nanophotonics addresses this challenge by tailoring the size and morphology of nanostructures to manipulate the optical near field, thus modulating the nonlinear response. Here, we explore a complementary strategy based on engineering the electronic band structure in the mesoscopic regime to enhance optical nonlinearities. Specifically, we demonstrate an increase in second-harmonic generation (SHG) from crystalline silver films as their thickness is reduced down to just a few atomic monolayers. Operating at the boundary between bulk and two-dimensional systems, these ultra-thin films exhibit a pronounced enhancement of SHG with decreasing thickness. This enhancement stems from quantum confinement effects that modify the interaction between electronic states and incident light, which we explain based on quantum-mechanical calculation. Our atomically-thin crystalline silver films provide a new means to overcome the small interaction volumes inherent to nanophotonic platforms, enabling efficient nanoscale nonlinear optics with potential applications in photonics, sensing, and quantum technologies.

physics.optics

In situ engineering hexagonal boron nitride in van der Waals heterostructures with selective SF6 etching

Van der Waals heterostructures are at the forefront in materials heterostructure engineering, offering the ultimate control in layer selectivity and capability to combine virtually any material. Hexagonal boron nitride (hBN), the most commonly used dielectric material, has proven indispensable in this field, allowing the encapsulation of active 2D materials preserving their exceptional electronic quality. However, not all device applications require full encapsulation but rather require open surfaces, or even selective patterning of hBN layers. Here, we report on a procedure to engineer top hBN layers within van der Waals heterostructures while preserving the underlying active 2D layers. Using a soft selective SF6 etching combined with a series of pre and post-etching treatments, we demonstrate that pristine surfaces can be exposed with atomic flatness while preserving the active layers electronic quality. We benchmark our technique using graphene encapsulated with hBN Hall bar devices. Using Raman spectroscopy combined with quantum transport, we show high quality can be preserved in etched regions by demonstrating low temperature carrier mobilities of 200,000 cm2Vs-1, ballistic transport probed through magnetic focusing, and intrinsic room temperature phonon-limited mobilities. Atomic force microscopy brooming and O2 plasma cleaning are identified as key pre-etching steps to obtaining pristine open surfaces while preserving electronic quality. The technique provides a clean method for opening windows into mesoscopic van der Waals devices that can be used for local probe experiments, patterning top hBN in situ, and exposing 2D layers to their environment for sensing applications.

cond-mat.mes-hall

Bottom-up Fabrication of 2D Rydberg Exciton Arrays in Cuprous Oxide

Solid-state platforms provide exceptional opportunities for advancing on-chip quantum technologies by enhancing interaction strengths through coupling, scalability, and robustness. Cuprous oxide ($\text{Cu}_{2}\text{O}$) has recently emerged as a promising medium for scalable quantum technology due to its high-lying Rydberg excitonic states, akin to those in hydrogen atoms. To harness these nonlinearities for quantum applications, the confinement dimensions must match the Rydberg blockade size, which can reach several microns in $\text{Cu}_{2}\text{O}$. Using a CMOS-compatible growth technique, this study demonstrates the bottom-up fabrication of site-selective arrays of $\text{Cu}_{2}\text{O}$ microparticles. We observed Rydberg excitons up to the principal quantum number $n$=5 within these $\text{Cu}_{2}\text{O}$ arrays on a quartz substrate and analyzed the spatial variation of their spectrum across the array, showing robustness and reproducibility on a large chip. These results lay the groundwork for the deterministic growth of $\text{Cu}_{2}\text{O}$ around photonic structures, enabling substantial light-matter interaction on integrated photonic platforms and paving the way for scalable, on-chip quantum devices.

quant-ph

Floquet Engineering of Polaritonic Amplification in Dispersive Photonic Time Crystals

In this study, we investigate the dynamics of dispersive photonic time crystals (PTCs) and their potential applications for controlling light-matter interaction. By employing the Lorentz-Drude model, we analyze theoretically and via numerical simulation the effects of periodic modulation of dispersion parameters, revealing the emergence of hybrid bandgaps from interaction of polaritonic branches with unique characteristics. Our study demonstrates that dispersive PTCs offer novel excitation channels and amplification possibilities, that require lower modulation frequencies compared to non-dispersive systems thus alleviating experimental challenges for the realization of PTCs in the optical regime. These findings pave the way for advancements in polaritonic lasing and resonant Raman scattering.

physics.optics

Non-native Quantum Generative Optimization with Adversarial Autoencoders

Large-scale optimization problems are prevalent in several fields, including engineering, finance, and logistics. However, most optimization problems cannot be efficiently encoded onto a physical system because the existing quantum samplers have too few qubits. Another typical limiting factor is that the optimization constraints are not compatible with the native cost Hamiltonian. This work presents a new approach to address these challenges. We introduce the adversarial quantum autoencoder model (AQAM) that can be used to map large-scale optimization problems onto existing quantum samplers while simultaneously optimizing the problem through latent quantum-enhanced Boltzmann sampling. We demonstrate the AQAM on a neutral atom sampler, and showcase the model by optimizing 64px by 64px unit cells that represent a broad-angle filter metasurface applicable to improving the coherence of neutral atom devices. Using 12-atom simulations, we demonstrate that the AQAM achieves a lower Renyi divergence and a larger spectral gap when compared to classical Markov Chain Monte Carlo samplers. Our work paves the way to more efficient mapping of conventional optimization problems into existing quantum samplers.

quant-ph

Plasmonic Enhancement of Second Harmonic Generation in Weyl Semimetal TaAs

In this work a hybrid nanoplasmonic-Weyl Semimetal (WSM) structure is realized for the first time utilizing silver nanopatch antennas and WSM Tantalum Arsenide (TaAs). The studied hybrid WSM-nanoplasmonic structure demonstrated a substantial, over x4.5 enhancement of the second harmonic generation (SHG) process compared to a bare TaAs film. To realize the hybrid structure while preserving TaAs properties, a scalable, non-destructive manufacturing approach was developed that involves the fabrication of TaAs flakes from single crystalline TaAs, overgrowth of a silicon nitride overlayer, and drop-casting of silver nanopatch antennas. The strong polarization response of both the bare flakes, along with the hybrid-nanoplasmonic cavities demonstrates that this approach uniquely preserves the TaAs crystal structure and its optical response while providing significant enhancement of the nonlinear properties. The developed method allows leveraging the capabilities of plasmonics to control and enhance light-matter interactions at the nanometer scale to access and engineer WSM response. This work is the first step towards high-performance nanophotonic devices utilizing WSM topological properties.

physics.optics

Ultraconfined plasmons in atomically thin crystalline silver nanostructures

The ability to confine light down to atomic scales is critical for the development of applications in optoelectronics and optical sensing as well as for the exploration of nanoscale quantum phenomena. Plasmons in metallic nanostructures can achieve this type of confinement, although fabrication imperfections down to the subnanometer scale hinder actual developments. Here, we demonstrate narrow plasmons in atomically thin crystalline silver nanostructures fabricated by prepatterning silicon substrates and epitaxially depositing silver films of just a few atomic layers in thickness. Combined with on-demand lateral shaping, this procedure allows for an unprecedented control over optical field confinement in the near-infrared spectral region. Specifically, we observe fundamental and higher-order plasmons featuring extreme spatial confinement and high-quality factors that reflect the crystallinity of the metal. Our approach holds potential for the design and exploitation of atomic-scale nanoplasmonic devices in optoelectronics, sensing, and quantum-physics applications.

cond-mat.mes-hall

Unveiling the coupling of single metallic nanoparticles to whispering-gallery microcavities

Whispering-gallery mode resonators host multiple trapped narrowband circulating optical resonances that find applications in quantum electrodynamics, optomechanics, and sensing. However, the spherical symmetry and low field leakage of dielectric microspheres make it difficult to probe their high-quality optical modes using far-field radiation. Even so, local field enhancement from metallic nanoparticles (MNPs) coupled to the resonators can interface the optical far-field and the bounded cavity modes. In this work, we study the interaction between whispering-gallery modes and MNP surface plasmons with nanometric spatial resolution by using electron-beam spectroscopies in a scanning transmission electron microscope. We show that gallery modes are induced over a selective spectral range of the nanoparticle plasmons, and additionally, their polarization can be controlled by the induced dipole moment of the MNP. Our study demonstrates a viable mechanism to effectively excite high-quality-factor whispering-gallery modes and holds potential for applications in optical sensing and light manipulation.

physics.optics

Can Copper Nanostructures Sustain High-Quality Plasmons?

Silver is considered to be the king among plasmonic materials because it features low inelastic absorption in the visible and infrared (vis-IR) spectral regions compared to other metals. In contrast, copper is commonly regarded as being too lossy for plasmonic applications. Here, we experimentally demonstrate vis-IR plasmons in long copper nanowires (NWs) with quality factors that exceed a value of 60, as determined by spatially resolved, high-resolution electron energy-loss spectroscopy (EELS) measurements. We explain this counterintuitive result by the fact that plasmons in these metal wires have most of their electromagnetic energy outside the metal, and thus, they are less sensitive to inelastic losses in the material. We present an extensive set of data acquired on long silver and copper NWs of varying diameters supporting this conclusion and further allowing us to understand the relative roles played by radiative and nonradiative losses in plasmons that span a wide range of energies down to $<20\,$meV. At such small plasmon energies, thermal population of these modes becomes significant enough to enable the observation of electron energy gains associated with plasmon absorption events. Our results support the use of copper as an attractive cheap and abundant material platform for high quality plasmons in elongated nanostructures.

cond-mat.mtrl-sci

Ultrafast Momentum-Resolved Probing of Plasmon Thermal Dynamics with Free Electrons

Current advances in ultrafast electron microscopy make it possible to combine optical pumping of a nanostructure and electron beam probing with subångstrom and femtosecond spatiotemporal resolution. We present a theory predicting that this technique can reveal a rich out-of-equilibrium dynamics of plasmon excitations in graphene and graphite samples. In a disruptive departure from the traditional probing of nanoscale excitations based on the identification of spectral features in the transmitted electrons, we show that measurement of angle-resolved, energy-integrated inelastic electron scattering can trace the temporal evolution of plasmons in these structures and provide momentum-resolved mode identification, thus avoiding the need for highly-monochromatic electron beams and the use of electron spectrometers. This previously unexplored approach to study the ultrafast dynamics of optical excitations can be of interest to understand and manipulate polaritons in 2D semiconductors and other materials exhibiting a strong thermo-optical response.

cond-mat.mtrl-sci

Nanoscale Nonlinear Spectroscopy with Electron Beams

We theoretically demonstrate the ability of electron beams to probe the nonlinear photonic response with nanometer spatial resolution, well beyond the capabilities of existing optical techniques. Although the interaction of electron beams with photonic modes is generally weak, the use of optical pumping produces stimulated electron-light interactions that can reach order-unity probabilities in photon-induded near field electron microscopy (PINEM). Here, we demonstrate that PINEM can locally and quantitatively probe the nonlinear optical response. Specifically, we predict a dependence of PINEM electron spectra on the sample nonlinearity that can reveal the second-harmonic (SH) response of optical materials with nanometer resolution, observed through asymmetries between electron energy losses and gains. We illustrate this concept by showing that PINEM spectra are sensitive to the SH near field of centrosymmetric structures and by finding substantial spectral asymmetries in geometries for which the linear interaction is reduced.

cond-mat.mes-hall

Plasmonics in Atomically-Thin Crystalline Silver Films

Light-matter interaction at the atomic scale rules fundamental phenomena such as photoemission and lasing, while enabling basic everyday technologies, including photovoltaics and optical communications. In this context, plasmons --the collective electron oscillations in conducting materials-- are important because they allow manipulating optical fields at the nanoscale. The advent of graphene and other two-dimensional crystals has pushed plasmons down to genuinely atomic dimensions, displaying appealing properties such as a large electrical tunability. However, plasmons in these materials are either too broad or lying at low frequencies, well below the technologically relevant near-infrared regime. Here we demonstrate sharp near-infrared plasmons in lithographically-patterned wafer-scale atomically-thin silver crystalline films. Our measured optical spectra reveal narrow plasmons (quality factor $\sim4$), further supported by a low sheet resistance comparable to bulk metal in few-atomic-layer silver films down to seven Ag(111) monolayers. Good crystal quality and plasmon narrowness are obtained despite the addition of a thin passivating dielectric, which renders our samples resilient to ambient conditions. The observation of spectrally sharp and strongly confined plasmons in atomically thin silver holds great potential for electro-optical modulation and optical sensing applications.

cond-mat.mes-hall

Tailored nanoscale plasmon-enhanced vibrational electron spectroscopy

Vibrational optical spectroscopies can be enhanced by surface plasmons to reach molecular-sized limits of detection and characterization. The level of enhancement strongly depends on microscopic details of the sample that are generally missed by macroscopic techniques. Here we investigate phonons in h-BN by coupling them to silver-nanowire plasmons, whose energy is tuned by modifying the nanowire length. Specifically, we use electron beam milling to accurately and iteratively change the nanowire length, followed by electron energy-loss spectroscopy to reveal the plasmon-enhanced vibrational features of h-BN. This allows us to investigate otherwise hidden bulk phonons and observe strong plasmon-phonon coupling. The new milling-and-spectroscopy technique holds great potential for resolving vibrational features in material nanostructures.

cond-mat.mes-hall

Lasing and Amplification from Two-Dimensional Atom Arrays

We explore the ability of two-dimensional periodic atom arrays to produce light amplification and generate laser emission when gain is introduced through external optical pumping. Specifically, we predict that lasing can take place for arbitrarily weak atomic scatterers assisted by cooperative interaction among atoms in a 2D lattice. We base this conclusion on analytical theory for three-level scatterers, which additionally reveals a rich interplay between lattice and atomic resonances. Our results provide a general background to understand light amplification and lasing in periodic atomic arrays, with promising applications in the generation, manipulation, and control of coherent photon states at the nanoscale.

cond-mat.mes-hall

Ultrafast broadband tuning of resonant optical nanostructures using phase change materials

The functionalities of a wide range of optical and opto-electronic devices are based on resonance effects and active tuning of the amplitude and wavelength response is often essential. Plasmonic nanostructures are an efficient way to create optical resonances, a prominent example is the extraordinary optical transmission (EOT) through arrays of nanoholes patterned in a metallic film. Tuning of resonances by heating, applying electrical or optical signals has proven to be more elusive, due to the lack of materials that can induce modulation over a broad spectral range and/or at high speeds. Here we show that nanopatterned metals combined with phase change materials (PCMs) can overcome this limitation due to the large change in optical constants which can be induced thermally or on an ultrafast timescale. We demonstrate resonance wavelength shifts as large as 385 nm - an order of magnitude higher than previously reported - by combining properly designed Au EOT nanostructures with Ge2Sb2Te5 (GST). Moreover, we show, through pump probe measurements, repeatable and reversible, large amplitude modulations in the resonances, especially at telecommunication wavelengths, over ps time scales and at powers far below those needed to produce a permanent phase transition. Our findings open a pathway to the design of hybrid metal PCM nanostructures with ultrafast and widely tuneable resonance responses, which hold potential impact on active nanophotonic devices such as tuneable optical filters, smart windows, biosensors and reconfigurable memories.

physics.optics