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Alessandro Alabastri

Publications and source records attributed to Alessandro Alabastri.

At least 19 recordsLinked to original sources

On-demand thermal power amplification enabled by active heat $Q$-switching

Thermal management underpins essentially every energy technology, from solar harvesters and waste-heat recovery to industrial process heating and electronic cooling. Yet, thermal systems remain limited compared to their electrical and optical counterparts: they lack a direct equivalent of active control elements that enable on-demand pulse generation. As a result, in conventional thermal energy storage architectures, the amount of energy stored and the peak power at which it can be released are both fixed at design time by material properties and heat-exchanger geometry, locking each device to a single operating point in the energy--power plane. This rigidity is incompatible with applications that require short, high-power thermal bursts on demand. Here we show that a counter-flow heat oscillator admits an actively switchable effective thermal quality factor, $Q$, and that modulating $Q$ on sub-dwell-time scales generates transient outlet power exceeding the steady input by more than an order of magnitude. We formalize the system as a dissipative resonant thermal cavity with $Q$ controlled by the balance between advective and conductive transport and environmental losses, and we experimentally demonstrate, in a water-based dual-channel device, $\sim$5-fold transient power amplification through controlled flow detuning, in quantitative agreement with our thermofluidic model. Active $Q$-switching establishes a distinct mode of thermal power management, accessing $\sim$5$\times$ (demonstrated experimentally) to $\sim$40$\times$ (projected numerically) peak-power amplification on continuous input through a single architecture, a regime inaccessible to passive thermal storage and a missing analogue of the active pulse-generation tools long available in optics and electronics.

physics.app-ph

Graduate Training in Quantum Information Science and Engineering: Lessons, Challenges, and a Roadmap from the NSF Research Traineeship Programs

Since 2019, eighteen NSF Research Traineeship (NRT) awards in quantum information science and engineering (QISE) and adjacent fields have been funded, constituting the largest NSF-coordinated investment in graduate QISE training in the United States. Synthesizing lessons from our programs, we work through the central tensions that every QISE graduate program must negotiate: between depth in a home discipline and breadth across the field, between structured instruction and open-ended experiential and hands-on learning, and between training individual specialists and cultivating teams that collectively cover all areas of QISE. We describe the structural and pedagogical innovations the NRT programs have developed in response, assess what is working and what remains unresolved, and sketch 12 open problems the community will need to address as QISE graduate education scales beyond the well-resourced research universities where it has up till now been mainly concentrated. Eight concrete recommendations follow: (1) adopt the startup model of team-based training as an organizing philosophy; (2) invest immediately in sensing and communication curriculum development; (3) build student agency into program governance, not just activities; (4) establish structural mechanisms for industrial engagement rather than depending on goodwill; (5) design for sustainability from year one; (6) develop graduate-level textbooks spanning all three QISE pillars: computing, sensing, and communications; (7) establish shared outcome assessment instruments across programs; and (8) develop structured mechanisms for faculty professional development in QISE.

physics.ed-ph

Layered Bimetal Nanoporous Platforms for SERS Sensing

Nanoporous metals are extensively investigated as platforms for applications in plasmonics. They present high surface areas and strong local electric fields that can be tuned at different energies, playing with the choice of the metals and the morphology of the porous layers. Until recently, research in the field of plasmonics has primarily focused on porous metals composed of a single element, with limited attention given to the impact of alloy composition. The investigation of bi-metallic systems has only just begun to emerge in the literature. In particular, combining two or more different plasmonic metals, it could be possible to explore the interactions between two metals excited at specific energies. This involves plasmonic coupling, electron transfer, band hybridization at the interface, electromagnetic field interactions, and possibly thermal and electronic energy transfer depending on separation, size, and materials involved. The analysis of bi-metal systems can also be interesting in biomolecule detection, such as in the case of Surface Enhanced Raman Scattering (SERS). Here we report, for the first time, a detailed study (comprising morphological analyses, numerical modelling, and optical spectroscopies) on bi-metal nanoporous platforms prepared with a dry-synthesis method enabling the easy and controllable fabrication of bilayers combining different metals such as Au, Ag, and Cu.

physics.app-ph

Static magnetic control of light emission in plasmonic nanojunctions

Localized surface plasmon resonances (LSPRs) in metal nanoparticles have been studied extensively through scattering and absorption. Static magnetic field-induced changes in plasmonic far-field response stem from the classical Hall effect and are generally very small in noble metals within the visible frequency range at readily accessible magnetic fields. Planar plasmonic tunnel junctions allow the study of nanogap LSPRs through current-driven light emission. We find that the electroluminescence of such junctions is modulated by tens of percent with a magnetic field of a few Teslas, exceeding Hall-based expectations by orders of magnitude. Complementary quantum mechanical and electromagnetic modeling reveals that a modest static magnetic field can introduce significant chirality in the transition dipoles generated during the electron tunneling process. This strongly affects the excitation of LSPRs and leads to magnetic-field sensitive far-field electroluminescent emission. This is a new paradigm for tunable nanoscale light sources.

physics.optics

Realization of a Chiral Photonic-Crystal Cavity with Broken Time-Reversal Symmetry

Light-matter interactions in chiral cavities offer a compelling route to manipulate material properties by breaking fundamental symmetries such as time-reversal symmetry. However, only a limited number of chiral cavity implementations exhibiting broken time-reversal symmetry have been demonstrated to date. These typically rely on either the application of strong magnetic fields, circularly polarized Floquet driving, or the hybridization of cavity modes with matter excitations in the ultrastrong coupling regime. Here, we present a one-dimensional terahertz photonic-crystal cavity that exhibits broken time-reversal symmetry. The cavity consists of a high-resistivity silicon wafer sandwiched between lightly n-doped InSb wafers. By exploiting the nonreciprocal response of a terahertz magnetoplasma and the exceptionally low effective mass of electrons in InSb, we demonstrate a circularly polarized cavity mode at 0.67 THz under a modest magnetic field of 0.3 T, with a quality factor exceeding 50. Temperature-, magnetic field-, and polarization-dependent measurements, supported by simulations, confirm the realization of a chiral cavity with broken time-reversal symmetry. This platform offers a robust and accessible approach for exploring chiral light--matter interactions and vacuum dressed quantum condensed matter in the terahertz regime.

physics.optics

Terahertz chiral photonic-crystal cavities for Dirac gap engineering in graphene

Strong coupling between matter and vacuum electromagnetic fields in a cavity can induce novel quantum phases in thermal equilibrium via symmetry breaking. Particularly intriguing is the coupling with circularly polarized cavity fields, which can break time-reversal symmetry (TRS) and lead to topological bands. This has spurred significant interest in developing chiral cavities that feature broken TRS, especially in the terahertz (THz) frequency range, where various large-oscillator-strength resonances exist. Here, we present a design for high-quality-factor THz chiral photonic-crystal cavities (PCCs) that achieves broken TRS using a magnetoplasma in a lightly doped semiconductor. We incorporate ab initio density functional theory calculations into the derived microscopic model, allowing a realistic estimate of the vacuum-induced gap in graphene when coupled to our chiral cavity. Our calculations show an enhancement in the light-matter interaction due to Dirac nodes and predict an energy gap on the order of 1 meV. The THz chiral PCCs offer a promising platform for exploring cavity-dressed condensed matter with broken TRS.

physics.optics

Electron-Phonon Temperature Inversion in Nanostructures under Pulsed Photoexcitation

Photoexcitation of metallic nanostructures with short optical pulses can drive non-thermal electronic states, which, upon decay, lead to elevated electronic temperatures ($T_e \gtrapprox 1000\,\mathrm{K}$) eventually equilibrating with the lattice ($T_p$) through electron-phonon scattering. Here, we show that, in spatially extended nanostructures, the lattice temperature can locally exceed that of the electrons, a seemingly counterintuitive transient effect termed hereafter ``temperature inversion'' ($T_p > T_e$). This phenomenon, fundamentally due to inhomogeneous absorption patterns and absent in smaller particles, emerges from a complex spatio-temporal interplay, between the electron-phonon coupling and competing electronic thermal diffusion. By combining rigorous three-dimensional (3D) finite-element-method-based simulations with practical reduced zero-dimensional (0D) analytical models, we identify the electron-phonon coupling coefficient ($G_{e-p}$) as the critical parameter governing this behavior. An optimal $G_{e-p}$ range allows the inversion, whereas a weak or overly strong coupling suppresses it. Among common plasmonic metals, platinum (Pt) exhibits the most pronounced and long-lived inversion, while gold (Au) and silver (Ag) show no significant inversion. Moreover, the close agreement between the 0D and 3D results, once an appropriate characteristic length is selected, highlights that the essential physics governing the inversion can be captured without full spatial complexity. These results provide insights for optimizing nanoscale energy transfer and hot-carrier-driven processes, guiding the strategic design of materials, geometries, and excitation conditions for enhanced ultrafast photothermal control.

cond-mat.mes-hall

Multimode Ultrastrong Coupling in Three-Dimensional Photonic-Crystal Cavities

Recent theoretical studies have highlighted the role of spatially varying cavity electromagnetic fields in exploring novel cavity quantum electrodynamics (cQED) phenomena, such as the potential realization of the elusive Dicke superradiant phase transition. One-dimensional photonic-crystal cavities (PCCs), widely used for studying solid-state cQED systems, have uniform spatial profiles in the lateral plane. Three-dimensional (3D) PCCs, which exhibit discrete in-plane translational symmetry, overcome this limitation, but fabrication challenges have hindered the achievement of strong coupling in 3D-PCCs. Here, we report the realization of multimode ultrastrong coupling in a 3D-PCC at terahertz frequencies. The multimode coupling between the 3D-PCC's cavity modes and the cyclotron resonance of a Landau-quantized two-dimensional electron gas in GaAs is significantly influenced by the spatial profiles of the cavity modes, leading to distinct coupling scenarios depending on the probe polarization. Our experimental results are in excellent agreement with a multimode extended Hopfield model that accounts for the spatial inhomogeneity of the cavity field. Guided by the model, we discuss the possible strong ground-state correlations between different cavity modes and introduce relevant figures of merit for the multimode ultrastrong coupling regime. Our findings emphasize the importance of spatially nonuniform cavity mode profiles in probing nonintuitive quantum phenomena expected for the ground states of cQED systems in the ultrastrong coupling regime.

quant-ph

Dry synthesis of bi-layer nanoporous metal films as plasmonic metamaterial

Nanoporous metals are a class of nanostructured materials finding extensive applications in multiple fields thanks to their unique properties attributed to their high surface area and interconnected nanoscale ligaments. They can be pre-pared following different strategies, but the deposition of an arbitrary pure porous metal is still challenging. Recently, a dry synthesis of nanoporous films based on the plasma treat-ment of metal thin layers deposited by physical vapour deposition has been demonstrated, as a general route to form pure nanoporous films from a large set of metals. An interest-ing aspect related to this approach is the possibility to apply the same methodology to deposit the porous films as a multilayer. In this way, it is possible to explore the properties of different porous metals in close contact. As demonstrated in this paper, interesting plasmonic properties emerge in a nanoporous Au-Ag bi-layer. The versatility of the method coupled with the possibility to include many different metals, provides an opportunity to tailor their optical resonances and to exploit the chemical and mechanical properties of compo-nents, which is of great interest to applications ranging from sensing, to photochemistry and photocatalysis.

physics.app-ph

Nanoporous Metals: From Plasmonic Properties to Applications in Enhanced Spectroscopy and Photocatalysis

The field of plasmonics is capable of enabling interesting applications in the different wavelength ranges, spanning from the ultraviolet up to the infrared. The choice of plasmonic material and how the material is nanostructured have significant implications for ultimate performance of any plasmonic device. Artificially designed nanoporous metals have interesting material properties including large specific surface area, distinctive optical properties, high electrical conductivity, and reduced stiffness, implying their potentials for many applications. This manuscript reviews the wide range of available nanoporous metals, mainly focusing on their properties as plasmonic materials. While extensive reports on the use and characterization of NPMs exist, a detailed discussion on their connection with surface plasmons and enhanced spectroscopies as well as photocatalysis is missing. Here, we report on different metals investigated, from the most used nanoporous gold to mixed metal compounds, and discuss each of these plasmonic materials suitability for a range of structural design and applications. Finally, we discuss the potentials and limitations of the traditional and alternative plasmonic materials for applications in enhanced spectroscopy and photocatalysis.

physics.app-ph

Quantifying efficiency of remote excitation for surface enhanced Raman spectroscopy in molecular junctions

Surface-enhanced Raman spectroscopy (SERS) is enabled by local surface plasmon resonances (LSPRs) in metallic nanogaps. When SERS is excited by direct illumination of the nanogap, the background heating of lattice and electrons can prevent further manipulation of the molecules. To overcome this issue, we report SERS in electromigrated gold molecular junctions excited remotely: surface plasmon polaritons (SPPs) are excited at nearby gratings, propagate to the junction, and couple to the local nanogap plasmon modes. Like direct excitation, remote excitation of the nanogap can generate both SERS emission and an open-circuit photovoltage (OCPV). We compare SERS intensity and OCPV in both direct and remote illumination configurations. SERS spectra obtained by remote excitation are much more stable than those obtained through direct excitation when photon count rates are comparable. By statistical analysis of 33 devices, coupling efficiency of remote excitation is calculated to be around 10%, consistent with the simulated energy flow.

cond-mat.mes-hall

Detection of strong light-matter interaction in a single nano-cavity with a thermal transducer

Recently, the concept of strong light-matter coupling has been demonstrated in semiconductor structures, and it is poised to revolutionize the design and implementation of components, including solid state lasers and detectors. We demonstrate an original nanospectroscopy technique that permits to study the light-matter interaction in single subwavelength-sized nano-cavities where far-field spectroscopy is not possible using conventional techniques. We inserted a thin ($\approx$ 150 nm) polymer layer with negligible absorption in the mid-IR (5 $μ$m < $λ$ < 12 $μ$m) inside a metal-insulator-metal resonant cavity, where a photonic mode and the intersubband transition of a semiconductor quantum well are strongly coupled. The intersubband transition peaks at $λ$ = 8.3 $μ$m, and the nano-cavity is overall 270 nm thick. Acting as a non-perturbative transducer, the polymer layer introduces only a limited alteration of the optical response while allowing to reveal the optical power absorbed inside the concealed cavity. Spectroscopy of the cavity losses is enabled by the polymer thermal expansion due to heat dissipation in the active part of the cavity, and performed using an atomic force microscope (AFM). This innovative approach allows the typical anticrossing characteristic of the polaritonic dispersion to be identified in the cavity loss spectra at the single nano-resonator level. Results also suggest that near-field coupling of the external drive field to the top metal patch mediated by a metal-coated AFM probe tip is possible, and it enables the near-field mapping of the cavity mode symmetry including in the presence of strong light-matter interaction.

physics.optics

All-optical Reconfiguration of Ultrafast Dichroism in Gold Metasurfaces

Optical metasurfaces have come into the spotlight as a promising platform for light manipulation at the nanoscale, including ultrafast all-optical control via excitation with femtosecond laser pulses. Recently, dichroic metasurfaces have been exploited to modulate the polarization state of light with unprecedented speed. Here, we theoretically predict and experimentally demonstrate by pump-probe spectroscopy the capability to reconfigure the ultrafast dichroic signal of a gold metasurface by simply acting on the polarization of the pump pulse, which is shown to reshape the spatio-temporal distribution of the optical perturbation. The photoinduced anisotropic response, driven by out-of-equilibrium carriers and extinguished in a sub-picosecond temporal window, is readily controlled in intensity by tuning the polarization direction of the excitation up to a full sign reversal. This work proves that nonlinear metasurfaces offer the flexibility to tailor their ultrafast optical response in a fully all-optically reconfigurable platform.

physics.optics

Challenges in Plasmonic Catalysis

The use of nanoplasmonics to control light and heat close to the thermodynamic limit enables exciting opportunities in the field of plasmonic catalysis. The decay of plasmonic excitations creates highly nonequilibrium distributions of hot carriers that can initiate or catalyze reactions through both thermal and nonthermal pathways. In this Perspective, we present the current understanding in the field of plasmonic catalysis, capturing vibrant debates in the literature, and discuss future avenues of exploration to overcome critical bottlenecks. Our Perspective spans first-principles theory and computation of correlated and far-from-equilibrium light-matter interactions, synthesis of new nanoplasmonic hybrids, and new steady-state and ultrafast spectroscopic probes of interactions in plasmonic catalysis, recognizing the key contributions of each discipline in realizing the promise of plasmonic catalysis. We conclude with our vision for fundamental and technological advances in the field of plasmon-driven chemical reactions in the coming years.

physics.optics

Three-dimensional Printing of Complex Graphite Structures

Graphite, with many industrial applications, is one of the widely sought-after allotropes of carbon. The sp2 hybridized and thermodynamically stable form of carbon forms a layered structure with strong in-plane carbon bonds and weak inter-layer van der Waals bonding. Graphite is also a high-temperature ceramic, and shaping them into complex geometries is challenging, given its limited sintering behavior even at high temperatures. Although the geometric design of the graphite structure in many of the applications could dictate its precision performance, conventional synthesis methods for formulating complex geometric graphite shapes are limited due to the intrinsic brittleness and difficulties of high-temperature processing. Here, we report the development of colloidal graphite ink from commercial graphite powders with reproducible rheological behavior that allows the fabrication of any complex architectures with tunable geometry and directionality via 3D printing at room temperature. The method is enabled via using small amounts of clay, another layered material, as an additive, allowing the proper design of the graphene ink and subsequent binding of graphite platelets during printing. Sheared layers of clay are easily able to flow, adapt, and interface with graphite layers forming strong binding between the layers and between particles that make the larger structures. The direct ink printing of complex 3D architectures of graphite without further heat treatments could lead to easy shape engineering and related applications of graphite at various length scales, including complex graphite molds or crucibles. The 3D printed complex graphitic structures exhibit excellent thermal, electrical, and mechanical properties, and the clay additive does not seem to alter these properties due to the excellent inter-layer dispersion and mixing within the graphite material.

cond-mat.mtrl-sci

Transient optical symmetry breaking for ultrafast broadband dichroism in plasmonic metasurfaces

Ultrafast nanophotonics is an emerging research field aimed at the development of nanodevices capable of light modulation with unprecedented speed. A promising approach exploits the optical nonlinearity of nanostructured materials (either metallic or dielectric) to modulate their effective permittivity via interaction with intense ultrashort laser pulses. While the ultrafast temporal dynamics of such nanostructures following photoexcitation has been studied in depth, sub-ps transient spatial inhomogeneities taking place at the nanoscale have been so far almost ignored. Here we theoretically predict and experimentally demonstrate that the inhomogeneous space-time distribution of photogenerated hot carriers induces a transient symmetry breaking in a plasmonic metasurface made of highly symmetric metaatoms. The process is fully reversible, and results in a broadband transient dichroic optical response with a recovery of the initial isotropic state in less than 1 picosecond, overcoming the speed bottleneck caused by slower relaxation processes, such as electron-phonon and phonon-phonon scattering. Our results pave the way to the development of ultrafast dichroic devices, capable of Tera bit/s modulation of light polarization.

physics.optics

Photoinduced Temperature Gradients in Sub-wavelength Plasmonic Structures: The Thermoplasmonics of Nanocones

Plasmonic structures are renowned for their capability to efficiently convert light into heat at the nanoscale. However, despite the possibility to generate deep sub-wavelength electromagnetic hot spots, the formation of extremely localized thermal hot spots is an open challenge of research, simply because of the diffusive spread of heat along the whole metallic nanostructure. Here we tackle this challenge by exploiting single gold nanocones. We theoretically show how these structures can indeed realize extremely high temperature gradients within the metal, leading to deep sub-wavelength thermal hot spots, owing to their capability of concentrating light at the apex under resonant conditions even under continuous wave illumination. A three-dimensional Finite Element Method model is employed to study the electromagnetic field in the structure and subsequent thermoplasmonic behaviour, in terms of the three-dimensional temperature distribution. We show how the latter is affected by nanocone size, shape, and composition of the surrounding environment. Finally, we anticipate the use of photoinduced temperature gradients in nanocones for applications in optofluidics and thermoelectrics or for thermally induced nanofabrication.

physics.optics

lambda DNA through a plasmonic nanopore What can be detected by means of Surface Enhanced Raman Scattering?

Engineered electromagnetic fields in plasmonic nanopores enable enhanced optical detection and their use in single molecule sequencing. Here, a plasmonic nanopore prepared in a thick nanoporous film is used to investigate the interaction between the metal and a long-chain double strand DNA molecule. We discuss how the matrix of nanoporous metal can interact with the molecule thanks to: i) transient aspecific interactions between the porous surface and DNA and ii) optical forces exerted by the localized field in a metallic nanostructure. A duration of interaction up to tens of milliseconds enables to collect high signal-to-noise Raman vibrations allowing an easy label-free reading of information from the DNA molecule. Moreover, in order to further increase the event of detection rate, we tested a polymeric porous hydrogel placed beneath the solid-state membrane. This approach enables a slowdown of the molecule diffusion, thus increasing the number of detected interactions by a factor of about 20.

physics.app-ph