arXiv subjects

Giulio Cerullo

Publications and source records attributed to Giulio Cerullo.

At least 19 recordsLinked to original sources

arXiv2026

X-ray driven displacive excitation of coherent phonons

Modulating electron-phonon coupling offers a route to control structural displacements and tune material functionality. Valence-to-conduction band transitions, however, provide limited leverage over the driving force. Here, we demonstrate coherent lattice dynamics in trigonal tellurium using free-electron laser pulses tuned to the Te N4,5-edge. Over a broad fluence range, the oscillation amplitude obeys the displacive excitation of coherent phonons framework, extended to core resonance with twice the driving efficiency of a visible pump. Ab initio calculations decompose the force into competing multiband contributions, inaccessible to optical excitation, whose balance shifts as carriers relax. Tunable extreme-ultraviolet and X-ray pulses thus open a regime in which the displacive response is set by band-dependent coupling to the lattice, not by the number and temperature of the photocarriers alone.

cond-mat.mtrl-sci↗

arXiv2026

All-optical switching of nonlinear structured light in crystal-engineered van der Waals materials

The orbital angular momentum (OAM) of light is a discrete, unbounded degree of freedom that underpins mode-multiplexed communications and high-dimensional quantum photonics. Yet, dynamic OAM control remains dependent on bulky free-space optics or cascaded architectures that separate switching from wavefront shaping, hindering nanoscale integration. Here, we engineer artificial van der Waals crystals from rhombohedrally stacked (3R) MoS$_2$, in which spatial control of the local crystal orientation imprints a nonlinear geometric phase onto the second-harmonic (SH) field, enabling background-free generation of SH vortex beams in an ultrathin (46 nm) van der Waals platform. Leveraging the C$_{3v}$ symmetry of 3R-MoS$_2$, we demonstrate monolithic, all-optical switching with sub-optical-cycle precision between Hermite-Gauss-like and Laguerre-Gaussian vortex SH beams with opposite topological charges ($l=\pm1$). Our results establish artificial 3R-MoS$_2$ crystals as a monolithic platform for the generation and all-optical reconfiguration of nonlinear structured light at the nanoscale, advancing active nanophotonic sources for integrated classical and quantum photonic technologies.

physics.optics↗

arXiv2026

Spatiotemporal Metasurface for Ultrafast All-Optical Wavefront Shaping

Optical metasurfaces have established themselves as exceptional nanophotonic platforms to control the properties of light at subwavelength scales. By properly designing the geometry and spatial arrangement of their constituent meta-atoms, engineered phase gradients can be imparted to an incoming field, thereby tailoring its wavefront with a virtually unlimited number of control knobs. However, once fabricated, a metasurface has a permanently fixed optical response. Here, we introduce a strategy for dynamic control, by theoretically predicting and experimentally demonstrating all-optical, reversible, and ultrafast wavefront shaping in a periodic semiconductor nanowire metasurface. A strongly astigmatic femtosecond optical pump pulse is used to photoexcite the resonant metasurface non-uniformly, inducing a transient, spatially inhomogeneous permittivity modulation that reshapes the wavefront of a delayed probe pulse. Ultrafast imaging measurements reveal transient defocusing of the transmitted field at selected probe wavelengths, with a switching time below one picosecond. Quantitative numerical modelling elucidates the defocusing mechanism as arising from the interplay between the unperturbed optical response of the resonant metasurface and the pump-induced spatial permittivity gradient. Our work establishes a fully all-optical and ultrafast route to the dynamic analogue of passive wavefront shaping in gradient metasurfaces, paving the way to all-optically reconfigurable metalenses.

physics.optics↗

arXiv2026

Nonequilibrium dynamics of high energy transitions in monolayer WSe$_{2}$

High-energy optical transitions in monolayer transition-metal dichalcogenides exhibit characteristics that are markedly distinct from those of lower-lying band-edge excitons. These differences arise from the involvement of electronic states located at regions of the Brillouin zone that are displaced from the $K$ valleys. In this work, we investigate the ultrafast dynamics of these high-energy excitations by employing broadband ultrafast transient absorption spectroscopy spanning the visible to ultraviolet spectral range. We observe that the formation and relaxation dynamics of one of the high energy transitions display a distinct behavior compared to the lower-energy excitonic resonances, developing on a significantly slower timescale. First-principles calculations of the excitonic landscape allow us to account for this delayed response and attribute it to the phonon-mediated formation of momentum-dark excitons.

cond-mat.mtrl-sci↗

arXiv2026

Iterative approach for high-quality binary intensity hologram generation in augmented reality applications

Binary amplitude spatial light modulators, such as digital micromirror devices (DMDs), are increasingly relevant for computer generated holography due to their high refresh rates, low cost, and due to the emergence of subwavelength pixel architectures. However, the binary constraint limits the reconstruction quality, as conventional approaches rely on a binarization applied as a final step after hologram computation which leads to reduced efficiency and contrast. We introduce an iterative estimation approach for the generation of off axis binary amplitude holograms, in which the binarization constraint is applied at each iteration. We validate the approach through numerical simulations and experimental reconstruction using a DMD based optical setup. Quantitative and qualitative comparisons with random superposition and Gerchberg Saxton methods demonstrate significant improvements in image contrast, light efficiency, and reconstruction fidelity, with comparable computational cost. The proposed method provides a practical route toward high quality CGH using binary modulators and supports emerging applications requiring high speed and high resolution holographic projection.

physics.optics↗

arXiv2026

Excitonic Mott transition without population inversion

Exciton dissociation via the excitonic Mott transition (EMT) governs the high-density optical response of semiconductors and sets fundamental limits for optoelectronic devices. The EMT is conventionally linked to the onset of population inversion and the emergence of optical gain. Here, we demonstrate that this paradigm can break down under ultrafast non-equilibrium excitation. Using femtosecond pump-probe optical spectroscopy, we drive a monolayer transition metal dichalcogenide into a dense photoexcited state in which the excitonic resonance is completely quenched within ~100 fs, while the optical gain is entirely absent across the explored fluence range. State-of-the-art real-time ab initio simulations reveal that the EMT is governed by an interplay of strongly nonthermal carrier populations and nonequilibrium dynamical screening of the Coulomb interaction. The quantitative agreement between theory and experiment identifies a distinct, ultrafast pathway to exciton ionization beyond quasi-equilibrium descriptions and demonstrates that population inversion is not a universal prerequisite for the EMT.

cond-mat.mes-hall↗

arXiv2026

Coherent multi-dimensional widefield microscopy

Understanding how electronic excitations evolve across space and time is essential for revealing the microscopic processes underlying quantum and optoelectronic materials. However, existing approaches cannot simultaneously resolve ultrafast coherent dynamics with microscopic spatial information: pump-probe microscopy lacks access to quantum coherence, while two-dimensional electronic spectroscopy (2DES) requires slow point-by-point scanning for spatial resolution. Here we introduce a widefield two-dimensional electronic spectroscopy microscope (2DESM) combining multidimensional coherent spectroscopy with widefield imaging, enabling simultaneous femtosecond temporal and micrometer spatial resolution across a broadband spectral range. Applying 2DESM to hBN-encapsulated WSe2, we directly visualize spatial variations in exciton coherence and relaxation associated with the local environment, establishing 2DESM as a powerful platform for probing many-body interactions, energy transport, and structure-function relationships in low-dimensional materials and devices.

physics.optics↗

arXiv2026

Valleytronics in 2D Materials Roadmap

Valleytronics exploits non-equivalent energy extrema in the electronic band structure of crystalline solids -- the valley degree of freedom -- to encode, manipulate, and read out information. The advent of 2D materials, first graphene and then transition-metal dichalcogenides, made valley control practical through optical, electrical, and magnetic routes. This foundation has enabled remarkable progress in recent years spanning established frontiers, such as valley exciton physics and valley Hall effects, as well as emerging directions including lightwave valleytronics, nanophotonic integration, flat-band valleytronics, and spin-valley qubits. In parallel, there are sustained efforts to scale up valleytronic materials and to predict new valleytronic platforms. This Roadmap brings together perspectives from leading experts to chart the key opportunities and challenges at the forefront of 2D material valleytronics. Each section captures a snapshot of progress in a key research area, identifies critical open challenges, and outlines pathways toward future valleytronics breakthroughs.

cond-mat.mes-hall↗

arXiv2026

Zero-Order Diffraction Suppression in Full Field-of-View Computer Generated Holography: A Camera In the Loop Interferometric Approach

We introduce a novel interferometric approach for suppressing zero-order diffraction (ZOD) in phase-only computer-generated holography. The technique relies on the destructive interference between the zeroth-order light and a suppression beam in a plane optically conjugated to the spatial light modulator (SLM). A camera-in-the-loop (CITL) calibration procedure retrieves the optimal pixel-wise phase map that cancels out the ZOD component with high precision, while preserving the full modulation depth of the SLM. Experimental demonstrations on point-cloud and 2D/3D holograms achieve up to 99% suppression of the ZOD intensity, without loss of image quality or field of view. Once calibrated, the correction can be applied to any hologram without recomputation, enabling real-time operation and robust performance over time. This method removes a long-standing barrier to the practical deployment of full-field holography, facilitating the development of compact, high-fidelity holographic engines for augmented and mixed reality displays.

physics.optics↗

arXiv2025

Tracking the Catastrophic Collapse of Hybrid Exciton-Phonon Order in a Quantum Material

Revealing the interactions binding electronic and lattice components of cooperative quantum order is central to sculpting new states of matter. This challenge is epitomized by the charge density wave material 1T-TiSe$_2$, where photoexcitation disrupts its presumed hybrid exciton-phonon order. This exposes a paradox: the electronic component collapses within femtoseconds while the periodic lattice distortion persists. If the lattice distortion outlives the excitonic condensate, were they truly intertwined? Here we resolve this by uncovering a low-frequency mode (approx. 0.13 THz) emerging only in the ordered state, signaling exciton-phonon coupling. This mode is consistent with a locked phason -- a collective excitation arising if coupling between the excitonic condensate and lattice reduces continuous phase symmetry to a discrete one, giving the excitonic Goldstone mode finite mass. This is captured by an effective theory describing a shared potential landscape. At a critical threshold, the collapse of excitonic order flattens the potential, triggering an exciton-phonon catastrophe: selective overheating of the charge density wave phonon, disappearance of the locked phason, and sudden loss of electronic coherence. Remarkably, the lattice distortion survives as a dynamically trapped, non-thermal remnant, confirmed by the anomalous temperature dependence of the phononic response. These findings demonstrate that coupled potential energy landscapes can be manipulated to selectively dismantle complex quantum orders, advancing material control through dynamical design.

physics.app-ph↗

arXiv2025

Integration of 2D Materials in Radial van der Waals Heterostructure Metasurfaces

Two-dimensional semiconductors, such as monolayer transition metal dichalcogenides (TMDC), exhibit strong excitonic transitions at room temperature and offer a unique platform for exploring light-matter interactions in nanoscale photonic systems. In this work, we demonstrate a compact and polarization-invariant photonic metasurface, fabricated from hexagonal boron-nitride (hBN) and based on radial bound states in the continuum (BIC), which are formed by radially distributed pairs of structurally asymmetric resonators. The metasurface employs multiple symmetry-breaking perturbations to support high quality-(Q-)factor resonances within a footprint smaller than 8 x 8 $\mu m^2$ - one-sixth of the area of previous approaches. Compared to established hBN metasurface designs, the radial geometry furthermore achieves significantly higher Q-factors with a reduced footprint. By integrating the hBN photonic structure with a WS$_2$ monolayer, we observe enhanced photoluminescence when its resonance is spectrally aligned with the exciton resonance, accompanied by signatures of discrete momentum-space patterns that identify the orbital-angular-momentum-carrying ring eigenmodes. These features persist over a wide range of excitation powers and show minimal linewidth broadening, indicating robust and spatially modulated exciton-photon coupling. This work establishes a scalable approach for generating hybrid photonic-excitonic states with momentum-space structure, offering new opportunities for exciton localization, valley emission, spatially programmable light-matter interaction in two-dimensional material platforms and compact luminescent devices based on 2D material-integrated metasurfaces.

physics.optics↗

arXiv2025

Broadband ultrafast self-heterodyned chiro-optical spectroscopy

Ultrafast chiro-optical spectroscopy provides unique access to the structural dynamics of molecules, spin-valley relaxation in semiconductors, and the non-equilibrium optical response of chiral nanophotonic systems. Yet, because chiral signals are intrinsically weak and time-resolved spectroscopy probes small photoinduced changes, transient chiro-optical responses are often difficult to isolate from parasitic achiral contributions. Here, we introduce a broadband ultrafast chiro-optical spectroscopy technique that integrates a birefringent common-path interferometer with an optical polarization bridge to sensitively detect photoinduced changes in the polarization state of light. Phase-sensitive self-heterodyned detection enables simultaneous measurement of transient circular dichroism and optical rotatory dispersion across a broad spectral range with ultrafast temporal resolution. Balanced detection suppresses excess laser noise, enabling exceptional sensitivity (<50 ${\mu}$deg) close to shot-noise limit. We demonstrate this approach on an array of gold nano-helicoids, supported by a full-wave time-resolved model of the spatiotemporal dynamics of plasmonic non-equilibrium carriers and their associated optical nonlinearities. The model traces the system's transient chiro-optical response back to photoinduced modulations of the electric-magnetic dipole interaction in the nano-helicoid, elucidating the connection of near- and far-field dynamics in the non-equilibrium regime. We further investigate spin excitation, thermalization, and relaxation in a lead halide perovskite, establishing a novel approach to broadband time-resolved Faraday rotation. The simplicity, sensitivity, and wide applicability of this detection scheme provide a powerful platform for broadband ultrafast chiro-optical spectroscopy, opening new opportunities in biochemistry, solid-state physics, and nanophotonics.

physics.optics↗

arXiv2025

Photoinduced Electronic Band Dynamics and Defect-mediated Surface Potential Evolution in PdSe$_2$

We use time- and angle-resolved photoemission spectroscopy (TR-ARPES) combined with density functional theory to investigate ultrafast carrier dynamics in low-symmetry layered semiconducting PdSe$_2$. The indirect bandgap is determined to be 0.55~eV. Following photoexcitation above this gap, we resolve a valence band shift and broadening, both lasting less than a picosecond, consistent with bandgap renormalization and carrier scattering, indicative of strong many-body interactions. Subsequently, hot carriers populate the conduction band minimum and are captured by defect states. A surface photovoltage (SPV) of $\sim$ 67~meV emerges, persisting for over 50~ps, driven by defect-assisted charge separation. The formation of native vacancies, promoted by the low-symmetry lattice, likely gives rise to the mid-gap states responsible for this long-lived SPV response. Detailed analysis of TR-ARPES spectra disentangles the contributions of bandgap renormalization, carrier scattering, defect states, and SPV. These findings establish PdSe$_2$ as a prototypical layered quantum material exhibiting exotic photoresponses on ultrafast timescales.

cond-mat.mes-hall↗

arXiv2025

Spin injection and emission helicity switching in a 2D perovskite/WSe2 heterostructure

The initialization and control of a long-lived spin population in lead halide perovskites are prerequisites for their use in spintronic applications. Here, we demonstrate circular polarization of the interlayer exciton emission in a (BA)2PbI4/WSe2 monolayer heterostructure. The helicity of this emission is controlled by tuning the energy of the excitation laser through the manifold of exciton resonances of the WSe2 monolayer, together with an emerging interlayer absorption feature of the heterostructure. Theoretical calculations show that this resonance arises from hybridized (BA)2PbI4/WSe2 states in the valence band. This hybrid character enables its observation in both linear absorption and ultrafast pump-probe spectroscopies, and plays a key role in controlling the sign of the helicity of the interlayer exciton emission. The tunable spin polarization demonstrated here, with the WSe2 monolayer effectively acting as a tunable spin filter, represents an important step toward the use of 2D perovskites in opto-spintronic applications.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast dynamics of coherent exciton-polaritons in van der Waals semiconductor metasurfaces

Enabling coherent light-matter interactions is a critical step toward next-generation quantum technologies. However, achieving this under ambient temperature conditions remains challenging due to rapid dephasing in optically excited systems. Optical metasurfaces based on quasi-bound states in the continuum have recently emerged as a powerful platform for reaching the strong light-matter coupling regime in flat, subwavelength thickness devices. Here, we investigate ultrafast exciton-polariton dynamics in self-hybridized WS$_2$ thin-film metasurfaces. Using hyperspectral momentum-resolved imaging, we reconstruct the highly anisotropic exciton-polariton dispersion, with a transition from positive to negative effective mass along orthogonal symmetry axes. Femtosecond pump-probe and multidimensional spectroscopy reveal detuning-dependent polariton dynamics with a coherence time up to ~110 fs, and allow direct observation of the coherent dynamics through ultrafast Rabi oscillations with ~45 fs period. We describe this behaviour with a three-eigenstate model that couples the photonic resonance with both bright and dark excitons, extending the conventional two-state picture of strong coupling. Our results establish van der Waals metasurfaces as a promising platform for next-generation polaritonic devices, enabling coherent quantum transfer of matter excitations at room temperature.

physics.optics↗

arXiv2025

Electrically tunable ultrafast dynamics and interactions of hybrid excitons in a 2D semiconductor bilayer

Extended efforts have been devoted to the study of strongly-interacting excitons and their dynamics, towards macroscopic quantum states of matter such as Bose-Einstein condensates of excitons and polaritons. Momentum-direct layer-hybridized excitons in transition metal dichalcogenides have attracted considerable attention due to their high oscillator strength and dipolar nature. However, the tunability of their interactions and dynamics remains unexplored. Here, we achieve an unprecedented control over the nonlinear properties of dipolar layer-hybridized excitons in an electrically gated van der Waals homobilayer monitored by transient optical spectroscopy. By applying a vertical electric field, we reveal strong Coulomb interactions of dipolar hybrid excitons, leading to opposite density-dependent energy shifts of the two main hybrid species based on their dipolar orientation, together with a strongly enhanced optical saturation of their absorption. Furthermore, by electrically tuning the interlayer tunneling between the hybridized carriers, we significantly extend the formation time of hybrid excitons, while simultaneously increasing their decay times. Our findings have implications for the search on quantum blockade and condensation of excitons and dipolaritons in two-dimensional materials.

cond-mat.mes-hall↗

arXiv2025

Topological Control of Polaritonic Flatbands in Anisotropic van der Waals Metasurfaces

Anisotropic van der Waals (vdW) materials exhibit direction-dependent optical and electronic properties, making them valuable for tailoring directional light-matter interactions. Rhenium disulfide (ReS$_2$) stands out for its strong in-plane anisotropy and its thickness-independent direct-bandgap excitons, which can hybridize with light to form exciton-polaritons. In parallel, metasurfaces, engineered arrays of nanoscale subwavelength resonators, can support ultra-sharp photonic modes in the form of quasi-bound states in the continuum (qBICs). Topological transformations of photonic modes can give rise to flatbands, i.e., dispersionless states with quenched kinetic energy and vanishing group velocity. Intrinsic material anisotropy offers an unexplored route to robust far-field flatband formation and control. Here, we demonstrate how structuring an intrinsically anisotropic excitonic material into a resonant metasurface fundamentally transforms its photonic topological features and light-matter coupling behavior, allowing us to drive and topologically control extended far-field flatband formation. To this end, we fabricate C$_4$-symmetric metasurfaces directly from bulk ReS$_2$. The intrinsic anisotropy lifts the initial double degeneracy of the qBIC mode and yields two distinctly polarized resonances. It also reshapes the topological landscape: the integer topological charge of the qBIC mode splits into momentum-separated half-integer singularities, thereby flattening the far-field photonic dispersion. The resulting topologically-controlled photonic flatbands are then tuned in resonance with the linearly polarized excitonic transitions of ReS$_2$, resulting in two distinct, directionally hybridized exciton-polariton flatband regimes. These findings establish anisotropic vdW metasurfaces as a new platform for topologically engineered flatbands and flatband-driven light-matter coupling.

physics.optics↗

arXiv2025

Ultrafast transition from coherent to incoherent polariton nonlinearities in a hybrid 1L-WS2/plasmon structure

Exciton polaritons based on atomically thin semiconductors are essential building blocks of quantum optoelectronic devices. Their properties are governed by an ultrafast and oscillatory energy transfer between their excitonic and photonic constituents, resulting in the formation of polaritonic quasiparticles with pronounced nonlinearities induced by the excitonic component. In metallic nanoresonators, dissipation phenomena limit the polariton lifetime to a few ten femtoseconds, so short that the role of these polaritons for the nonlinearities of such hybrids is yet unexplored. Here, we use ultrafast two-dimensional electronic spectroscopy (2DES) to uncover coherent polariton dynamics in a hybrid monolayer (1L) WS2/plasmonic nanostructure. With respect to an uncoupled WS2 flake, we observe an over 20-fold, polarization-dependent enhancement of the optical nonlinearity and a rapid evolution of the 2DES spectra within ~70 fs. We relate these dynamics to a transition from coherent polaritons to incoherent excitations, unravel the microscopic optical nonlinearities, and show the potential of coherent polaritons for ultrafast all-optical switching.

cond-mat.mes-hall↗