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Francesco Gucci

Publications and source records attributed to Francesco Gucci.

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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

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

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

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

Ultrafast valleytronic logic operations

Information processing currently reaches speeds as high as 800 GHz. However, the underlying transistor technology is quickly approaching its fundamental limits and further progress requires a disruptive approach. One such path is to manipulate quantum properties of solids, such as the valley degree of freedom, with ultrashort controlled lightwaves. Here we employ a sequence of few-optical-cycle visible pulses controlled with attosecond precision to excite and switch the valley pseudospin in a 2D semiconductor. We show that a pair of pulses separated in time with linear orthogonal polarizations can induce a valley-selective population. Additionally, exploiting a four-pump excitation protocol, we perform logic operations such as valley de-excitation and re-excitation at room temperature at rates as high as ~10 THz.

cond-mat.mes-hall