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Stiven Forti

Publications and source records attributed to Stiven Forti.

At least 19 recordsLinked to original sources

Direct observation of flat bands in near-magic-angle twisted bilayer CVD graphene

Advances in chemical vapor deposition (CVD) growth have driven graphene crystal quality to unprecedented levels, yet it is still unknown whether this route can realize the fragile flat-band and correlated states of the magic-angle (MA) twisted bilayer graphene (TBG). Here, we report on the experimental observation by room-temperature nano-angle-resolved photoemission spectroscopy (nano-ARPES) of flat bands in a TBG sample close to the MA, assembled via a grow-and-stack protocol based on low-pressure CVD of graphene on copper. Our study indicates electronic bands fully comparable to those measured in exfoliation-based samples and determines the size of the largest near-MA domain to be compatible with electronic transport experiments, motivating further experiments on flat band physics in CVD-graphene.

cond-mat.mes-hall

Lifshitz transitions and isospin polarization in twist-decoupled monolayer-bilayer graphene

Bernal-stacked bilayer graphene (BLG) hosts correlated electronic phases tied to low-energy Lifshitz transitions at saddle points in its valence band. To access this regime, ultralow charge disorder and control over a vertical electric field are simultaneously required. Here, we employ a twist-decoupled monolayer (MLG) to bias a proximal BLG in the absence of an external displacement field (D). We thereby reveal three-fold degenerate quantum Hall states at D = 0, with multiple transitions driven by doping, magnetic and electric field. Spontaneous broken symmetry in the vicinity of the valence band edge is signaled by the emergence of quantum oscillations with anomalous frequencies and large quasiparticle mass. These results indicate that electronic interactions in BLG are preserved in presence of an atomically close MLG, while showcasing the potential of CVD-grown graphene multilayers for the exploration of correlated phases of matter.

cond-mat.mes-hall

Ultrafast signatures of Dirac / flat-band hybrid states from time-resolved ARPES

Hybridization of highly itinerant Dirac electrons with localized flat-band states is predicted to yield emergent phenomena such as exotic heavy-fermion behaviour. Epitaxial graphene on two-dimensional adsorbate structures on SiC(0001), which host flat bands, offers a promising platform to explore these effects. However, direct experimental evidence of interlayer hybridization in such systems has so far been lacking. Here, we address this gap using time- and angle-resolved photoemission spectroscopy (trARPES) where interlayer hybridization manifests in three key observations: (1) accelerated Dirac-carrier relaxation arising from additional electronic and phononic decay channels provided by the flat-band subsystem, (2) transient charging of the Dirac cone enabled by direct optical excitation from the flat bands, and (3) ultrafast back-transfer of charge into the flat bands on timescales governed by the interlayer coupling strength. We further demonstrate that the degree of hybridization can be tuned via the atomic number of the atoms intercalated at the graphene-SiC interface, establishing a controllable platform for investigating exotic correlated ground states.

cond-mat.mtrl-sci

Influence of twist angle on ultrafast charge separation in WS2-graphene heterostructures

Van der Waals (vdW) heterostructures, formed by stacking two-dimensional materials, offer highly tunable electronic and optical properties, with the twist angle between layers acting as a critical tuning parameter. While its impact on moir\'e patterns, band structure, and correlated states is well-established, the influence of twist angle on ultrafast charge transfer remains controversial. Here, we employ time- and angle-resolved photoemission spectroscopy (trARPES) to directly probe ultrafast charge transfer in epitaxially grown WS\textsubscript{2}-graphene heterostructures with twist angles of 0$^{\circ}$ and 30$^{\circ}$. Upon photoexcitation at $\hbar\omega = 3.1\,\mathrm{eV}$, we observe efficient charge separation at 0$^{\circ}$, while at 30$^{\circ}$, electron and hole transfer occur at similar rates. Our results highlight the crucial role of the twist angle in controlling charge separation efficiency, offering valuable insights for designing vdW heterostructures for applications in photovoltaics and optoelectronics.

cond-mat.mtrl-sci

Nickel intercalation in epitaxial graphene on SiC(0001): a novel platform for engineering two-dimensional heterostructures

Two-dimensional (2D) magnetic materials integrated with graphene offer a compelling platform for next-generation spintronic devices, yet nickel in its 2D form remains largely unexplored, due to fundamental synthesis limitations. Here, we report the controlled intercalation of Ni beneath epitaxial graphene on the Si-face of SiC(0001), achieved through a scalable colloidal nanoparticle deposition route. Chemically synthesized Ni nanoparticles (~10 nm diameter) are uniformly deposited onto graphene via immersion in colloidal solution at room temperature; subsequent thermal annealing at 650 {\deg}C drives intercalation, yielding well-ordered Ni islands at the graphene/buffer-layer interface with morphology dictated by annealing conditions. Scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES), supported by density functional theory (DFT) calculations, elucidate the atomic and electronic structure of the intercalated layers. DFT simulations further confirm the thermodynamic stability of the 2D nanostructures as a function of shape and lateral size, predicting a robust average magnetic moment of 0.9 $\mu_B$ per atom. The resulting Ni-intercalated graphene on SiC constitutes a well-defined 2D heterostructure combining preserved graphene band structure with robust interfacial magnetism, stable under ambient conditions. These findings establish a reproducible, scalable pathway to engineer magnetic graphene-based heterostructures and open new avenues for their integration into spintronic architectures.

cond-mat.mtrl-sci

Influence of sulphur vacancies on ultrafast charge separation in WS$_2$-graphene heterostructures

Understanding how defects influence charge separation in WS$_2$-graphene heterostructures is crucial for future applications in light harvesting and detection. Previous studies have reported widely varying lifetimes for the charge-separated state, all supposedly linked to electron trapping at sulphur vacancies. The exact impact of these defects, however, has remained unclear. Here, we deliberately introduce sulphur vacancies by annealing the heterostructures at high temperatures in ultrahigh vacuum. Angle-resolved photoemission spectroscopy (ARPES) reveals that these vacancies modify both the band alignment and doping level of the heterostructure. Time-resolved ARPES (trARPES) further shows that increasing the sulphur vacancy concentration prolongs the lifetime of electrons in the WS$_2$ conduction band but shortens the lifetime of the charge-separated state. Guided by model calculations, we attribute this behaviour to shifts in the energy alignment between sulphur vacancy states and graphene's Dirac point, combined with a reduced excitonic absorption. The model also yields a transfer time for electrons tunneling from sulphur vacancies into graphene's Dirac cone of $\sim$4ps, consistent with our trARPES measurements. Our study clarifies the role of sulphur vacancies in WS$_2$-graphene heterostructures, further improving our microscopic understanding of charge dynamics for future optoelectronic applications.

cond-mat.mes-hall

Real-Space Plasmon Imaging Reveals Modified Electronic Structure of Gold at the Monolayer Limit

Atomically thin materials exhibit electronic and optical properties distinct from their three-dimensional counterparts. For metals, particularly gold, monolayer studies remain largely unexplored due to fabrication and characterisation challenges. Here we report the first optical study of a stable quasi-freestanding gold monolayer formed by Au intercalation between graphene and SiC. Mid-infrared nanoimaging reveals plasmon-polaritons with wavelengths nearly an order of magnitude shorter than free-space light. Analysis of their dispersion using a Drude model yields a relaxation time of $\tau = 18\,$fs, comparable to bulk gold, and a Drude weight of $D = 1.3\,$mS$\cdot$eV, nearly twice the bulk expectation. These results establish monolayer gold as a two-dimensional metal, opening opportunities for nanoscale photonics, plasmonics and ultra-thin electronics.

physics.optics

SpectraFormer: an Attention-Based Raman Unmixing Tool for Accessing the Graphene Buffer-Layer Signature on SiC

Raman spectroscopy is a key tool for graphene characterization, yet its application to graphene grown on silicon carbide (SiC) is strongly limited by the intense and variable second-order Raman response of the substrate. This limitation is critical for buffer layer graphene, a semiconducting interfacial phase, whose vibrational signatures are overlapped with the SiC background and challenging to be reliably accessed using conventional reference-based subtraction, due to strong spatial and experimental variability of the substrate signal. Here we present SpectraFormer, a transformer-based deep learning model that reconstructs the SiC Raman substrate contribution directly from post-growth partially masked spectroscopic data without relying on explicit reference measurements. By learning global correlations across the entire Raman shift range, the model captures the statistical structure of the SiC background and enables accurate reconstruction of its contribution in mixed spectra. Subtraction of the reconstructed substrate signal reveals weak vibrational features associated with ZLG that are inaccessible through conventional analysis methods. The extracted spectra are validated by ab initio vibrational calculations, allowing assignment of the resolved features to specific modes and confirming their physical consistency. By leveraging a state-of-the-art attention-based deep learning architecture, this approach establishes a robust, reference-free framework for Raman analysis of graphene on SiC and provides a foundation, compatible with real-time data acquisition, to its integration into automated, closed-loop AI-assisted growth optimization.

cond-mat.mtrl-sci

Phason-driven temperature-dependent transport in moir\'e graphene

The electronic and vibrational properties of 2D materials are dramatically altered by the formation of a moir\'e superlattice. The lowest-energy phonon modes of the superlattice are two acoustic branches (called phasons) that describe the sliding motion of one layer with respect to the other. Considering their low-energy dispersion and damping, these modes may act as a significant source of scattering for electrons in moir\'e materials. Here, we investigate temperature-dependent electrical transport in minimally twisted bilayer graphene, a moir\'e system developing multiple weakly-dispersive electronic bands and a reconstructed lattice structure. We measure a linear-in-temperature resistivity across the band manyfold above $T\sim{10}$ K, preceded by a quadratic temperature dependence. While the linear-in-temperature resistivity is up to two orders of magnitude larger than in monolayer graphene, it is reduced (approximately by a factor of three) with respect to magic-angle twisted bilayer graphene. Moreover, it is modulated by the recursive band filling, with minima located close to the full filling of each band. Comparing our results with a semiclassical transport calculation, we show that the experimental trends are compatible with scattering processes mediated by longitudinal phasons, which dominate the resistivity over the contribution from conventional acoustic phonons of the monolayer. Our findings highlight the close relation between vibrational modes unique to moir\'e materials and carrier transport therein.

cond-mat.mes-hall

Novel structures of Gallenene intercalated in epitaxial Graphene

The creation of atomically thin layers of non-exfoliable materials remains a crucial challenge, requiring the development of innovative techniques. Here, confinement epitaxy is exploited to realize two-dimensional gallium via intercalation in epitaxial graphene grown on silicon carbide. Novel superstructures arising from the interaction of gallenene (a monolayer of gallium) with graphene and the silicon carbide substrate are investigated. The coexistence of different gallenene phases, including b010-gallenene and the elusive high-pressure Ga(III) phase, is identified. This work sheds new light on the formation of two-dimensional gallium and provides a platform for investigating the exotic electronic and optical properties of confined gallenene.

cond-mat.mtrl-sci

Influence of doping on non-equilibrium carrier dynamics in graphene

Controlling doping is key to optimizing graphene for high-speed electronic and optoelectronic devices. However, its impact on non-equilibrium carrier lifetimes remains debated. Here, we systematically tune the doping level of quasi-freestanding epitaxial graphene on SiC(0001) via potassium deposition and probe its ultrafast carrier dynamics directly in the band structure using time- and angle-resolved photoemission spectroscopy (trARPES). We find that increased doping lowers both the peak electronic temperature and the cooling rate of Dirac carriers, which we attribute to higher electronic heat capacity and reduced phonon emission phase space. Comparing quasi-freestanding graphene with graphene on a carbon buffer layer reveals faster relaxation in the latter, likely due to additional phonon modes being available for heat dissipation. These findings offer new insights for optimizing graphene in electronic and photonic technologies.

cond-mat.mes-hall

Influence of excitation energy on microscopic quantum pathways for ultrafast charge transfer in van der Waals heterostructures

Efficient charge separation in van der Waals (vdW) heterostructures is crucial for optimizing light harvesting and detection applications. However, precise control over the microscopic pathways governing ultrafast charge transfer remains an open challenge. These pathways are intrinsically linked to charge transfer states with strongly delocalized wave functions that appear at various momenta in the Brillouin zone. Here, we use time- and angle-resolved photoemission spectroscopy (trARPES) to investigate the possibility of steering carriers through specific charge transfer states in a prototypical WS\textsubscript{2}-graphene heterostructure. By selectively exciting electron-hole pairs at the K-point (A-exciton resonance) and close to the Q-point (C-exciton resonance) of WS\textsubscript{2} with different pump photon energies, we find that charge separation is faster at higher excitation energies. This behavior is attributed to the fact that absorption at the C-exciton resonance generates electron-hole populations at energies well above the direct band gap. The resulting elevated carrier temperatures open an additional, highly efficient charge-transfer channel for holes in the WS\textsubscript{2} valence band, leading to an overall acceleration of interlayer hole transfer for C-exciton excitation. The microscopic insights gained in this work can be leveraged to optimize the performance of vdW heterostructures in optoelectronic devices.

cond-mat.mes-hall

Intercalated structures formed by platinum on epitaxial graphene on SiC(0001)

Graphene on SiC intercalated with two-dimensional metal layers, such as Pt, offers a versatile platform for applications in spintronics, catalysis, and beyond. Recent studies have demonstrated that Pt atoms can intercalate at the heterointerface between SiC(0001) and the C-rich $(6\sqrt{3}\times6\sqrt{3})$R30{\deg} reconstructed surface (hereafter referred as the buffer layer). However, key aspects such as intercalated phase structure and intercalation mechanisms remain unclear. In this work, we investigate changes in morphology, chemistry, and electronic structure for both buffer layer and monolayer graphene grown on SiC(0001) following Pt deposition and annealing cycles, which eventually led to Pt intercalation at temperatures above 500{\deg}C. Atomic-resolution imaging of the buffer layer reveals a single intercalated Pt layer that removes the periodic corrugation of the buffer layer, arising from partial bonding of C-atoms with Si-atoms of the substrate. In monolayer graphene, the Pt-intercalated regions exhibit a two-level structure: the first level corresponds to a Pt layer intercalated below the buffer layer, while the second level contains a second Pt layer, giving rise to a $(12\times12)$ superstructure relative to graphene. Upon intercalation, Pt atoms appear as silicides, indicating a reaction with Si atoms from the substrate. Additionally, charge neutral $\pi$-bands corresponding to quasi-free-standing monolayer and bilayer graphene emerge. Analysis of multiple samples, coupled with a temperature-dependent study of the intercalation rate, demonstrates the pivotal role of buffer layer regions in facilitating the Pt intercalation in monolayer graphene. These findings provide valuable insight into Pt intercalation, advancing the potential for applications.

cond-mat.mtrl-sci

Adaptive AI-Driven Material Synthesis: Towards Autonomous 2D Materials Growth

Two-dimensional (2D) materials are poised to revolutionize current solid-state technology with their extraordinary properties. Yet, the primary challenge remains their scalable production. While there have been significant advancements, much of the scientific progress has depended on the exfoliation of materials, a method that poses severe challenges for large-scale applications. With the advent of artificial intelligence (AI) in materials science, innovative synthesis methodologies are now on the horizon. This study explores the forefront of autonomous materials synthesis using an artificial neural network (ANN) trained by evolutionary methods, focusing on the efficient production of graphene. Our approach demonstrates that a neural network can iteratively and autonomously learn a time-dependent protocol for the efficient growth of graphene, without requiring pretraining on what constitutes an effective recipe. Evaluation criteria are based on the proximity of the Raman signature to that of monolayer graphene: higher scores are granted to outcomes whose spectrum more closely resembles that of an ideal continuous monolayer structure. This feedback mechanism allows for iterative refinement of the ANN's time-dependent synthesis protocols, progressively improving sample quality. Through the advancement and application of AI methodologies, this work makes a substantial contribution to the field of materials engineering, fostering a new era of innovation and efficiency in the synthesis process.

cond-mat.mes-hall

Rapid synthesis of uniformly small nickel nanoparticles for the surface functionalization of epitaxial graphene

Nickel nanoparticles (Ni NPs), thanks to their peculiar properties, are interesting materials for many applications including catalysis, hydrogen storage, and sensors. In this work, Ni NPs are synthesized in aqueous solution by a simple and rapid procedure with cetyltrimethylammonium bromide (CTAB) as a capping agent, and are extensively characterized by dynamic light scattering (DLS), scanning electron microscopy (SEM), and atomic force microscopy (AFM). We investigated their shape, dimension, and their distribution on the surfaces of SiO2 and epitaxial graphene (EG) samples. Ni NPs have an average diameter of ~11 nm, with a narrow size dispersion, and their arrangement on the surface is strongly dependent on the substrate. EG samples functionalized with Ni NPs are further characterized by X-ray photoelectron spectroscopy (XPS), as made and after thermal annealing above 350{\deg}C to confirm the degradation of CTAB and the presence of metallic Ni(0). Moreover, high resolution scanning tunneling microscopy (STM) topographies reveal the structural stability of the NPs up to 550 {\deg}C.

cond-mat.mtrl-sci

Built-in Bernal gap in large-angle-twisted monolayer-bilayer graphene

Atomically thin materials offer multiple opportunities for layer-by-layer control of their electronic properties. While monolayer graphene (MLG) is a zero-gap system, Bernal-stacked bilayer graphene (BLG) acquires a finite band gap when the symmetry between the layers' potential energy is broken, usually, via a displacement electric field applied in double-gate devices. Here, we introduce a twistronic stack comprising both MLG and BLG, synthesized via chemical vapor deposition, showing a Bernal gap in the absence of external fields. Although a large ($\sim30^{\circ}$) twist angle decouples the MLG and BLG electronic bands near Fermi level, proximity-induced energy shifts in the outermost layers result in a built-in asymmetry, which requires a displacement field of $0.14$ V/nm to be compensated. The latter corresponds to a $\sim10$ meV intrinsic BLG gap, a value confirmed by our thermal-activation measurements. The present results highlight the role of structural asymmetry and encapsulating environment, expanding the engineering toolbox for monolithically-grown graphene multilayers.

cond-mat.mes-hall

k-resolved ultrafast light-induced band renormalization in monolayer WS$_2$ on graphene

Understanding and controlling the electronic properties of two-dimensional materials is crucial for their potential applications in nano- and optoelectronics. Monolayer transition metal dichalcogenides such as WS$_2$ have garnered significant interest due to their strong light-matter interaction and extreme sensitivity of the band structure to the presence of photogenerated electron-hole pairs. In this study, we investigate the transient electronic structure of monolayer WS$_2$ on a graphene substrate after resonant excitation of the A-exciton using time- and angle-resolved photoemission spectroscopy. We observe a pronounced band structure renormalization including a substantial reduction of the transient band gap that is in good quantitative agreement with our {\it ab initio} theory that reveals the importance of both intrinsic WS$_2$ and extrinsic substrate contributions to the transient band structure of monolayer WS$_2$. Our findings not only deepen the fundamental understanding of band structure dynamics in two-dimensional materials but also offer valuable insights for the development of novel electronic and optoelectronic devices based on monolayer TMDs and their heterostructures with graphene.

cond-mat.mtrl-sci

Growth and applications of two-dimensional single crystals

Two-dimensional (2D) materials have received extensive research attentions over the past two decades due to their intriguing physical properties (such as the ultrahigh mobility and strong light-matter interaction at atomic thickness) and a broad range of potential applications (especially in the fields of electronics and optoelectronics). The growth of single-crystal 2D materials is the prerequisite to realize 2D-based high-performance applications. In this review, we aim to provide an in-depth analysis of the state-of-the-art technology for the growth and applications of 2D materials, with particular emphasis on single crystals. We first summarize the major growth strategies for monolayer 2D single crystals. Following that, we discuss the growth of multilayer single crystals, including the control of thickness, stacking sequence, and heterostructure composition. Then we highlight the exploration of 2D single crystals in electronic and optoelectronic devices. Finally, a perspective is given to outline the research opportunities and the remaining challenges in this field.

cond-mat.mtrl-sci