arXiv subjects

Andrea C. Ferrari

Publications and source records attributed to Andrea C. Ferrari.

At least 19 recordsLinked to original sources

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↗

arXiv2025

A foundation model for atomistic materials chemistry

Atomistic simulations of matter, especially those that leverage first-principles (ab initio) electronic structure theory, provide a microscopic view of the world, underpinning much of our understanding of chemistry and materials science. Over the last decade or so, machine-learned force fields have transformed atomistic modeling by enabling simulations of ab initio quality over unprecedented time and length scales. However, early ML force fields have largely been limited by: (i) the substantial computational and human effort of developing and validating potentials for each particular system of interest; and (ii) a general lack of transferability from one chemical system to the next. Here we show that it is possible to create a general-purpose atomistic ML model, trained on a public dataset of moderate size, that is capable of running stable molecular dynamics for a wide range of molecules and materials. We demonstrate the power of the MACE-MP-0 model - and its qualitative and at times quantitative accuracy - on a diverse set of problems in the physical sciences, including properties of solids, liquids, gases, chemical reactions, interfaces and even the dynamics of a small protein. The model can be applied out of the box as a starting or "foundation" model for any atomistic system of interest and, when desired, can be fine-tuned on just a handful of application-specific data points to reach ab initio accuracy. Establishing that a stable force-field model can cover almost all materials changes atomistic modeling in a fundamental way: experienced users get reliable results much faster, and beginners face a lower barrier to entry. Foundation models thus represent a step towards democratising the revolution in atomic-scale modeling that has been brought about by ML force fields.

physics.chem-ph↗

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↗

arXiv2025

The 2D Materials Roadmap

Over the past two decades, 2D materials have rapidly evolved into a diverse and expanding family of material platforms. Many members of this materials class have demonstrated their potential to deliver transformative impact on fundamental research and technological applications across different fields. In this roadmap, we provide an overview of the key aspects of 2D material research and development, spanning synthesis, properties and commercial applications. We specifically present roadmaps for high impact 2D materials, including graphene and its derivatives, transition metal dichalcogenides, MXenes as well as their heterostructures and moiré systems. The discussions are organized into thematic sections covering emerging research areas (e.g., twisted electronics, moiré nano-optoelectronics, polaritronics, quantum photonics, and neuromorphic computing), breakthrough applications in key technologies (e.g., 2D transistors, energy storage, electrocatalysis, filtration and separation, thermal management, flexible electronics, sensing, electromagnetic interference shielding, and composites) and other important topics (computational discovery of novel materials, commercialization and standardization). This roadmap focuses on the current research landscape, future challenges and scientific and technological advances required to address, with the intent to provide useful references for promoting the development of 2D materials.

cond-mat.mtrl-sci↗

arXiv2025

Raman Forbidden Layer-Breathing Modes in Layered Semiconductor Materials Activated by Phonon and Optical Cavity Effects

We report Raman forbidden layer-breathing modes (LBMs) in layered semiconductor materials (LSMs). The intensity distribution of all observed LBMs depends on layer number, incident light wavelength and refractive index mismatch between LSM and underlying substrate. These results are understood by a Raman scattering theory via the proposed spatial interference model, where the naturally occurring optical and phonon cavities in LSMs enable spatially coherent photon-phonon coupling mediated by the corresponding one-dimensional periodic electronic states. Our work reveals the spatial coherence of photon and phonon fields on the phonon excitation via photon/phonon cavity engineering.

cond-mat.mtrl-sci↗

arXiv2025

Adhesion and Reconstruction of Graphene/Hexagonal Boron Nitride Heterostructures: A Quantum Monte Carlo Study

We investigate interlayer adhesion and relaxation at interfaces between graphene and hexagonal boron nitride (hBN) monolayers in van der Waals heterostructures. The adhesion potential between graphene and hBN is calculated as a function of local lattice offset using diffusion quantum Monte Carlo methods, which provide an accurate treatment of van der Waals interactions. Combining the adhesion potential with elasticity theory, we determine the relaxed structures of graphene and hBN layers at interfaces, finding no metastable structures. The adhesion potential is well described by simple Lennard-Jones pair potentials that we parameterize using our quantum Monte Carlo data. Encapsulation of graphene between near-aligned crystals of hBN gives rise to a moiré pattern whose period is determined by the misalignment angle between the hBN crystals superimposed over the moiré superlattice previously studied in graphene on an hBN substrate. We model minibands in such supermoiré superlattices and find them to be sensitive to a 180$^\circ$ rotation of one of the encapsulating hBN crystals. We find that monolayer and bilayer graphene placed on a bulk hBN substrate and bulk hBN/graphene/bulk hBN systems do not relax to adopt a common lattice constant. The energetic balance is much closer for free-standing monolayer graphene/hBN bilayers and hBN/graphene/hBN trilayers. The layers in an alternating stack of graphene and hBN are predicted to strain to adopt a common lattice constant and hence we obtain a new, stable three-dimensional crystal with a unique electronic structure.

cond-mat.mes-hall↗

arXiv2024

Laser Activation of Single Group-IV Colour Centres in Diamond

Spin-photon interfaces based on group-IV colour centres in diamond offer a promising platform for quantum networks. A key challenge in the field is realizing precise single-defect positioning and activation, which is crucial for scalable device fabrication. Here we address this problem by demonstrating a two-step fabrication method for tin vacancy (SnV-) centres that uses site-controlled ion implantation followed by local femtosecond laser annealing with in-situ spectral monitoring. The ion implantation is performed with sub-50 nm resolution and a dosage that is controlled from hundreds of ions down to single ions per site, limited by Poissonian statistics. Using this approach, we successfully demonstrate site-selective creation and modification of single SnV- centres. The technique opens a window onto materials tuning at the single defect level, and provides new insight into defect structures and dynamics during the annealing process. While demonstrated for SnV- centres, this versatile approach can be readily generalised to other implanted colour centres in diamond and wide-bandgap materials.

quant-ph↗

arXiv2024

Electromechanical response of saddle points in twisted hBN moiré superlattices

In twisted layered materials (t-LMs), an inter-layer rotation can break inversion symmetry and create an interfacial array of staggered out-of-plane polarization due to AB/BA stacking registries. This symmetry breaking can also trigger the formation of edge in-plane polarizations localized along the perimeter of AB/BA regions (i.e., saddle point domains). However, a comprehensive experimental investigation of these features is still lacking. Here, we use piezo force microscopy to probe the electromechanical behavior of twisted hexagonal boron nitride (t-hBN). For a parallel stacking alignment of t-hBN, we reveal very narrow (width ~ 20 nm) saddle point polarizations, which we also measure in the anti-parallel configuration. These localized polarizations can still be found on a multiply-stacked t-hBN structure, determining the formation of a double moiré. We also visualize a t-hBN moiré superlattice in the topography maps with atomic force microscopy, related to the strain accumulated at the saddle point domains. Our findings imply that polarizations in t-hBN do not only point in the out-of-plane direction, but also show an in-plane component, giving rise to a much more complex 3D polarization field.

cond-mat.mtrl-sci↗

arXiv2024

Nature of long-lived moiré interlayer excitons in electrically tunable MoS$_{2}$/MoSe$_{2}$ heterobilayers

Interlayer excitons in transition-metal dichalcogenide heterobilayers combine high binding energy and valley-contrasting physics with long optical lifetime and strong dipolar character. Their permanent electric dipole enables electric-field control of emission energy, lifetime, and location. Device material and geometry impacts the nature of the interlayer excitons via their real- and momentum-space configurations. Here, we show that interlayer excitons in MoS$_{2}$/MoSe$_{2}$ heterobilayers are formed by charge carriers residing at the Brillouin zone edges, with negligible interlayer hybridization. We find that the moiré superlattice leads to the reversal of the valley-dependent optical selection rules, yielding a positively valued g-factor and cross-polarized photoluminescence. Time-resolved photoluminescence measurements reveal that the interlayer exciton population retains the optically induced valley polarization throughout its microsecond-long lifetime. The combination of long optical lifetime and valley polarization retention makes MoS$_{2}$/MoSe$_{2}$ heterobilayers a promising platform for studying fundamental bosonic interactions and developing excitonic circuits for optical information processing.

cond-mat.mes-hall↗

arXiv2023

Microwave-based quantum control and coherence protection of tin-vacancy spin qubits in a strain-tuned diamond membrane heterostructure

Robust spin-photon interfaces in solids are essential components in quantum networking and sensing technologies. Ideally, these interfaces combine a long-lived spin memory, coherent optical transitions, fast and high-fidelity spin manipulation, and straightforward device integration and scaling. The tin-vacancy center (SnV) in diamond is a promising spin-photon interface with desirable optical and spin properties at 1.7 K. However, the SnV spin lacks efficient microwave control and its spin coherence degrades with higher temperature. In this work, we introduce a new platform that overcomes these challenges - SnV centers in uniformly strained thin diamond membranes. The controlled generation of crystal strain introduces orbital mixing that allows microwave control of the spin state with 99.36(9) % gate fidelity and spin coherence protection beyond a millisecond. Moreover, the presence of crystal strain suppresses temperature dependent dephasing processes, leading to a considerable improvement of the coherence time up to 223(10) $μ$s at 4 K, a widely accessible temperature in common cryogenic systems. Critically, the coherence of optical transitions is unaffected by the elevated temperature, exhibiting nearly lifetime-limited optical linewidths. Combined with the compatibility of diamond membranes with device integration, the demonstrated platform is an ideal spin-photon interface for future quantum technologies.

cond-mat.mes-hall↗

arXiv2023

Control of Raman scattering quantum interference pathways in graphene

Graphene is an ideal platform to study the coherence of quantum interference pathways by tuning doping or laser excitation energy. The latter produces a Raman excitation profile that provides direct insight into the lifetimes of intermediate electronic excitations and, therefore, on quantum interference, which has so far remained elusive. Here, we control the Raman scattering pathways by tuning the laser excitation energy in graphene doped up to 1.05eV, above what achievable with electrostatic doping. The Raman excitation profile of the G mode indicates its position and full width at half maximum are linearly dependent on doping. Doping-enhanced electron-electron interactions dominate the lifetime of Raman scattering pathways, and reduce Raman interference. This paves the way for engineering quantum pathways in doped graphene, nanotubes and topological insulators.

cond-mat.mes-hall↗

arXiv2022

Identification of exciton complexes in a charge-tuneable Janus WSeS monolayer

Janus transition-metal dichalcogenide monolayers are fully artificial materials, where one plane of chalcogen atoms is replaced by chalcogen atoms of a different type. Theory predicts an in-built out-of-plane electric field, giving rise to long-lived, dipolar excitons, while preserving direct-bandgap optical transitions in a uniform potential landscape. Previous Janus studies had broad photoluminescence (>15 meV) spectra obfuscating their excitonic origin. Here, we identify the neutral, and negatively charged inter- and intravalley exciton transitions in Janus WSeS monolayer with $\sim 6$ meV optical linewidth. We combine a recently developed synthesis technique, with the integration of Janus monolayers into vertical heterostructures, allowing doping control. Further, magneto-optic measurements indicate that monolayer WSeS has a direct bandgap at the K points. This work provides the foundation for applications such as nanoscale sensing, which relies on resolving excitonic energy shifts, and photo-voltaic energy harvesting, which requires efficient creation of long-lived excitons and integration into vertical heterostructures.

cond-mat.mes-hall↗

arXiv2022

Ultrashort pulse generation from a graphene-coupled passively mode-locked terahertz laser

The generation of stable trains of ultra-short (fs-ps), terahertz (THz)-frequency radiation pulses, with large instantaneous intensities, is an underpinning requirement for the investigation of light-matter interactions, for metrology and for ultra-high-speed communications. In solid-state electrically-pumped lasers, the primary route for generating short pulses is through passive mode-locking. However, this has not yet been achieved in the THz range, defining one of the longest standing goals over the last two decades. In fact, the realization of passive mode-locking has long been assumed to be inherently hindered by the fast recovery times associated with the intersubband gain of THz lasers. Here, we demonstrate a self-starting miniaturized ultra-short pulse THz laser, exploiting an original device architecture that includes the surface patterning of multilayer-graphene saturable absorbers distributed along the entire cavity of a double-metal semiconductor 2.30-3.55 THz wire laser. Self-starting pulsed emission with 4.0-ps-long pulses in a compact, all-electronic, all-passive and inexpensive configuration is demonstrated.

physics.optics↗

arXiv2022

Electrically tuneable nonequilibrium optical response of graphene

The ability to tune the optical response of a material via electrostatic gating is crucial for optoelectronic applications, such as electro-optic modulators, saturable absorbers, optical limiters, photodetectors and transparent electrodes. The band structure of single layer graphene (SLG), with zero-gap, linearly dispersive conduction and valence bands, enables an easy control of the Fermi energy E$_F$ and of the threshold for interband optical absorption. Here, we report the tunability of the SLG non-equilibrium optical response in the near-infrared (1000-1700nm/0.729-1.240eV), exploring a range of E$_F$ from -650 to 250 meV by ionic liquid gating. As E$_F$ increases from the Dirac point to the threshold for Pauli blocking of interband absorption, we observe a slow-down of the photobleaching relaxation dynamics, which we attribute to the quenching of optical phonon emission from photoexcited charge carriers. For E$_F$ exceeding the Pauli blocking threshold, photobleaching eventually turns into photoinduced absorption, due to hot electrons' excitation increasing SLG absorption. The ability to control both recovery time and sign of nonequilibrium optical response by electrostatic gating makes SLG ideal for tunable saturable absorbers with controlled dynamics.

cond-mat.mtrl-sci↗

arXiv2021

Quantum control of the tin-vacancy spin qubit in diamond

Group-IV color centers in diamond are a promising light-matter interface for quantum networking devices. The negatively charged tin-vacancy center (SnV) is particularly interesting, as its large spin-orbit coupling offers strong protection against phonon dephasing and robust cyclicity of its optical transitions towards spin-photon entanglement schemes. Here, we demonstrate multi-axis coherent control of the SnV spin qubit via an all-optical stimulated Raman drive between the ground and excited states. We use coherent population trapping and optically driven electronic spin resonance to confirm coherent access to the qubit at 1.7 K, and obtain spin Rabi oscillations at a rate of $Ω/2π$=3.6(1) MHz. All-optical Ramsey interferometry reveals a spin dephasing time of $T_2^*$=1.3(3)$μ$s and two-pulse dynamical decoupling already extends the spin coherence time to $T_2$=0.33(14) ms. Combined with transform-limited photons and integration into photonic nanostructures, our results make the SnV a competitive spin-photon building block for quantum networks.

quant-ph↗

arXiv2021

Wafer-scale integration of graphene-based photonic devices

Graphene and related materials can lead to disruptive advances in next generation photonics and optoelectronics. The challenge is to devise growth, transfer and fabrication protocols providing high (>5,000 cm2 V-1 s-1) mobility devices with reliable performance at the wafer scale. Here, we present a flow for the integration of graphene in photonics circuits. This relies on chemical vapour deposition (CVD) of single layer graphene (SLG) matrices comprising up to ~12000 individual single crystals (SCs), grown to match the geometrical configuration of the devices in the photonic circuit. This is followed by a transfer approach which guarantees coverage over ~80% of the device area, and integrity for up to 150 mm wafers, with room temperature mobility ~5000 cm2 V-1 s-1. We use this process flow to demonstrate double SLG electro-absorption modulators with modulation efficiency ~0.25, 0.45, 0.75, 1 dB V-1 for device lengths ~30, 60, 90, 120 μm. The data rate is up to 20 Gbps. Encapsulation with single-layer hBN is used to protected SLG during plasma-enhanced CVD of Si3N4, ensuring reproducible device performance. Our full process flow (from growth to device fabrication) enables the commercial implementation of graphene-based photonic devices.

physics.app-ph↗

arXiv2020

Exciton-phonon coupling strength in single-layer MoSe2 at room temperature

Single-layer transition metal dichalcogenides are at the center of an ever increasing research effort both in terms of fundamental physics and applications. Exciton-phonon coupling plays a key role in determining the (opto)electronic properties of these materials. However, the exciton-phonon coupling strength has not been measured at room temperature. Here, we develop two-dimensional micro-spectroscopy to determine exciton-phonon coupling of single-layer MoSe2. We detect beating signals as a function of waiting time T, induced by the coupling between the A exciton and the A'1 optical phonon. Analysis of two-dimensional beating maps combined with simulations provides the exciton-phonon coupling. The Huang-Rhys factor of ~1 is larger than in most other inorganic semiconductor nanostructures. Our technique offers a unique tool to measure exciton-phonon coupling also in other heterogeneous semiconducting systems with a spatial resolution ~260 nm, and will provide design-relevant parameters for the development of optoelectronic devices.

cond-mat.mes-hall↗

arXiv2020

Tunable broadband light emission from graphene

Graphene is an ideal material for integrated nonlinear optics thanks to its strong light-matter interaction and large nonlinear optical susceptibility. Graphene has been used in optical modulators, saturable absorbers, nonlinear frequency converters, and broadband light emitters. For the latter application, a key requirement is the ability to control and engineer the emission wavelength and bandwidth, as well as the electronic temperature of graphene. Here, we demonstrate that the emission wavelength of graphene$'$ s broadband hot carrier photoluminescence can be tuned by integration on photonic cavities, while thermal management can be achieved by out-of-plane heat transfer to hexagonal boron nitride. Our results pave the way to graphene-based ultrafast broadband light emitters with tunable emission.

physics.optics↗