arXiv subjects

D. De Fazio

Publications and source records attributed to D. De Fazio.

14 recordsLinked to original sources

arXiv2023

Monolayer WS$_2$ electro- and photo-luminescence enhancement by TFSI treatment

Layered material heterostructures (LMHs) can be used to fabricate electroluminescent devices operating in the visible spectral region. A major advantage of LMH-light emitting diodes (LEDs) is that electroluminescence (EL) emission can be tuned across that of different exciton complexes (e.g. biexcitons, trions, quintons) by controlling the charge density. However, these devices have an EL quantum efficiency as low as$\sim$10$^{-4}$\%. Here, we show that the superacid bis-(triuoromethane)sulfonimide (TFSI) treatment of monolayer WS$_2$-LEDs boosts EL quantum efficiency by over one order of magnitude at room temperature. Non-treated devices emit light mainly from negatively charged excitons, while the emission in treated ones predominantly involves radiative recombination of neutral excitons. This paves the way to tunable and efficient LMH-LEDs

cond-mat.mtrl-sci↗

arXiv2022

Complex angular momentum theory of state-to state integral cross sections: resonance effects in the F+HD->HF(v'=3)+D reaction

State-to-state reactive integral cross sections (ICS) are often affected by quantum mechanical resonances, especially at relatively low energies. An ICS is usually obtained by summing partial waves at a given value of energy. For this reason, the knowledge of pole positions and residues in the complex energy plane is not sufficient for a quantitative description of the patterns produced by a resonance. Such description is available in terms of the poles of an S-matrix element in the complex plane of the total angular momentum. The approach was recently implemented in a computer code ICS_Regge, available in the public domain [Comp. Phys. Comm. 185 (2014) 2127]. In this paper, we employ the ICS Regge package to analyse in detail, for the first time, the resonance patterns predicted for the integral cross sections (ICS) of the benchmark F+HD->HF(v'=3)+D reaction. The v = 0, j = 0, Omega = 0 -> v' = 3, j'= 0,1,2, and Omega' = 0,1,2 transitions are studied for collision energies from 58.54 to 197.54 meV. For these energies, we find several resonances, whose contributions to the ICS vary from symmetric and asymmetric Fano shapes to smooth sinusoidal Regge oscillations. Complex energies of metastable states and Regge pole positions and residues are found by Pad /'e reconstruction of the scattering matrix elements. Accuracy of the ICS Regge code, relation between complex energies and Regge poles, various types of Regge trajectories, and the origin of the J-shifting approximation are also discussed.

quant-ph↗

arXiv2020

Graphene-Quantum Dots Hybrid Photodetectors with Low Dark-Current Readout

Graphene-based photodetectors have shown responsivities up to 10$^8$A/W and photoconductive gains up to 10$^{8}$ electrons per photon. These photodetectors rely on a highly absorbing layer in close proximity of graphene, which induces a shift of the graphene chemical potential upon absorption, hence modifying its channel resistance. However, due to the semi-metallic nature of graphene, the readout requires dark currents of hundreds of $μ$A up to mA, leading to high power consumption needed for the device operation. Here we propose a novel approach for highly responsive graphene-based photodetectors with orders of magnitude lower dark current levels. A shift of the graphene chemical potential caused by light absorption in a layer of colloidal quantum dots, induces a variation of the current flowing across a metal-insulator-graphene diode structure. Owing to the low density of states of graphene near the neutrality point, the light-induced shift in chemical potential can be relatively large, dramatically changing the amount of current flowing across the insulating barrier, and giving rise to a novel type of gain mechanism. This readout requires dark currents of hundreds of nA up to few $μ$A, orders of magnitude lower than other graphene-based photodetectors, while keeping responsivities of $\sim$70A/W in the infrared, almost two orders of magnitude higher compared to established germanium on silicon and indium gallium arsenide infrared photodetectors. This makes the device appealing for applications where high responsivity and low power consumption are required.

physics.app-ph↗

arXiv2019

Graphene Overcoats for Ultra-High Storage Density Magnetic Media

Hard disk drives (HDDs) are used as secondary storage in a number of digital electronic devices owing to low cost ($<$0.1\$/GB at 2016 prices) and large data storage capacity (10TB with a 3.5 inch HDD). Due to the exponentially increasing amount of data, there is a need to increase areal storage densities beyond$\sim$1Tb/in$^2$. This requires the thickness of carbon overcoats (COCs) to be$<$2nm. Friction, wear, corrosion, and thermal stability are critical concerns$<$2nm, where most of the protective properties of current COCs are lost. This limits current technology and restricts COC integration with heat assisted magnetic recording technology (HAMR), since this also requires laser irradiation stability. Here we show that graphene-based overcoats can overcome all these limitations. 2-4 layers of graphene enable two-fold reduction in friction and provide better corrosion and wear than state-of-the-art COCs. A single graphene layer is enough to reduce corrosion$\sim$2.5 times. We also show that graphene can withstand HAMR conditions. Thus, graphene-based overcoats can enable ultrahigh areal density HDDs$>$10Tb/in$^2$.

physics.app-ph↗

arXiv2019

High-mobility, wet-transferred graphene grown by chemical vapor deposition

We report high room-temperature mobility in single layer graphene grown by Chemical Vapor Deposition (CVD) after wet transfer on SiO$_2$ and hexagonal boron nitride (hBN) encapsulation. By removing contaminations trapped at the interfaces between single-crystal graphene and hBN, we achieve mobilities up to$\sim70000cm^2 V^{-1} s^{-1}$ at room temperature and$\sim120000cm^2 V^{-1} s^{-1}$ at 9K. These are over twice those of previous wet transferred graphene and comparable to samples prepared by dry transfer. We also investigate the combined approach of thermal annealing and encapsulation in polycrystalline graphene, achieving room temperature mobilities$\sim30000 cm^2 V^{-1} s^{-1}$. These results show that, with appropriate encapsulation and cleaning, room temperature mobilities well above $10000cm^2 V^{-1} s^{-1}$ can be obtained in samples grown by CVD and transferred using a conventional, easily scalable PMMA-based wet approach.

cond-mat.mes-hall↗

arXiv2019

Coherent anti-Stokes Raman Spectroscopy of single and multi-layer graphene

We report stimulated Raman spectroscopy of the G phonon in both single and multi-layer graphene, through Coherent anti-Stokes Raman Scattering (CARS). The signal generated by the third order nonlinearity is dominated by a vibrationally non-resonant background (NVRB), which obscures the Raman lineshape. We demonstrate that the vibrationally resonant CARS peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the NVRB. We model the observed spectra, taking into account the electronically resonant nature of both CARS and NVRB. We show that CARS can be used for graphene imaging with vibrational sensitivity.

cond-mat.mes-hall↗

arXiv2018

Direct observation of intravalley spin relaxation in single-layer WS$_2$

In monolayer Transition Metal Dichalcogenides (TMDs) the valence and conduction bands are spin split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the conduction band is such that the so-called dark exciton, consisting of an electron and a hole with opposite spin orientation, has lower energy than the A exciton. A possible mechanism leading to the transition from bright to dark excitons involves the scattering of the electrons from the upper to the lower conduction band state in K. Here we exploit the valley selective optical selection rules and use two-color helicity-resolved pump-probe spectroscopy to directly measure the intravalley spin-flip relaxation dynamics of electrons in the conduction band of single-layer WS$_2$. This process occurs on a sub-ps time scale and it is significantly dependent on the temperature, indicative of a phonon-assisted relaxation. These experimental results are supported by time-dependent ab-initio calculations which show that the intra-valley spin-flip scattering occurs on significantly longer time scales only exactly at the K point. In a realistic situation the occupation of states away from the minimum of the conduction band leads to a dramatic reduction of the scattering time.

cond-mat.mtrl-sci↗

arXiv2018

Raman spectroscopy of graphene under ultrafast laser excitation

The equilibrium optical phonons of graphene are well characterized in terms of anharmonicity and electron-phonon interactions, however their non-equilibrium properties in the presence of hot charge carriers are still not fully explored. Here we study the Raman spectrum of graphene under ultrafast laser excitation with 3ps pulses, which trade off between impulsive stimulation and spectral resolution. We localize energy into hot carriers, generating non-equilibrium temperatures in the ~1700-3100K range, far exceeding that of the phonon bath, while simultaneously detecting the Raman response. The linewidth of both G and 2D peaks show an increase as function of the electronic temperature. We explain this as a result of the Dirac cones' broadening and electron-phonon scattering in the highly excited transient regime, important for the emerging field of graphene-based photonics and optoelectronics.

cond-mat.mes-hall↗

arXiv2017

Broadband, electrically tuneable, third harmonic generation in graphene

Optical harmonic generation occurs when high intensity light ($>10^{10}$W/m$^{2}$) interacts with a nonlinear material. Electrical control of the nonlinear optical response enables applications such as gate-tunable switches and frequency converters. Graphene displays exceptionally strong-light matter interaction and electrically and broadband tunable third order nonlinear susceptibility. Here we show that the third harmonic generation efficiency in graphene can be tuned by over two orders of magnitude by controlling the Fermi energy and the incident photon energy. This is due to logarithmic resonances in the imaginary part of the nonlinear conductivity arising from multi-photon transitions. Thanks to the linear dispersion of the massless Dirac fermions, ultrabroadband electrical tunability can be achieved, paving the way to electrically-tuneable broadband frequency converters for applications in optical communications and signal processing.

cond-mat.mes-hall↗

arXiv2017

Vertically-Illuminated, Resonant-Cavity-Enhanced, Graphene-Silicon Schottky Photodetectors

We report vertically-illuminated, resonant cavity enhanced, graphene-Si Schottky photodetectors (PDs) operating at 1550nm. These exploit internal photoemission at the graphene-Si interface. To obtain spectral selectivity and enhance responsivity, the PDs are integrated with an optical cavity, resulting in multiple reflections at resonance, and enhanced absorption in graphene. Our devices have wavelength-dependent photoresponse with external (internal) responsivity~20mA/W (0.25A/W). The spectral-selectivity may be further tuned by varying the cavity resonant wavelength. Our devices pave the way for developing high responsivity hybrid graphene-Si free-space illuminated PDs for free-space optical communications, coherence optical tomography and light-radars

physics.app-ph↗

arXiv2016

Graphene-based, mid-infrared, room-temperature pyroelectric bolometers with ultrahigh temperature coefficient of resistance

Graphene is ideally suited for photonic and optoelectronic applications, with a variety of photodetectors (PDs) in the visible, near-infrared (NIR), and THz reported to date, as well as thermal detectors in the mid-infrared (MIR). Here, we present a room temperature-MIR-PD where the pyroelectric response of a LiNbO3 crystal is transduced with high gain (up to 200) into resistivity modulation for graphene, leading to a temperature coefficient of resistance up to 900%/K, two orders of magnitude higher than the state of the art, for a device area of 300x300um2. This is achieved by fabricating a floating metallic structure that concentrates the charge generated by the pyroelectric substrate on the top-gate capacitor of the graphene channel. This allows us to resolve temperature variations down to 15umK at 1 Hz, paving the way for a new generation of detectors for MIR imaging and spectroscopy

physics.ins-det↗

arXiv2015

High Responsivity, Large-Area Graphene/MoS2 Flexible Photodetectors

We present flexible photodetectors (PDs) for visible wavelengths fabricated by stacking centimetre-scale chemical vapour deposited (CVD) single layer graphene (SLG) and single layer CVD MoS2, both wet transferred onto a flexible polyethylene terephthalate substrate. The operation mechanism relies on injection of photoexcited electrons from MoS2 to the SLG channel. The external responsivity is 45.5A/W and the internal 570A/W at 642nm. This is at least two orders of magnitude higher than bulk-semiconductor flexible membranes and other flexible PDs based on graphene and layered materials. The photoconductive gain is up to 4x10^5. The photocurrent is in the 0.1-100 uA range. The devices are semi-transparent, with just 8% absorption at 642nm and work stably upon bending to a curvature of 6cm. These capabilities and the low voltage operation (<1V) make them attractive for wearable applications.

cond-mat.mtrl-sci↗

arXiv2015

Ultrafast pseudospin dynamics in graphene

Interband optical transitions in graphene are subject to pseudospin selection rules. Impulsive excitation with linearly polarized light generates an anisotropic photocarrier occupation in momentum space that evolves at timescales shorter than 100fs. Here, we investigate the evolution of non-equilibrium charges towards an isotropic distribution by means of fluence-dependent ultrafast spectroscopy and develop an analytical model able to quantify the isotropization process. In contrast to conventional semiconductors, the isotropization is governed by optical phonon emission, rather than electron-electron scattering, which nevertheless contributes in shaping the anisotropic photocarrier occupation within the first few fs.

cond-mat.mes-hall↗

arXiv2015

Valley and spin dynamics in monolayer MoS$_{2}$

Valleytronics targets the exploitation of the additional degrees of freedom in materials where the energy of the carriers may assume several equal minimum values (valleys) at non-equivalent points of the reciprocal space. In single layers of transition metal dichalcogenides (TMDs) the lack of inversion symmetry, combined with a large spin-orbit interaction, leads to a conduction (valence) band with different spin-polarized minima (maxima) having equal energies. This offers the opportunity to manipulate information at the level of the charge (electrons or holes), spin (up or down) and crystal momentum (valley). Any implementation of these concepts, however, needs to consider the robustness of such degrees of freedom, which are deeply intertwined. Here we address the spin and valley relaxation dynamics of both electrons and holes with a combination of ultrafast optical spectroscopy techniques, and determine the individual characteristic relaxation times of charge, spin and valley in a MoS$_{2}$ monolayer. These results lay the foundations for understanding the mechanisms of spin and valley polarization loss in two-dimensional TMDs: spin/valley polarizations survive almost two-orders of magnitude longer for holes, where spin and valley dynamics are interlocked, than for electrons, where these degrees of freedom are decoupled. This may lead to novel approaches for the integration of materials with large spin-orbit in robust spintronic/valleytronic platforms.

cond-mat.mtrl-sci↗