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1.
ACS Appl Mater Interfaces ; 15(43): 50237-50245, 2023 Nov 01.
Article in English | MEDLINE | ID: mdl-37862590

ABSTRACT

Properly tuning the Fermi level position in topological insulators is of vital importance to tailor their spin-polarized electronic transport and to improve the efficiency of any functional device based on them. Here, we report the full in situ metal organic chemical vapor deposition (MOCVD) and study of a highly crystalline Bi2Te3/Sb2Te3 topological insulator heterostructure on top of large area (4″) Si(111) substrates. The bottom Sb2Te3 layer serves as an ideal seed layer for the growth of highly crystalline Bi2Te3 on top, also inducing a remarkable shift of the Fermi level to place it very close to the Dirac point, as visualized by angle-resolved photoemission spectroscopy. To exploit such ideal topologically protected surface states, we fabricate the simple spin-charge converter Si(111)/Sb2Te3/Bi2Te3/Au/Co/Au and probe the spin-charge conversion (SCC) by spin pumping ferromagnetic resonance. A large SCC is measured at room temperature and is interpreted within the inverse Edelstein effect, thus resulting in a conversion efficiency of λIEEE ∼ 0.44 nm. Our results demonstrate the successful tuning of the surface Fermi level of Bi2Te3 when grown on top of Sb2Te3 with a full in situ MOCVD process, which is highly interesting in view of its future technology transfer.

2.
Nanomaterials (Basel) ; 13(6)2023 Mar 08.
Article in English | MEDLINE | ID: mdl-36985871

ABSTRACT

In vitro and in vivo stimulation and recording of neuron action potential is currently achieved with microelectrode arrays, either in planar or 3D geometries, adopting different materials and strategies. IrO2 is a conductive oxide known for its excellent biocompatibility, good adhesion on different substrates, and charge injection capabilities higher than noble metals. Atomic layer deposition (ALD) allows excellent conformal growth, which can be exploited on 3D nanoelectrode arrays. In this work, we disclose the growth of nanocrystalline rutile IrO2 at T = 150 °C adopting a new plasma-assisted ALD (PA-ALD) process. The morphological, structural, physical, chemical, and electrochemical properties of the IrO2 thin films are reported. To the best of our knowledge, the electrochemical characterization of the electrode/electrolyte interface in terms of charge injection capacity, charge storage capacity, and double-layer capacitance for IrO2 grown by PA-ALD was not reported yet. IrO2 grown on PtSi reveals a double-layer capacitance (Cdl) above 300 µF∙cm-2, and a charge injection capacity of 0.22 ± 0.01 mC∙cm-2 for an electrode of 1.0 cm2, confirming IrO2 grown by PA-ALD as an excellent material for neuroelectronic applications.

3.
Nanomaterials (Basel) ; 14(1)2023 Dec 20.
Article in English | MEDLINE | ID: mdl-38202475

ABSTRACT

In a previous investigation, the authors proposed nitrogen as a possible candidate for exploiting the donor spin in silicon quantum devices. This system is characterized by a ground state deeper than the other group V impurities in silicon, offering less stringent requirements on the device temperature necessary to access the unionized state. The nitrogen donor is slightly displaced from the substitutional site, and upon heating, the system undergoes a motional transition. In the present article, we show the results from our investigation on the spin-relaxation times in natSi and 28Si substrates and discuss the motional effects on relaxation. The stretched exponential relaxation observed is interpreted as a distribution of spin-lattice relaxation times, whose origin is also discussed. This information greatly contributes to the assessment of a nitrogen-doped silicon system as a potential candidate for quantum devices working at temperatures higher than those required for other group V donors in silicon.

4.
Chem Mater ; 34(19): 8603-8612, 2022 Oct 11.
Article in English | MEDLINE | ID: mdl-36248232

ABSTRACT

In this work, we report the hot-injection synthesis of Cs3ZnCl5 colloidal nanocrystals (NCs) with tunable amounts of Cu+ and Mn2+ substituent cations. All the samples had a rodlike morphology, with a diameter of ∼14 nm and a length of ∼30-100 nm. Alloying did not alter the crystal structure of the host Cs3ZnCl5 NCs, and Cu ions were mainly introduced in the oxidation state +1 according to X-ray photoelectron and electron paramagnetic resonance spectroscopies. The spectroscopic analysis of unalloyed, Cu-alloyed, Mn-alloyed, and Cu, Mn coalloyed NCs indicated that (i) the Cs3ZnCl5 NCs have a large band gap of ∼5.35 eV; (ii) Cu(I) aliovalent alloying leads to an absorption shoulder/peak at ∼4.8 eV and cyan photoluminescence (PL) peaked at 2.50 eV; (iii) Mn(II) isovalent alloying leads to weak Mn PL, which intensifies remarkably in the coalloyed samples, prompted by an energy transfer (ET) process between the Cu and Mn centers, favored by the overlap between the lowest (6A1 → 4T1) transition for tetrahedrally coordinated Mn2+ and the PL profile from Cu(I) species in the Cs3ZnCl5 NCs. The efficiency of this ET process reaches a value of 61% for the sample with the highest extent of Mn alloying. The PL quantum yield (QY) values in these Cu, Mn coalloyed NCs are lower at higher Mn contents. The analysis of the Mn PL dynamics in these samples indicates that this PL drop stems from inter-Mn exciton migration, which increases the likelihood of trapping in defect sites, in agreement with previous studies.

5.
J Magn Reson ; 334: 107102, 2022 Jan.
Article in English | MEDLINE | ID: mdl-34847488

ABSTRACT

The field of electron spin resonance (ESR) is in constant need of improving its capabilities. Among other things, this means having better resonators to reach improved spin sensitivity and enable larger microwave-power-to-microwave-magnetic-field conversion factors. Surface micro-resonators, made of small metallic patches on a dielectric substrate, provide very good absolute spin sensitivity and high conversion factors due to their very small mode volume. However, such resonators suffer from relatively low spin concentration sensitivity and a low-quality factor, a fact that offsets some of their significant potential advantages. The use of superconducting patches to replace the metallic layer seems a reasonable and straightforward solution to the quality factor issue, at least for measurements carried out at cryogenic temperatures. Nevertheless, superconducting materials, especially those that can operate at moderate cryogenic temperatures, are not easily incorporated into setups requiring high magnetic fields due to the electric current vortices generated in the latter's surface. This makes the transition from normal conducting materials to superconductors highly nontrivial. Here we present the design, fabrication, and testing results of surface micro-resonators made of yttrium barium copper oxide (YBCO), a superconducting material that operates also at high magnetic fields and makes it possible to pursue ESR at moderate cryogenic temperatures (up to ∼ 80 K). We show that with a unique experimental setup, these resonators can be made to operate well even at high fields of ∼ 1.2 T. Furthermore, we analyze the effect of current vortices on the ESR signal and the spins' coherence times. Finally, we provide a head-to-head comparison of YBCO vs copper resonators of the same dimensions, which clearly shows their pros and cons and directs us to future potential developments and improvements in this field.

6.
Nano Lett ; 21(14): 6211-6219, 2021 Jul 28.
Article in English | MEDLINE | ID: mdl-34260252

ABSTRACT

Controlled insertion of electronic states within the band gap of semiconductor nanocrystals (NCs) is a powerful tool for tuning their physical properties. One compelling example is II-VI NCs incorporating heterovalent coinage metals in which hole capture produces acceptor-bound excitons. To date, the opposite donor-bound exciton scheme has not been realized because of the unavailability of suitable donor dopants. Here, we produce a model system for donor-bound excitons in CdSeS NCs engineered with sulfur vacancies (VS) that introduce a donor state below the conduction band (CB), resulting in long-lived intragap luminescence. VS-localized electrons are almost unaffected by trapping, and suppression of thermal quenching boosts the emission efficiency to 85%. Magneto-optical measurements indicate that the VS are not magnetically coupled to the NC bands and that the polarization properties are determined by the spin of the valence-band photohole, whose spin flip is massively slowed down due to suppressed exchange interaction with the donor-localized electron.

7.
Chem Mater ; 32(13): 5897-5903, 2020 Jul 14.
Article in English | MEDLINE | ID: mdl-33814699

ABSTRACT

We report here the synthesis of undoped and Cu-doped Cs2ZnCl4 nanocrystals (NCs) in which we could tune the concentration of Cu from 0.7 to 7.5%. Cs2ZnCl4 has a wide band gap (4.8 eV), and its crystal structure is composed of isolated ZnCl4 tetrahedra surrounded by Cs+ cations. According to our electron paramagnetic resonance analysis, in 0.7 and 2.1% Cu-doped NCs the Cu ions were present in the +1 oxidation state only, while in NCs at higher Cu concentrations we could detect Cu(II) ions (isovalently substituting the Zn(II) ions). The undoped Cs2ZnCl4 NCs were non emissive, while the Cu-doped samples had a bright intragap photoluminescence (PL) at ∼2.6 eV mediated by band-edge absorption. Interestingly, the PL quantum yield was maximum (∼55%) for the samples with a low Cu concentration ([Cu] ≤ 2.1%), and it systematically decreased when further increasing the concentration of Cu, reaching 15% for the NCs with the highest doping level ([Cu] = 7.5%). The same (∼2.55 eV) emission band was detected under X-ray excitation. Our density functional theory calculations indicated that the PL emission could be ascribed only to Cu(I) ions: these ions promote the formation of trapped excitons, through which an efficient emission takes place. Overall, these Cu-doped Cs2ZnCl4 NCs, with their high photo- and radio-luminescence emission in the blue spectral region that is free from reabsorption, are particularly suitable for applications in ionizing radiation detection.

8.
J Am Chem Soc ; 140(40): 12989-12995, 2018 Oct 10.
Article in English | MEDLINE | ID: mdl-30198712

ABSTRACT

We show here the first colloidal synthesis of double perovskite Cs2AgInCl6 nanocrystals (NCs) with a control over their size distribution. In our approach, metal carboxylate precursors and ligands (oleylamine and oleic acid) are dissolved in diphenyl ether and reacted at 105 °C with benzoyl chloride. The resulting Cs2AgInCl6 NCs exhibit the expected double perovskite crystal structure, are stable under air, and show a broad spectrum white photoluminescence (PL) with quantum yield of ∼1.6 ± 1%. The optical properties of these NCs were improved by synthesizing Mn-doped Cs2AgInCl6 NCs through the simple addition of Mn-acetate to the reaction mixture. The NC products were characterized by the same double perovskite crystal structure, and Mn doping levels up to 1.5%, as confirmed by elemental analyses. The effective incorporation of Mn ions inside Cs2AgInCl6 NCs was also proved by means of electron spin resonance spectroscopy. A bright orange emission characterized our Mn-doped Cs2AgInCl6 NCs with a PL quantum yield as high as ∼16 ± 4%.

9.
Nat Commun ; 7: 13886, 2016 12 21.
Article in English | MEDLINE | ID: mdl-28000670

ABSTRACT

Control of electron spin coherence via external fields is fundamental in spintronics. Its implementation demands a host material that accommodates the desirable but contrasting requirements of spin robustness against relaxation mechanisms and sizeable coupling between spin and orbital motion of the carriers. Here, we focus on Ge, which is a prominent candidate for shuttling spin quantum bits into the mainstream Si electronics. So far, however, the intrinsic spin-dependent phenomena of free electrons in conventional Ge/Si heterojunctions have proved to be elusive because of epitaxy constraints and an unfavourable band alignment. We overcome these fundamental limitations by investigating a two-dimensional electron gas in quantum wells of pure Ge grown on Si. These epitaxial systems demonstrate exceptionally long spin lifetimes. In particular, by fine-tuning quantum confinement we demonstrate that the electron Landé g factor can be engineered in our CMOS-compatible architecture over a range previously inaccessible for Si spintronics.

10.
Front Neurosci ; 10: 482, 2016.
Article in English | MEDLINE | ID: mdl-27826226

ABSTRACT

Emerging brain-inspired architectures call for devices that can emulate the functionality of biological synapses in order to implement new efficient computational schemes able to solve ill-posed problems. Various devices and solutions are still under investigation and, in this respect, a challenge is opened to the researchers in the field. Indeed, the optimal candidate is a device able to reproduce the complete functionality of a synapse, i.e., the typical synaptic process underlying learning in biological systems (activity-dependent synaptic plasticity). This implies a device able to change its resistance (synaptic strength, or weight) upon proper electrical stimuli (synaptic activity) and showing several stable resistive states throughout its dynamic range (analog behavior). Moreover, it should be able to perform spike timing dependent plasticity (STDP), an associative homosynaptic plasticity learning rule based on the delay time between the two firing neurons the synapse is connected to. This rule is a fundamental learning protocol in state-of-art networks, because it allows unsupervised learning. Notwithstanding this fact, STDP-based unsupervised learning has been proposed several times mainly for binary synapses rather than multilevel synapses composed of many binary memristors. This paper proposes an HfO2-based analog memristor as a synaptic element which performs STDP within a small spiking neuromorphic network operating unsupervised learning for character recognition. The trained network is able to recognize five characters even in case incomplete or noisy images are displayed and it is robust to a device-to-device variability of up to ±30%.

11.
Nat Nanotechnol ; 10(3): 227-31, 2015 Mar.
Article in English | MEDLINE | ID: mdl-25643256

ABSTRACT

Free-standing silicene, a silicon analogue of graphene, has a buckled honeycomb lattice and, because of its Dirac bandstructure combined with its sensitive surface, offers the potential for a widely tunable two-dimensional monolayer, where external fields and interface interactions can be exploited to influence fundamental properties such as bandgap and band character for future nanoelectronic devices. The quantum spin Hall effect, chiral superconductivity, giant magnetoresistance and various exotic field-dependent states have been predicted in monolayer silicene. Despite recent progress regarding the epitaxial synthesis of silicene and investigation of its electronic properties, to date there has been no report of experimental silicene devices because of its air stability issue. Here, we report a silicene field-effect transistor, corroborating theoretical expectations regarding its ambipolar Dirac charge transport, with a measured room-temperature mobility of ∼100 cm(2) V(-1) s(-1) attributed to acoustic phonon-limited transport and grain boundary scattering. These results are enabled by a growth-transfer-fabrication process that we have devised--silicene encapsulated delamination with native electrodes. This approach addresses a major challenge for material preservation of silicene during transfer and device fabrication and is applicable to other air-sensitive two-dimensional materials such as germanene and phosphorene. Silicene's allotropic affinity with bulk silicon and its low-temperature synthesis compared with graphene or alternative two-dimensional semiconductors suggest a more direct integration with ubiquitous semiconductor technology.

12.
ACS Appl Mater Interfaces ; 6(5): 3455-61, 2014 Mar 12.
Article in English | MEDLINE | ID: mdl-24512108

ABSTRACT

Al:HfO2 is grown on III-V compound substrates by atomic layer deposition after an in situ trimethylaluminum-based preconditioning treatment of the III-V surface. After post-deposition rapid thermal annealing at 700 °C, the cubic/tetragonal crystalline phase is stabilized and the chemical composition of the stack is preserved. The observed structural evolution of Al:HfO2 on preconditioned III-V substrates shows that the in-diffusion of semiconductor species from the substrate through the oxide is inhibited. Al-induced stabilization of the Al:HfO2 crystal polymorphs up to 700 °C can be used as a permittivity booster methodology with possibly important implications in the stack scaling issues of high-mobility III-V based logic applications.

13.
Adv Mater ; 26(13): 2096-101, 2014 Apr 02.
Article in English | MEDLINE | ID: mdl-24347540

ABSTRACT

The structural and electronic properties of a Si nanosheet (NS) grown onto a MoS2 substrate by means of molecular beam epitaxy are assessed. Epitaxially grown Si is shown to adapt to the trigonal prismatic surface lattice of MoS2 by forming two-dimensional nanodomains. The Si layer structure is distinguished from the underlying MoS2 surface structure. The local electronic properties of the Si nanosheet are dictated by the atomistic arrangement of the layer and unlike the MoS2 hosting substrate they are qualified by a gap-less density of states.

14.
Nano Lett ; 13(10): 4963-8, 2013 Oct 09.
Article in English | MEDLINE | ID: mdl-23984940

ABSTRACT

The localization of the donor electron wave function can be of key importance in various silicon applications, since for example it determines the interactions between neighboring donors. Interestingly, the physical confinement of the electrons in quasi-one-dimensional nanostructures, like silicon nanowires, noticeably affects this property. Using fully ab initio calculations, we show that the delocalization of the donor electron wave function along the axis of a nanowire is much greater in [011] oriented nanowires for phosphorus and selenium donors. We also demonstrate that its value can be controlled by applying a compressive or tensile uniaxial strain. Finally, we discuss the implications of these features from both an experimental and a theoretical point of view.

16.
Nanotechnology ; 23(21): 215204, 2012 Jun 01.
Article in English | MEDLINE | ID: mdl-22552118

ABSTRACT

We report the electronic transport on n-type silicon single electron transistors (SETs) fabricated in complementary metal oxide semiconductor (CMOS) technology. The n-type metal oxide silicon SETs (n-MOSSETs) are built within a pre-industrial fully depleted silicon on insulator (FDSOI) technology with a silicon thickness down to 10 nm on 200 mm wafers. The nominal channel size of 20 × 20 nm(2) is obtained by employing electron beam lithography for active and gate level patterning. The Coulomb blockade stability diagram is precisely resolved at 4.2 K and it exhibits large addition energies of tens of meV. The confinement of the electrons in the quantum dot has been modeled by using a current spin density functional theory (CS-DFT) method. CMOS technology enables massive production of SETs for ultimate nanoelectronic and quantum variable based devices.


Subject(s)
Metals/chemistry , Nanostructures/chemistry , Nanotechnology/instrumentation , Semiconductors , Silicon/chemistry , Transistors, Electronic , Electron Transport , Equipment Design , Equipment Failure Analysis , Nanostructures/ultrastructure , Particle Size
17.
Nano Lett ; 12(3): 1509-15, 2012 Mar 14.
Article in English | MEDLINE | ID: mdl-22364321

ABSTRACT

The self-assembly of Ge(1)Sb(2)Te(4) nanowires (NWs) for phase change memories application was achieved by metal organic chemical vapor deposition, catalyzed by Au nanoislands in a narrow range of temperatures and deposition pressures. In the optimized conditions of 400 °C, 50 mbar, the NWs are Ge(1)Sb(2)Te(4) single hexagonal crystals. Phase change memory switching was reversibly induced by nanosecond current pulses through metal-contacted NWs with threshold voltage of about 1.35 V.


Subject(s)
Crystallization/methods , Gases/chemistry , Metals/chemistry , Nanostructures/chemistry , Nanostructures/ultrastructure , Organic Chemicals/chemistry , Macromolecular Substances/chemistry , Materials Testing , Molecular Conformation , Particle Size , Phase Transition , Surface Properties
18.
Nano Lett ; 11(11): 4509-14, 2011 Nov 09.
Article in English | MEDLINE | ID: mdl-21950460

ABSTRACT

We report a density functional study of the electronic properties and hyperfine structure of substitutional selenium in silicon nanowires using plane-wave pseudopotential techniques. We simulated hydrogen passivated [001] oriented nanowires with a diameter up to 2 nm, analyzing the effect of quantum confinement on the defect formation energy and on the hyperfine parameters as a function of the diameter and of the defect position. We show that substitutional Se in silicon has favorable configurations for positions near the surface with possible formation of chalcogen-hydrogen complexes. We also show that hyperfine interactions increase at small diameters, as long as the nanowire is large enough to prevent surface distortion which modifies the symmetry of the donor wave function. Moreover, surface effects lead to strong differences in the hyperfine parameters depending on the Se location inside the nanowire, allowing the identification of an impurity site on the basis of electron paramagnetic resonance spectra.


Subject(s)
Hydrogen/chemistry , Models, Chemical , Nanotubes/chemistry , Nanotubes/ultrastructure , Selenium/chemistry , Silicon/chemistry , Computer Simulation , Diffusion
19.
J Nanosci Nanotechnol ; 10(4): 2650-5, 2010 Apr.
Article in English | MEDLINE | ID: mdl-20355479

ABSTRACT

We review the effects of microwave irradiation on low dimensional electron systems in Silicon nanostructures. Depending on the temperature and the energy scales involved, different effects may be observed on the transition probabilities of elastic and inelastic processes. In particular two cases of 0 dimensional confinement are analyzed, i.e., the trapping of a single electron in point defects close to a two dimensional electron system, and in single donor atoms trapped in the channel of a nanoMOSFET. Microwave dependent capture and emission phenomena and photon assisted tunneling are described in such kind of systems. Consequences on the single spin resonance detection and on the spin manipulation are discussed.

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