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See detailCoevaporation Stabilizes Tin-Based Perovskites in a Single Sn-Oxidation State
Singh, Ajay UL; Hieulle, Jeremy UL; Ferreira Machado, Joana Andreia UL et al

in Nano Letters (2022)

Chemically processed methylammonium tin-triiodide (CH3NH3SnI3) films include Sn in different oxidation states, leading to poor stability and low power conversion efficiency of the resulting solar cells ... [more ▼]

Chemically processed methylammonium tin-triiodide (CH3NH3SnI3) films include Sn in different oxidation states, leading to poor stability and low power conversion efficiency of the resulting solar cells (PSCs). The development of absorbers with Sn [2+] only has been identified as one of the critical steps to develop all Sn-based devices. Here, we report on coevaporation of CH3NH3I and SnI2 to obtain absorbers with Sn being only in the preferred oxidation state [+2] as confirmed by X-ray photoelectron spectroscopy. The Sn [4+]-free absorbers exhibit smooth highly crystalline surfaces and photoluminescence measurements corroborating their excellent optoelectronic properties. The films show very good stability under heat and light. Photoluminescence quantum yields up to 4 × 10^-3 translate in a quasi Fermi-level splittings exceeding 850 meV under one sun equivalent conditions showing high promise in developing lead-free, high efficiency, and stable PSCs. [less ▲]

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See detailNanomechanical Spectroscopy of 2D Materials
Kirchhof, Jan N.; Yu, Yuefeng; Antheaume, Gabriel et al

in Nano Letters (2022), 22(20), 8037--8044

We introduce a nanomechanical platform for fast and sensitive measurements of the spectrally resolved optical dielectric function of 2D materials. At the heart of our approach is a suspended 2D material ... [more ▼]

We introduce a nanomechanical platform for fast and sensitive measurements of the spectrally resolved optical dielectric function of 2D materials. At the heart of our approach is a suspended 2D material integrated into a high Q silicon nitride nanomechanical resonator illuminated by a wavelength-tunable laser source. From the heating-related frequency shift of the resonator as well as its optical reflection measured as a function of photon energy, we obtain the real and imaginary parts of the dielectric function. Our measurements are unaffected by substrate-related screening and do not require any assumptions on the underling optical constants. This fast ($\tau$rise∼135 ns), sensitive (noise-equivalent power = 90 pW/√Hz), and broadband (1.2-3.1 eV, extendable to UV-THz) method provides an attractive alternative to spectroscopic or ellipsometric characterization techniques. [less ▲]

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See detailElectrical Control over Phonon Polarization in Strained Graphene
Sonntag, Jens; Reichardt, Sven UL; Beschoten, Bernd et al

in Nano Letters (2021), 21(7), 2898--2904

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See detailMachine learning in nanoscience: big data at small scales
Brown, Keith A.; Brittman, Sarah; Maccaferri, Nicolò UL et al

in Nano Letters (2020), 20(1), 2-10

Recent advances in machine learning (ML) offer new tools to extract new insights from large data sets and to acquire small data sets more effectively. Researchers in nanoscience are experimenting with ... [more ▼]

Recent advances in machine learning (ML) offer new tools to extract new insights from large data sets and to acquire small data sets more effectively. Researchers in nanoscience are experimenting with these tools to tackle challenges in many fields. In addition to ML’s advancement of nanoscience, nanoscience provides the foundation for neuromorphic computing hardware to expand the implementation of ML algorithms. In this mini-review, which is not able to be comprehensive, we highlight some recent efforts to connect the ML and nanoscience communities focusing on three types of interaction: (1) using ML to analyze and extract new information from large nanoscience data sets, (2) applying ML to accelerate materials discovery, including the use of active learning to guide experimental design, and (3) the nanoscience of memristive devices to realize hardware tailored for ML. We conclude with a discussion of challenges and opportunities for future interactions between nanoscience and ML researchers. [less ▲]

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See detailSpeeding up nanoscience and nanotechnology with ultrafast plasmonics
Maccaferri, Nicolò UL; Meuret, Sophie; Kornienko, Nikolay et al

in Nano Letters (2020)

Surface plasmons are collective oscillations of free electrons at the interface between a conducting material and the dielectric environment. These excitations support the formation of strongly enhanced ... [more ▼]

Surface plasmons are collective oscillations of free electrons at the interface between a conducting material and the dielectric environment. These excitations support the formation of strongly enhanced and confined electromagnetic fields. As well, they display fast dynamics lasting tens of femtoseconds and can lead to a strong nonlinear optical response at the nanoscale. Thus, they represent the perfect tool to drive and control fast optical processes, such as ultrafast optical switching, single photon emission, as well as strong coupling interactions to explore and tailor photochemical reactions. In this Virtual Issue, we gather several important papers published in Nano Letters in the past decade reporting studies on the ultrafast dynamics of surface plasmons. [less ▲]

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See detailHyperbolic Meta-Antennas Enable Full Control of Scattering and Absorption of Light
Maccaferri, Nicolò UL; Zhao, Yingqi; Isoniemi, Tommi et al

in Nano Letters (2019), 19(3), 1851-1859

We introduce a novel concept of hybrid metal-dielectric meta-antenna supporting type II hyperbolic dispersion, which enables full control of absorption and scattering of light in the visible/near-infrared ... [more ▼]

We introduce a novel concept of hybrid metal-dielectric meta-antenna supporting type II hyperbolic dispersion, which enables full control of absorption and scattering of light in the visible/near-infrared spectral range. This ability lies in the different nature of the localized hyperbolic Bloch-like modes excited within the meta-antenna. The experimental evidence is corroborated by a comprehensive theoretical study. In particular, we demonstrate that two main modes, one radiative and one non-radiative, can be excited by direct coupling with the free-space radiation. We show that the scattering is the dominating electromagnetic decay channel, when an electric dipolar mode is induced in the system, whereas a strong absorption process occurs when a magnetic dipole is excited. Also, by varying the geometry of the system, the relative ratio of scattering and absorption, as well as their relative enhancement and/or quenching, can be tuned at will over a broad spectral range, thus enabling full control of the two channels. Importantly, both radiative and nonradiative modes supported by our architecture can be excited directly with far-field radiation. This is observed to occur even when the radiative channels (scattering) are almost totally suppressed, thereby making the proposed architecture suitable for practical applications. Finally, the hyperbolic meta-antennas possess both angular and polarization independent structural integrity, unlocking promising applications as hybrid meta-surfaces or as solvable nanostructures. [less ▲]

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See detailOn-Demand Intracellular Delivery of Single Particles in Single Cells by 3D Hollow Nanoelectrodes
Huang, Jian-An; Caprettini, Valeria; Zhao, Yingqi et al

in Nano Letters (2019), 19(2), 722-731

Delivery of molecules into intracellular compartments is one of the fundamental requirements in molecular biology. However, the possibility of delivering a precise number of nano-objects with single ... [more ▼]

Delivery of molecules into intracellular compartments is one of the fundamental requirements in molecular biology. However, the possibility of delivering a precise number of nano-objects with single-particle resolution is still an open challenge. Here we present an electrophoretic platform based on 3D hollow nanoelectrodes to enable delivery of single nanoparticles into single selected cells and monitoring of the single-particle delivery by surface-enhanced Raman scattering (SERS). The gold-coated hollow nanoelectrode capable of confinement and enhancement of electromagnetic fields upon laser illumination can distinguish the SERS signals of a single nanoparticle flowing through the nanoelectrode. Tight wrapping of cell membranes around the nanoelectrodes allows effective membrane electroporation such that single gold nanorods are delivered on demand into a living cell by electrophoresis. The capability of the 3D hollow nanoelectrodes to porate cells and reveal single emitters from the background in continuous flow is promising for the analysis of both intracellular delivery and sampling. [less ▲]

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See detailPlasmonic nanopores for single-molecule detection and manipulation: towards sequencing applications
Garoli, Denis; Yamazaki, Hirohito; Maccaferri, Nicolò UL et al

in Nano Letters (2019), 19(11), 7553-7562

Solid-state nanopore-based sensors are promising platforms for next-generation sequencing technologies, featuring label-free single-molecule sensitivity, rapid detection, and low-cost manufacturing. In ... [more ▼]

Solid-state nanopore-based sensors are promising platforms for next-generation sequencing technologies, featuring label-free single-molecule sensitivity, rapid detection, and low-cost manufacturing. In recent years, solid-state nanopores have been explored due to their miscellaneous fabrication methods and their use in a wide range of sensing applications. Here, we highlight a novel family of solid-state nanopores which have recently appeared, namely plasmonic nanopores. The use of plasmonic nanopores to engineer electromagnetic fields around a nanopore sensor allows for enhanced optical spectroscopies, local control over temperature, thermophoresis of molecules and ions to/from the sensor, and trapping of entities. This Mini Review offers a comprehensive understanding of the current state-of-the-art plasmonic nanopores for single-molecule detection and biomolecular sequencing applications and discusses the latest advances and future perspectives on plasmonic nanopore-based technologies. [less ▲]

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See detailChasing plasmons in flatland
Celano, Umberto; Maccaferri, Nicolò UL

in Nano Letters (2019), 19(11), 7549-7552

Two-dimensional layered crystals, including graphene and transition metal dichalcogenides, represent an interesting avenue for studying light-matter interactions at the nanoscale in confined geometries ... [more ▼]

Two-dimensional layered crystals, including graphene and transition metal dichalcogenides, represent an interesting avenue for studying light-matter interactions at the nanoscale in confined geometries. They offer several attractive properties, such as large exciton binding energies, strong excitonic resonances, and tunable bandgaps from the visible to the near-IR along with large spin–orbit coupling, direct band gap transitions, and valley-selective responses. [less ▲]

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See detailIntravalley Spin-Flip Relaxation Dynamics in Single-Layer WS2
Wang, Zilong; Molina-Sanchez, Alejandro; Altmann, Patrick et al

in NANO LETTERS (2018), 18(11), 6882-6891

In monolayer (1L) 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 ... [more ▼]

In monolayer (1L) 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 excitons, consisting of electrons and holes with opposite spin orientation, have lower energy than A excitons. The transition from bright to dark excitons involves the scattering of electrons from the upper to the lower conduction band at the K point of the Brillouin zone, with detrimental effects for the optoelectronic response of 1L-TMDs, since this reduces their light emission efficiency. 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 in 1L-WS2. This occurs on a sub-ps time scale, and it is significantly dependent on temperature, indicative of phonon-assisted relaxation. Time-dependent ab initio calculations show that intravalley spin-flip scattering occurs on significantly longer time scales only at the K point, while the occupation of states away from the minimum of the conduction band significantly reduces the scattering time. Our results shed light on the scattering processes determining the light emission efficiency in optoelectronic and photonic devices based on 1L-TMDs. [less ▲]

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See detailTailoring mechanically tunable strain fields in graphene
Goldsche, Matthias; Sonntag, Jens; Khodkov, Tymofiy et al

in Nano Letters (2018), 18(3), 1707--1713

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See detailMagnetic Control of the Chiroptical Plasmonic Surfaces
Zubritskaya, Irina; Maccaferri, Nicolò UL; Inchausti Ezeiza, Xabier et al

in Nano Letters (2018), 18(1), 302-307

A major challenge facing plasmon nanophotonics is the poor dynamic tunability. A functional nanophotonic element would feature the real-time sizable tunability of transmission, reflection of light's ... [more ▼]

A major challenge facing plasmon nanophotonics is the poor dynamic tunability. A functional nanophotonic element would feature the real-time sizable tunability of transmission, reflection of light's intensity or polarization over a broad range of wavelengths, and would be robust and easy to integrate. Several approaches have been explored so far including mechanical deformation, thermal, or refractive index effects, and all-optical switching. Here we devise an ultrathin chiroptical surface, built on two-dimensional nanoantennas, where the chiral light transmission is controlled by the externally applied magnetic field. The magnetic field-induced modulation of the far-field chiroptical response with this surface exceeds 100% in the visible and near-infrared spectral ranges, opening the route for nanometer-thin magnetoplasmonic light-modulating surfaces tuned in real time and featuring a broad spectral response. [less ▲]

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See detailAb Initio Calculations of Ultrashort Carrier Dynamics in Two-Dimensional Materials: Valley Depolarization in Single-Layer WSe2
Molina-Sanchez, Alejandro UL; Sangalli, Davide; Wirtz, Ludger UL et al

in Nano Letters (2017), 17

In single-layer WSe2, a paradigmatic semiconducting transition metal dichalcogenide, a circularly polarized laser field can selectively excite electronic transitions in one of the inequivalent K± valleys ... [more ▼]

In single-layer WSe2, a paradigmatic semiconducting transition metal dichalcogenide, a circularly polarized laser field can selectively excite electronic transitions in one of the inequivalent K± valleys. Such selective valley population corresponds to a pseudospin polarization. This can be used as a degree of freedom in a “valleytronic” device provided that the time scale for its depolarization is sufficiently large. Yet, the mechanism behind the valley depolarization still remains heavily debated. Recent time–dependent Kerr experiments have provided an accurate way to visualize the valley dynamics by measuring the rotation of a linearly polarized probe pulse applied after a circularly polarized pump pulse. We present here a clear, accurate and parameter–free description of the valley dynamics. By using an atomistic, ab initio approach we fully disclose the elemental mechanisms that dictate the depolarization effects. Our results are in excellent agreement with recent time–dependent Kerr experiments. We explain the Kerr dynamics and its temperature dependence in terms of electron–phonon me- diated processes that induce spin–flip inter–valley transitions. [less ▲]

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See detailTuning the Pseudospin Polarization of Graphene by a Pseudomagnetic Field
Georgi, Alexander; Nemes-Incze, Peter; Carrillo-Bastos, Ramon et al

in Nano Letters (2017), 17

One of the intriguing characteristics of honeycomb lattices is the appearance of a pseudomagnetic field as a result of mechanical deformation. In the case of graphene, the Landau quantization resulting ... [more ▼]

One of the intriguing characteristics of honeycomb lattices is the appearance of a pseudomagnetic field as a result of mechanical deformation. In the case of graphene, the Landau quantization resulting from this pseudomagnetic field has been measured using scanning tunneling microscopy. Here we show that a signature of the pseudomagnetic field is a local sublattice symmetry breaking observable as a redistribution of the local density of states. This can be interpreted as a polarization of graphene’s pseudospin due to a strain induced pseudomagnetic field, in analogy to the alignment of a real spin in a magnetic field. We reveal this sublattice symmetry breaking by tunably straining graphene using the tip of a scanning tunneling microscope. The tip locally lifts the graphene membrane from a SiO2 support, as visible by an increased slope of the I(z) curves. The amount of lifting is consistent with molecular dynamics calculations, which reveal a deformed graphene area under the tip in the shape of a Gaussian. The pseudomagnetic field induced by the deformation becomes visible as a sublattice symmetry breaking which scales with the lifting height of the strained deformation and therefore with the pseudomagnetic field strength. Its magnitude is quantitatively reproduced by analytic and tight-binding models, revealing fields of 1000 T. These results might be the starting point for an effective THz valley filter, as a basic element of valleytronics. [less ▲]

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See detailQuantum Interference Effects in Resonant Raman Spectroscopy of Single- and Triple-Layer MoTe2 from First-Principles
Pereira Coutada Miranda, Henrique UL; Reichardt, Sven UL; Froehlicher, Guillaume et al

in Nano Letters (2017), 17(4), 2381--2388

We present a combined experimental and theoretical study of resonant Raman spectroscopy in single- and triple-layer MoTe2. Raman intensities are computed entirely from first-principles by calculating ... [more ▼]

We present a combined experimental and theoretical study of resonant Raman spectroscopy in single- and triple-layer MoTe2. Raman intensities are computed entirely from first-principles by calculating finite differences of the dielectric susceptibility. In our analysis, we investigate the role of quantum interference effects and the electron−phonon coupling. With this method, we explain the experimentally observed intensity inversion of the A′1 vibrational modes in triple-layer MoTe2 with increasing laser photon energy. Finally, we show that a quantitative comparison with experimental data requires the proper inclusion of excitonic effects. [less ▲]

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See detailAnisotropic Nanoantenna-Based Magnetoplasmonic Crystals for Highly Enhanced and Tunable Magneto-Optical Activity
Maccaferri, Nicolò UL; Bergamini, Luca; Pancaldi, Matteo et al

in Nano Letters (2016), 16(4), 2533-2542

We present a novel concept of a magnetically tunable plasmonic crystal based on the excitation of Fano lattice surface modes in periodic arrays of magnetic and optically anisotropic nanoantennas. We show ... [more ▼]

We present a novel concept of a magnetically tunable plasmonic crystal based on the excitation of Fano lattice surface modes in periodic arrays of magnetic and optically anisotropic nanoantennas. We show how coherent diffractive far-field coupling between elliptical nickel nanoantennas is governed by the two in-plane, orthogonal and spectrally detuned plasmonic responses of the individual building block, one directly induced by the incident radiation and the other induced by the application of an external magnetic field. The consequent excitation of magnetic field-induced Fano lattice surface modes leads to highly tunable and amplified magneto-optical effects as compared to a continuous film or metasurfaces made of disordered noninteracting magnetoplasmonic anisotropic nanoantennas. The concepts presented here can be exploited to design novel magnetoplasmonic sensors based on coupled localized plasmonic resonances, and nanoscale metamaterials for precise control and magnetically driven tunability of light polarization states. [less ▲]

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See detailUnified Description of the Optical Phonon Modes in N-Layer MoTe2
Froehlicher, Guillaume; Lorchat, Etienne; Fernique, François et al

in Nano Letters (2015), 15

N-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three-dimensional) and monolayer (quasi-two-dimensional) limits ... [more ▼]

N-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three-dimensional) and monolayer (quasi-two-dimensional) limits. Here, using high-resolution micro-Raman spectroscopy, we report a unified experimental description of the Γ-point optical phonons in N-layer 2H-molybdenum ditelluride (MoTe2). We observe series of N-dependent low-frequency interlayer shear and breathing modes (below 40 cm–1, denoted LSM and LBM) and well-defined Davydov splittings of the mid-frequency modes (in the range 100–200 cm–1, denoted iX and oX), which solely involve displacements of the chalcogen atoms. In contrast, the high-frequency modes (in the range 200–300 cm–1, denoted iMX and oMX), arising from displacements of both the metal and chalcogen atoms, exhibit considerably reduced splittings. The manifold of phonon modes associated with the in-plane and out-of-plane displacements are quantitatively described by a force constant model, including interactions up to the second nearest neighbor and surface effects as fitting parameters. The splittings for the iX and oX modes observed in N-layer crystals are directly correlated to the corresponding bulk Davydov splittings between the E2u/E1g and B1u/A1g modes, respectively, and provide a measurement of the frequencies of the bulk silent E2u and B1u optical phonon modes. Our analysis could readily be generalized to other layered crystals [less ▲]

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See detailLow B field magneto-phonon resonances in single-layer and bilayer graphene
Neumann, Christoph; Reichardt, Sven UL; Drögeler, Marc et al

in Nano Letters (2015), 15(3), 1547--1552

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See detailActive Magnetoplasmonic Ruler
Zubritskaya, Irina; Lodewijks, Kristof; Maccaferri, Nicolò UL et al

in Nano Letters (2015), 15(5), 3204-3211

Plasmon rulers are an emerging concept in which the strong near-field coupling of plasmon nanoantenna elements is employed to obtain structural information at the nanoscale. Here, we combine ... [more ▼]

Plasmon rulers are an emerging concept in which the strong near-field coupling of plasmon nanoantenna elements is employed to obtain structural information at the nanoscale. Here, we combine nanoplasmonics and nanomagnetism to conceptualize a magnetoplasmonic dimer nanoantenna that would be able to report nanoscale distances while optimizing its own spatial orientation. The latter constitutes an active operation in which a dynamically optimized optical response per measured unit length allows for the measurement of small and large nanoscale distances with about 2 orders of magnitude higher precision than current state-of-the-art plasmon rulers. We further propose a concept to optically measure the nanoscale response to the controlled application of force with a magnetic field. [less ▲]

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See detailMagnetoplasmonic Design Rules for Active Magneto-Optics
Lodewijks, Kristof; Maccaferri, Nicolò UL; Pakizeh, Tavakol et al

in Nano Letters (2014), 14(12), 7207-7214

Light polarization rotators and nonreciprocal optical isolators are essential building blocks in photonics technology. These macroscopic passive devices are commonly based on magneto-optical Faraday and ... [more ▼]

Light polarization rotators and nonreciprocal optical isolators are essential building blocks in photonics technology. These macroscopic passive devices are commonly based on magneto-optical Faraday and Kerr polarization rotation. Magnetoplasmonics, the combination of magnetism and plasmonics, is a promising route to bring these devices to the nanoscale. We introduce design rules for highly tunable active magnetoplasmonic elements in which we can tailor the amplitude and sign of the Kerr response over a broad spectral range. [less ▲]

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