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Nicolas Ubrig

Publications and source records attributed to Nicolas Ubrig.

At least 19 recordsLinked to original sources

Beam Routing through Excitons in Transition Metal Dichalcogenide Monolayers

Routing light at the nanoscale typically relies on nanostructured surfaces to imprint directionality on the emission. Using low-temperature, angle-resolved cathodoluminescence spectroscopy, we show that the intrinsic excitonic transitions of a semiconductor can themselves produce routed emission. We probe monolayers of WSe$_2$, MoSe$_2$, and MoTe$_2$ and resolve the excitonic species of monolayer WSe$_2$ -- the bright exciton, the trion, and the spin-forbidden dark exciton -- through their distinct angular emission profiles. While the in-plane transition dipoles of the bright exciton and trion radiate predominantly toward the surface normal, the out-of-plane dipole of the dark exciton, inaccessible under normal-incidence optical excitation, produces a directional emission channel at large angles. We further tune the balance between neutral and charged exciton emission through the local dielectric environment. Our results establish dark excitons in TMD monolayers as a platform for directional light emission in compact photonic architectures without additional nanostructuring.

cond-mat.mtrl-sci

Signatures of collective photon emission and ferroelectric ordering of excitons near their Mott insulating state in a WSe$_2$/WS$_2$ heterobilayer

Spontaneous symmetry breaking, arising from the competition of interactions and quantum fluctuations, is fundamental to understanding ordered electronic phases. Although electrically neutral, optical excitations like excitons can interact through their dipole moment, raising the possibility of optically active ordered phases. The effects of spontaneous ordering on optical properties remain largely unexplored. Recent observations of the excitonic Mott insulating state in semiconducting moir\'e crystals make them promising for addressing this question. Here, we present evidence for an in-plane ferroelectric phase of dipolar moir\'e excitons driven by strong exciton-exciton interactions. We discover a surprising speed-up of photon emission at late times and low densities in excitonic decay. This counterintuitive behavior is attributed to collective radiance, linked to the transition between disordered and symmetry-broken ferroelectric phases of moir\'e excitons. Our findings provide first evidence for strong dipolar inter-site interactions in moir\'e lattices, demonstrate collective photon emission as a probe for moir\'e quantum materials, and pave the way for exploring cooperative optical phenomena in strongly correlated systems.

cond-mat.mes-hall

Positive oscillating magnetoresistance in a van der Waals antiferromagnetic semiconductor

In all van der Waals layered antiferromagnetic semiconductors investigated so far a negative magnetoresistance has been observed in vertical transport measurements, with characteristic trends that do not depend on applied bias. Here we report vertical transport measurements on layered antiferromagnetic semiconductor CrPS$_4$ that exhibit a drastically different behavior, namely a strongly bias dependent, positive magnetoresistance that is accompanied by pronounced oscillations for devices whose thickness is smaller than 10 nm. We establish that this unexpected behavior originates from transport being space-charge limited, and not injection limited as for layered antiferromagetic semiconductors studid earlier. Our analysis indicates that the positive magnetoresistance and the oscillations only occur when electrons are injected into in-gap defect states, whereas when electrons are injected into the conduction band the magnetoresistance vanishes. We propose a microscopic explanation for the observed phenomena that combines concepts typical of transport through disordered semiconductors with known properties of the CrPS$_4$ magnetic state, which captures all basic experimental observations. Our results illustrate the need to understand in detail the nature of transport through vdW magnets, to extract information about the nature of the order magnetic states and its microscopic properties.

cond-mat.mes-hall

Brightened Optical Transition as Indicator of Multiferroicity in a Layered Antiferromagnet

Two-dimensional van der Waals magnets show strong interconnection between their electrical, magnetic, and structural properties. Here we reveal the emergence of a luminescent transition upon crossing the N\'eel transition temperature of CrPS$_4$, a layered antiferromagnetic semiconductor. This luminescent transition occurs above the lowest absorption level. We attribute the optical transitions to excited states of the t$_{\rm 2g}$ orbitals of the Cr$^{3+}$ ions, which are influenced by the distortion of the octahedral crystal field. Specifically, we find at the crossing of the N\'eel temperature changes the distortion from an anti-polar to polar arrangement, thereby not only activating an additional luminescent pathway but also inducing a significant in-plane static dipole moment detected by a marked enhancement in the intensity of the second harmonic generation. Our findings suggest the presence of a multiferroic state in CrPS$_4$ below the N\'eel temperature.

cond-mat.mtrl-sci

Multiple antiferromagnetic phases and magnetic anisotropy in exfoliated CrBr$_3$ multilayers

In twisted two-dimensional (2D) magnets, the stacking dependence of the magnetic exchange interaction can lead to regions of ferromagnetic and antiferromagnetic interlayer order, separated by non-collinear, skyrmion-like spin textures. Recent experimental searches for these textures have focused on CrI$_3$, known to exhibit either ferromagnetic or antiferromagnetic interlayer order, depending on layer stacking. However, the very strong uniaxial anisotropy of CrI$_3$ disfavors smooth non-collinear phases in twisted bilayers. Here, we report the experimental observation of three distinct magnetic phases -- one ferromagnetic and two antiferromagnetic -- in exfoliated CrBr$_3$ multilayers, and reveal that the uniaxial anisotropy is significantly smaller than in CrI$_3$. These results are obtained by magnetoconductance measurements on CrBr$_3$ tunnel barriers and Raman spectroscopy, in conjunction with density functional theory calculations, which enable us to identify the stackings responsible for the different interlayer magnetic couplings. The detection of all locally stable magnetic states predicted to exist in CrBr$_3$ and the excellent agreement found between theory and experiments, provide complete information on the stacking-dependent interlayer exchange energy and establish twisted bilayer CrBr$_3$ as an ideal system to deterministically create non-collinear magnetic phases.

cond-mat.mtrl-sci

Gate-controlled Magnetotransport and Electrostatic Modulation of Magnetism in 2D magnetic semiconductor CrPS$_4$

Using field-effect transistors (FETs) to explore atomically thin magnetic semiconductors with transport measurements is difficult, because the very narrow bands of most 2D magnetic semiconductors cause carrier localization, preventing transistor operation. Here, we show that exfoliated layers of CrPS$_4$ -- a 2D layered antiferromagnetic semiconductor whose bandwidth approaches 1 eV -- allow the realization of FETs that operate properly down to cryogenic temperature. Using these devices, we perform conductance measurements as a function of temperature and magnetic field, to determine the full magnetic phase diagram, which includes a spin-flop and a spin-flip phase. We find that the magnetoconductance depends strongly on gate voltage, reaching values as high as 5000 % near the threshold for electron conduction. The gate voltage also allows the magnetic states to be tuned, despite the relatively large thickness of the CrPS$_4$ multilayers employed in our study. Our results show the need to employ 2D magnetic semiconductors with sufficiently large bandwidth to realize properly functioning transistors, and identify a candidate material to realize a fully gate-tunable half-metallic conductor.

cond-mat.mes-hall

Magnetism-induced band-edge shift as mechanism for magnetoconductance in CrPS$_4$ transistors

Transistors realized on 2D antiferromagnetic semiconductor CrPS$_4$ exhibit large magnetoconductance, due to magnetic-field-induced changes in magnetic state. The microscopic mechanism coupling conductance and magnetic state is not understood. We identify it by analyzing the evolution of the parameters determining the transistor behavior -- carrier mobility and threshold voltage -- with temperature and magnetic field. For temperatures T near the N\'eel temperature $T_N$, the magnetoconductance originates from a mobility increase due to the applied magnetic field that reduces spin fluctuation induced disorder. For $T << T_N$, instead, what changes is the threshold voltage, so that increasing the field at fixed gate voltage increases the density of accumulated electrons. The phenomenon is explained by a conduction band-edge shift correctly predicted by \emph{ab-initio} calculations. Our results demonstrate that the bandstructure of CrPS$_4$ depends on its magnetic state and reveal a mechanism for magnetoconductance that had not been identified earlier.

cond-mat.mes-hall

Full control of solid-state electrolytes for electrostatic gating

Ionic gating is a powerful technique to realize field-effect transistors (FETs) enabling experiments not possible otherwise. So far, ionic gating has relied on the use of top-electrolyte gates, which pose experimental constraints and make device fabrication complex. Promising results obtained recently in FETs based on solid-state electrolytes remain plagued by spurious phenomena of unknown origin, preventing proper transistor operation, and causing limited control and reproducibility. Here we explore a class of solid-state electrolytes for gating (Lithium-ion conducting glass-ceramics, LICGCs), identify the processes responsible for the spurious phenomena and irreproducible behavior,and demonstrate properly functioning transistors exhibiting high density ambipolar operation with gate capacitance of ~20-50 $μ$F/cm$^2$ (depending on the polarity of the accumulated charges). Using two-dimensional semiconducting transition-metal dichalcogenides we demonstrate the ability to implement ionic-gate spectroscopy to determine the semiconducting bandgap, and to accumulate electron densities above 10$^{14}$ cm$^{-2}$, resulting in gate-induced superconductivity in MoS$_2$ multilayers. As LICGCs are implemented in a back-gate configuration, they leave the surface of the material exposed, enabling the use of surface-sensitive techniques (such as scanning tunneling microscopy and photoemission spectroscopy) impossible so far in ionic-liquid gated devices. They also allow double ionic gated devices providing independent control of charge density and electric field.

cond-mat.mtrl-sci

Observation of flat $Γ$ moiré bands in twisted bilayer WSe$_2$

The recent observation of correlated phases in transition metal dichalcogenide moiré systems at integer and fractional filling promises new insight into metal-insulator transitions and the unusual states of matter that can emerge near such transitions. Here, we combine real- and momentum-space mapping techniques to study moiré superlattice effects in 57.4$^{\circ}$ twisted WSe$_2$ (tWSe$_2$). Our data reveal a split-off flat band that derives from the monolayer $Γ$ states. Using advanced data analysis, we directly quantify the moiré potential from our data. We further demonstrate that the global valence band maximum in tWSe$_2$ is close in energy to this flat band but derives from the monolayer K-states which show weaker superlattice effects. These results constrain theoretical models and open the perspective that $Γ$-valley flat bands might be involved in the correlated physics of twisted WSe$_2$.

cond-mat.str-el

Probing magnetism in exfoliated VI$_3$ layers with magnetotransport

We perform magnetotransport experiments on VI$_3$ multilayers, to investigate the relation between ferromagnetism in bulk and in exfoliated layers. The magnetoconductance measured on field-effect transistors and tunnel barriers shows that the Curie temperature of exfoliated multilayers is $T_C$ = 57 K, larger than in bulk ($T_{\rm C,bulk}$ = 50 K). Below $T \approx$ 40 K, we observe an unusual evolution of the tunneling magnetoconductance, analogous to the phenomenology observed in bulk. Comparing the magnetoconductance measured for fields applied in- or out-of-plane corroborates the analogy, allows us to determine that the orientation of the easy-axis in multilayers is similar to that in bulk, and suggests that the in-plane component of the magnetization points in different directions in different layers. Besides establishing that the magnetic state of bulk and multilayers are similar, our experiments illustrate the complementarity of magnetotransport and magneto-optical measurements to probe magnetism in 2D materials.

cond-mat.mes-hall

Light sources with bias tunable spectrum based on van der Waals interface transistors

Light-emitting electronic devices are ubiquitous in key areas of current technology, such as data communications, solid-state lighting, displays, and optical interconnects. Controlling the spectrum of the emitted light electrically, by simply acting on the device bias conditions, is an important goal with potential technological repercussions. However, identifying a material platform enabling broad electrical tuning of the spectrum of electroluminescent devices remains challenging. Here, we propose light-emitting field-effect transistors based on van der Waals interfaces of atomically thin semiconductors as a promising class of devices to achieve this goal. We demonstrate that large spectral changes in room-temperature electroluminescence can be controlled both at the device assembly stage -- by suitably selecting the material forming the interfaces -- and on-chip, by changing the bias to modify the device operation point. Even though the precise relation between device bias and kinetics of the radiative transitions remains to be understood, our experiments show that the physical mechanism responsible for light emission is robust, making these devices compatible with simple large areas device production methods.

cond-mat.mes-hall

Quasi 1D electronic transport in a 2D magnetic semiconductor

We investigate electronic transport through exfoliated multilayers of CrSBr, a 2D semiconductor that is attracting attention because of its magnetic properties. We find an extremely pronounced anisotropy that manifests itself in qualitative and quantitative differences of all quantities measured along the in-plane \textit{a} and \textit{b} crystallographic directions. In particular, we observe a qualitatively different dependence of the conductivities $σ_a$ and $σ_b$ on temperature and gate voltage, accompanied by orders of magnitude differences in their values ($σ_b$/$σ_a \approx 3\cdot10^2-10^5$ at low temperature and large negative gate voltage). We also find a different behavior of the longitudinal magnetoresistance in the two directions, and the complete absence of the Hall effect in transverse resistance measurements. These observations appear not to be compatible with a description in terms of conventional band transport of a 2D doped semiconductor. The observed phenomenology -- together with unambiguous signatures of a 1D van Hove singularity that we detect in energy resolved photocurrent measurements -- indicate that electronic transport through CrSBr multilayers is better interpreted by considering the system as formed by weakly and incoherently coupled 1D wires, than by conventional 2D band transport. We conclude that CrSBr is the first 2D semiconductor to show distinctly quasi 1D electronic transport properties.

cond-mat.mes-hall

Quenching the band gap of 2D semiconductors with a perpendicular electric field

The electronic band structure of atomically thin semiconductors can be tuned by the application of a perpendicular electric field. The principle was demonstrated experimentally shortly after the discovery of graphene by opening a finite band gap in graphene bilayers, which naturally are zero-gap semiconductors. So far, however, the same principle could not be employed to control a broader class of materials, because the required electric fields are beyond reach in current devices. To overcome this limitation, we have realized double ionic gated transistors that enable the application of very large electric fields. Using these devices, we show that the band gap of few-layer semiconducting transition metal dichalcogenides can be continuously suppressed from 1.5 eV to zero. Our results illustrate an unprecedented level of control of the band structures of 2D semiconductors, which is important for future research and applications.

cond-mat.mes-hall

Magnetization dependent tunneling conductance of ferromagnetic barriers

Recent experiments on van der Waals antiferrmagnets such as CrI3, CrCl3 and MnPS3 have shown that using atomically thin layers as tunnel barriers and measuring the temperature ($T$) and magnetic field ($H$) dependence of the conductance allows their magnetic phase diagram to be mapped. In contrast, barriers made of CrBr3 -- the sole van der Waals ferromagnet investigated in this way -- were found to exhibit small and featureless magnetoconductance, seemingly carrying little information about magnetism. Here we show that -- despite these early results -- the conductance of CrBr3 tunnel barriers does provide detailed information about the magnetic state of atomically thin CrBr3 crystals for $T$ both above and below the Curie temperature ($T_C = 32$ K). Our analysis establishes that the tunneling conductance depends on $H$ and $T$ exclusively through the magnetization $M(H,T)$, over the entire temperature range investigated (2-50 K). The phenomenon is reproduced in detail by the spin-dependent Fowler-Nordheim model for tunneling, and is a direct manifestation of the spin splitting of the CrBr3 conduction band. These findings demonstrate that the investigation of magnetism by tunneling conductance measurements is not limited to antiferromagnets, but can also be applied to ferromagnetic materials.

cond-mat.mtrl-sci

Ionic Gate Spectroscopy of 2D Semiconductors

Reliable and precise measurements of the relative energy of band edges in semiconductors are needed to determine band gaps and band offsets, as well as to establish the band diagram of devices and heterostructures. These measurements are particularly important in the field of two-dimensional materials, in which many new semiconducting systems are becoming available through exfoliation of bulk crystals. For two-dimensional semiconductors, however, commonly employed techniques suffer from difficulties rooted either in the physics of these systems, or of technical nature. The very large exciton binding energy, for instance, prevents the band gap to be determined from a simple spectral analysis of photoluminescence, and the limited lateral size of atomically thin crystals makes the use of conventional scanning tunneling spectroscopy cumbersome. Ionic gate spectroscopy is a newly developed technique that exploits ionic gate field-effect transistors to determine quantitatively the relative alignment of band edges of two-dimensional semiconductors in a straightforward way, directly from transport measurements (i.e., from the transistor electrical characteristics). The technique relies on the extremely large geometrical capacitance of ionic gated devices that -- under suitable conditions -- enables a change in gate voltage to be directly related to a shift in chemical potential. Here we present an overview of ionic gate spectroscopy, and illustrate its relevance with applications to different two-dimensional semiconducting transition metal dichalcogenides and van der Waals heterostructures.

cond-mat.mes-hall

Giant anomalous Hall effect in quasi-two-dimensional layered antiferromagnet Co$_{1/3}$NbS$_2$

The discovery of the anomalous Hall effect (AHE) in bulk metallic antiferromagnets (AFMs) motivates the search of the same phenomenon in two-dimensional (2D) systems, where a quantized anomalous Hall conductance can in principle be observed. Here, we present experiments on micro-fabricated devices based on Co$_{1/3}$NbS$_2$, a layered AFM that was recently found to exhibit AHE in bulk crystals below the Néel temperature T$_N$ = 29 K. Transport measurements reveal a pronounced resistivity anisotropy, indicating that upon lowering temperature the electronic coupling between individual atomic layers is increasingly suppressed. The experiments also show an extremely large anomalous Hall conductivity of approximately 400 S/cm, more than one order of magnitude larger than in the bulk, which demonstrates the importance of studying the AHE in small exfoliated crystals, less affected by crystalline defects. Interestingly, the corresponding anomalous Hall conductance, when normalized to the number of contributing atomic planes, is $\sim \, 0.6 \; e^2/h$ per layer, approaching the value expected for the quantized anomalous Hall effect. The observed strong anisotropy of transport and the very large anomalous Hall conductance per layer make the properties of Co$_{1/3}$NbS$_2$ compatible with the presence of partially filled topologically non-trivial 2D bands originating from the magnetic superstructure of the antiferromagnetic state. Isolating atomically thin layers of this material and controlling their charge density may therefore provide a viable route to reveal the occurrence of the quantized AHE in a 2D AFM.

cond-mat.mes-hall

Design of van der Waals Interfaces for Broad-Spectrum Optoelectronics

Van der Waals (vdW) materials offer new ways to assemble artificial electronic media with properties controlled at the design stage, by combining atomically defined layers into interfaces and heterostructures. Their potential for optoelectronics stems from the possibility to tailor the spectral response over a broad range by exploiting interlayer transitions between different compounds with an appropriate band-edge alignment. For the interlayer transitions to be radiative, however, a serious challenge comes from details of the materials --such as lattice mismatch or even a small misalignment of the constituent layers-- that can drastically suppress the electron-photon coupling. The problem was evidenced in recent studies of heterostructures of monolayer transition metal dichalcogenides, whose band edges are located at the K-point of reciprocal space. Here we demonstrate experimentally that the solution to the interlayer coupling problem is to engineer type-II interfaces by assembling atomically thin crystals that have the bottom of the conduction band and the top of the valence band at the $Γ$-point, thus avoiding any momentum mismatch. We find that this type of vdW interfaces exhibits radiative optical transition irrespective of lattice constant, rotational/translational alignment of the two layers, or whether the constituent materials are direct or indirect gap semiconductors. The result, which is robust and of general validity, drastically broadens the scope of future optoelectronics device applications based on 2D materials.

cond-mat.mes-hall

Synthetic Semimetals with van der Waals Interfaces

The assembly of suitably designed van der Waals (vdW) heterostructures represents a new approach to produce artificial systems with engineered electronic properties. Here, we apply this strategy to realize synthetic semimetals based on vdW interfaces formed by two different semiconductors. Guided by existing ab-initio calculations, we select WSe$_2$ and SnSe$_2$ mono and multilayers to assemble vdW interfaces, and demonstrate the occurrence of semimetallicity by means of different transport experiments. Semimetallicity manifests itself in a finite minimum conductance upon sweeping the gate over a large range in ionic liquid gated devices, which also offer spectroscopic capabilities enabling the quantitative determination of the band overlap. The semimetallic state is additionally revealed in Hall effect measurements by the coexistence of electrons and holes, observed by either looking at the evolution of the Hall slope with sweeping the gate voltage or with lowering temperature. Finally, semimetallicity results in the low-temperature metallic conductivity of interfaces of two materials that are themselves insulating. These results demonstrate the possibility to implement a state of matter that had not yet been realized in vdW interfaces, and represent a first step towards using these interfaces to engineer topological or excitonic insulating states.

cond-mat.mes-hall