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The energy gap of Bernal-stacked bilayer graphene can be tuned by applying a perpendicular electric field. The origin of this gap can be traced down to the breaking of its inversion symmetry by an onsite potential difference between the layers. This degree of tunability makes bilayer graphene a perfect playground for the study of the effects of electric fields, such as the crystalline field, which are developed when layers of other materials are deposited on top of it. Here, we introduce a novel device architecture allowing a simultaneous control over the applied displacement field and the crystalline alignment between two materials. Our experimental and numerical results confirm that the crystal field and electrostatic doping due to the interface reflect the 120$^{\circ}$ symmetry of the bilayer graphene/BN heterostructure and are highly affected by the commensurate state. These results provide an unique insight into the role of the twist angle in the development of internal crystal fields and intrinsic electrostatic doping in heterostructures. Our results highligth the importance of layer alignment, beyond the existence of a moir\'e superlattice, to understand and simulate the intrinsic properties of a van der Waal heterostructure.

The charge neutrality point of bilayer graphene, denoted as {\nu} = 0 state, manifests competing phases marked by spontaneously broken isospin (spin/valley/layer) symmetries under external magnetic and electric fields. However, due to their electrically insulating nature, identifying these phases through electrical conductance measurements remains challenging. A recent theoretical proposal introduces a novel approach, employing thermal transport measurements to detect these competing phases. Here, we experimentally explore the bulk thermal transport of the {\nu} = 0 state in bilayer graphene to investigate its ground states and collective excitations associated with isospin. While the theory anticipates a finite thermal conductance in the {\nu} = 0 state, our findings unveil an absence of detectable thermal conductance. Through variations in the external electric field and temperature-dependent measurements, our results suggest towards gapped collective excitations at {\nu} = 0 state. Our findings underscore the necessity for further investigations into the nature of {\nu} = 0.

Cryogenic field-effect transistors (FETs) offer great potential for a wide range of applications, the most notable example being classical control electronics for quantum information processors. In the latter context, on-chip FETs with low power consumption are a crucial requirement. This, in turn, requires operating voltages in the millivolt range, which are only achievable in devices with ultra-steep subthreshold slopes. However, in conventional cryogenic metal-oxide-semiconductor (MOS)FETs based on bulk material, the experimentally achieved inverse subthreshold slopes saturate around a few mV/dec due to disorder and charged defects at the MOS interface. FETs based on two-dimensional materials offer a promising alternative. Here, we show that FETs based on Bernal stacked bilayer graphene encapsulated in hexagonal boron nitride and graphite gates exhibit inverse subthreshold slopes of down to 250 ${\mu}$V/dec at 0.1 K, approaching the Boltzmann limit. This result indicates an effective suppression of band tailing in van-der-Waals heterostructures without bulk interfaces, leading to superior device performance at cryogenic temperature., Comment: 22 pages, 18 figures

The optically dark states play an important role in the electronic and optical properties of monolayers (MLs) of semiconducting transition metal dichalcogenides. The effect of temperature on the in-plane-field activation of the neutral and charged dark excitons is investigated in a WSe$_2$ ML encapsulated in hexagonal BN flakes. The brightening rates of the neutral dark (X$^D$) and grey (X$^G$) excitons and the negative dark trion (T$^D$) differ substantially at a particular temperature. More importantly, they vanish considerably by about 3 -- 4 orders of magnitude with the temperature increased from 4.2 K to 100 K. The quenching of the dark-related emissions is accompanied by the two-order-of-magnitude increase in the emissions of their neutral bright counterparts, $i.e.$ neutral bright exciton (X$^B$) and spin-singlet (T$^S$) and spin-triplet (T$^T$) negative trions, due to the thermal activations of dark states. Furthermore, the energy splittings between the dark X$^D$ and T$^D$ complexes and the corresponding bright X$^B$, T$^S$, and T$^T$ ones vary with temperature rises from 4.2 K to 100 K. This can be explained in terms of the different exciton-phonon couplings for the bright and dark excitons stemming from their distinct symmetry properties., Comment: Main text: 6 pages, 4 figures. Supplementary: 5 pages, 4 figures

In transition metal dichalcogenide semiconductor monolayers the spin dynamics of electrons is controlled by the original spin-valley locking effect resulting from the interplay between spin-orbit interaction and inversion asymmetry. As a consequence, for electrons occupying bottom conduction bands, a carrier spin flip occurs only if there is a simultaneous change of valley. However, very little is known about the intra-valley spin relaxation processes. In this work we have performed stationary and time-resolved photoluminescence measurements in high quality WSe$_2$ monolayers. Our experiments highlight an efficient relaxation from bright to dark excitons, due to a fast intra-valley electron transfer from the top to the bottom conduction band with opposite spins. A combination of experiments and theoretical analysis allows us to infer a spin relaxation time of about $\tau_s\sim10~$ps, driven by the interplay between $\Gamma$-valley chiral phonons and spin-orbit mixing., Comment: 10 pages, 4 figures

The optical emission spectra of semiconducting transition-metal dichalcogenide monolayers highlight fascinating recombination processes of charged excitons (trions). When charge tunable WSe2 monolayers are moderately doped with electrons, a strong luminescence peak emerges just below the well-understood spectral lines associated with the recombination of negatively charged bright and dark trions. Despite previous investigations, its origin remains elusive. Here, we demonstrate that this luminescence peak is the result of electron-electron assisted recombination that brightens the dark trion emission. Supporting evidence for this second-order recombination process comes from identifying the equivalent brightened emission of positively charged dark trions when the monolayer is electrostatically doped with holes. Remarkably, the discovered hole-hole assisted luminescence peak emerges in the near infrared, about 500 meV below the well-studied spectral region of excitons and trions. In addition to identifying new recombination channels of these excitonic complexes, our findings accurately determine the spin-split energies of the conduction and valence bands. Both of which play crucial roles in understanding the optical properties of WSe2 based homo- and hetero-structures., Comment: 13 pages, 4 figures

We present a technique for integrating ultraclean carbon nanotubes into superconducting circuits, aiming to realize Josephson junctions based on one-dimensional elementary quantum conductors. This technique primarily involves depositing the nanotube in the final step, thus preserving it from the inherent contaminations of nanofabrication and maintaining contact solely with superconducting electrodes and a crystalline hBN substrate. Through transport measurements performed in both the normal and superconducting states, we demonstrate that our method yields high-quality junctions with Josephson energies suitable for quantum device applications, such as carbon nanotube-based superconducting qubits.

Magic-angle twisted bilayer graphene (MATBG) stands as one of the most versatile materials in condensed-matter physics due to its hosting of a wide variety of exotic phases while also offering convenient tunability. However, the fabrication of MATBG is still manual, and remains to be a challenging and inefficient process, with devices being highly dependent on specific fabrication methods, that often result in inconsistency and variability. In this work, we present an optimized protocol for the fabrication of MATBG samples, for which we use deterministic graphene anchoring to stabilize the twist-angle, and a careful bubble removal techniques to ensure a high twist-angle homogeneity. We use low-temperature transport experiments to extract the average twist-angle between pairs of leads. We find that up to 38 percent of the so fabricated devices show micrometer square sized regions with a twist-angle in the range 1.1 plus/minus 0.1 degrees, and a twist-angle variation of only 0.02 degrees, where in some instances such regions were up to 36 micrometer square large. We are certain that the discussed protocols can be directly transferred to non-graphene materials, and will be useful for the growing field of moire materials.

Graphene provides a unique platform for hosting high quality 2D electron systems. Encapsulating graphene with hexagonal boron nitride (hBN) to shield it from noisy environments offers the potential to achieve ultrahigh performance nanodevices, such as photodiodes and transistors. However, the absence of a bandgap at the Dirac point presents challenges for using this system as a useful transistor. In this study, we investigated the functionality of hBN-aligned monolayer graphene as a field effect transistor (FET). By precisely aligning the hBN and graphene, bandgaps open at the first Dirac point and at the hole-doped induced Dirac point via an interfacial moir\'e potential. To characterize this as a submicrometer scale FET, we fabricated a global bottom gate to tune the density of a conducting channel and a local top gate to switch off this channel. This demonstrated that the system could be tuned to an optimal on/off ratio regime by separately controlling the gates. These findings provide a valuable reference point for the further development of FETs based on graphene heterostructures.

Light incident upon materials can induce changes in their electrical conductivity, a phenomenon referred to as photoresistance. In semiconductors, the photoresistance is negative, as light-induced promotion of electrons across the band gap enhances the number of charge carriers participating in transport. In superconductors, the photoresistance is positive because of the destruction of the superconducting state, whereas in normal metals it is vanishing. Here we report a qualitative deviation from the standard behavior in metallic graphene. We show that Dirac electrons exposed to continuous wave (CW) terahertz (THz) radiation can be thermally decoupled from the lattice by 50~K which activates hydrodynamic electron transport. In this regime, the resistance of graphene constrictions experiences a decrease caused by the THz-driven superballistic flow of correlated electrons. We analyze the dependencies of the negative photoresistance on the carrier density, and the radiation power and show that our superballistic devices operate as sensitive phonon-cooled bolometers and can thus offer a picosecond-scale response time. Beyond their fundamental implications, our findings underscore the practicality of electron hydrodynamics in designing ultra-fast THz sensors and electron thermometers., Comment: 7 pages, 3 figures

Van der Waals heterostructures provide a versatile platform for tailoring electronic properties through the integration of two-dimensional materials. Among these combinations, the interaction between bilayer graphene and transition metal dichalcogenides (TMDs) stands out due to its potential for inducing spin-orbit coupling (SOC) in graphene. Future devices concepts require the understanding the precise nature of SOC in TMD/bilayer graphene heterostructures and its influence on electronic transport phenomena. Here, we experimentally confirm the presence of two distinct types of SOC, Ising (1.55 meV) and Rashba (2.5 meV), in bilayer graphene when interfaced with molybdenum disulphide, recognized as one of the most stable TMDs. Furthermore, we reveal a non-monotonic trend in conductivity with respect to the electric displacement field at charge neutrality. This phenomenon is ascribed to the existence of single-particle gaps induced by the Ising SOC, which can be closed by a critical displacement field. Remarkably, our findings also unveil sharp peaks in the magnetoconductivity around the critical displacement field, challenging existing theoretical models.

Recent experiments on magic-angle twisted bilayer graphene (MATBLG) indicate an unusual coexistence of heavy and light electrons, characteristic of Heavy-Fermion physics. Yet, these experiments lack direct evidence of the existence of local moments associated with the heavy electrons, a key component of Heavy-Fermion physics. Thermopower serves as a sensitive probe for measuring entropy and can, therefore, unveil the presence of local moments by assessing their impact on entropy. In this work, we have carried out comprehensive thermopower studies on MATBLG by varying temperatures ($T$) and magnetic fields ($B$). While the resistance exhibits prominent resistance peaks at integer fillings apart from the Dirac point (DP, $\nu = 0$) and full band filling ($\nu = \pm 4$), the thermopower remains featureless and symmetric to the DP with opposite signs, in complete violation of the Mott formula, even up to $\sim 100K$. This discrepancy indicates that resistance and thermopower are carried by different kinds of carriers. With the expected sign changes at the DP and full band filling, the thermopower demonstrates additional sign changes within the conduction and valence bands around $\nu \sim \pm 1$, persisting from $5K$ to $50K$. These observations cannot be explained solely by thermopower arising from an emergent Heavy-Fermion band picture, which is highly sensitive to temperature. Instead, our data is consistent with the dominant contribution coming from the entropy of the localized moments of heavy electrons. To validate the claim, we studied the thermopower with $B_{\parallel}$ and $B_{\perp}$, revealing a $30\%$ and $50\%$ reduction, respectively, and attributed to the partial polarization of the local moments (spin/valley), resulting in decreased entropy. Our results highlight the thermopower contribution from local moments and establish the Heavy-Fermion physics in MATBLG.

The superconducting (SC) state of magic-angle twisted bilayer graphene (MATBG) shows exceptional properties, as it consists of an unprecedentedly small electron (hole) ensemble of only ~ 10 power 11 carriers per square centimeter, which is five orders of magnitude lower than in traditional superconductors. This results in an ultra-low electronic heat capacity and kinetic inductance of this truly two-dimensional SC, and provides record-breaking key parameters for a variety of quantum sensing applications, in particular in thermal sensing and single photon detection (SPD), which traditionally exploit thermal effects in nanostructured superconducting thin films. In this work, we systematically study the interaction of the superconducting state of MATBG with individual light quanta. We discover full destruction of the SC state upon absorption of a single infrared photon even in a 16 square micrometer sized device, which showcases its exceptional bolometric sensitivity. Upon voltage biasing close to its critical current, we further show that this non-optimized device can be used as a SPD, whose click-rate is proportional to the number of absorbed photons, following Poissonian statistics. Our work offers insights into the MATBG-photon interaction and shows up pathways to use low-carrier density graphene-based superconductors as a new platform for developing revolutionary new quantum devices and sensors.

We report on the observation of the circular ratchet effect excited by terahertz laser radiation in a specially designed two-dimensional metamaterial consisting of a graphene monolayer deposited on a graphite gate patterned with an array of triangular antidots. We show that a periodically driven Dirac fermion system with spatial asymmetry converts the a.c. power into a d.c. current, whose direction reverses when the radiation helicity is switched. The circular ratchet effect is demonstrated for room temperature and a radiation frequency of 2.54 THz. It is shown that the ratchet current magnitude can be controllably tuned by the patterned and uniform back gate voltages. The results are analyzed in the light of the developed microscopic theory considering electronic and plasmonic mechanisms of the ratchet current formation., Comment: 10 pages, 8 figures, 2 tables

Extensive efforts have been undertaken to combine superconductivity and the quantum Hall effect so that Cooper-pair transport between superconducting electrodes in Josephson junctions is mediated by one-dimensional edge states. This interest has been motivated by prospects of finding new physics, including topologically-protected quasiparticles, but also extends into metrology and device applications. So far it has proven challenging to achieve detectable supercurrents through quantum Hall conductors. Here we show that domain walls in minimally twisted bilayer graphene support exceptionally robust proximity superconductivity in the quantum Hall regime, allowing Josephson junctions to operate in fields close to the upper critical field of superconducting electrodes. The critical current is found to be non-oscillatory and practically unchanging over the entire range of quantizing fields, with its value being limited by the quantum conductance of ballistic, strictly one-dimensional electronic channels residing within the domain walls. The system described is unique in its ability to support Andreev bound states at quantizing fields and offers many interesting directions for further exploration., Comment: 24 pages, 14 figures

Superconductivity (SC) in twisted bilayer graphene (tBLG) has been explored by varying carrier concentrations, twist angles, and screening strength, with the aim of uncovering its origin and possible connections to strong electronic correlations in narrow bands and various resulting broken symmetries. However, the link between the tBLG band structure and the onset of SC and other orders largely remains unclear. In this study, we address this crucial gap by examining in-situ band structure tuning of a near magic-angle ($\theta \approx0.95^\circ$) tBLG device with displacement field ($D$) and reveal remarkable competition between SC and other broken symmetries. At zero $D$, the device exhibits superconducting signatures without the resistance peak at half-filling, a characteristic signature with a strong electronic correlation. As $D$ increases, the SC is suppressed, accompanied by the appearance of a resistance peak at half-filling. Hall density measurements reveal that at zero $D$, SC arises around the van Hove singularity (vHs) from an isospin or spin-valley unpolarized band. At higher $D$, the suppression of SC coincides with broken isospin symmetry near half-filling with lifted degeneracy ($g_d \sim 2$). Additionally, as the SC phase becomes weaker with $D$, vHs shifts to higher fillings, highlighting the modification of the underlying band structure with the applied electric field. These findings, with recent theoretical study on SC in tBLG, highlight the competition, rather being connected concomitantly, between SC and other orders promoted by broken symmetries.

We report the observation of the terahertz-induced ratchet effect in graphene-based two-dimensional (2D) metamaterials. The metamaterial consists of a graphite gate patterned with an array of triangular antidots placed under a graphene monolayer. We show that the ratchet current appears due to the noncentrosymmetry of the periodic structure unit cell. The ratchet current is generated owing to the combined action of a spatially periodic in-plane electrostatic potential and a periodically modulated radiation electric field caused by near-field diffraction. The magnitude and direction of the ratchet current are shown to be controlled by voltages applied to both back and patterned gates, which change the lateral asymmetry, carrier type and density. The phenomenological and microscopic theories of ratchet effects in graphene-based 2D metamaterials are developed. The experimental data are discussed in the light of the theory based on the solution of the Boltzmann kinetic equation and the calculated electrostatic potential profile. The theory describes well all the experimental results and shows that the observed ratchet current consists of the Seebeck thermoratchet contribution as well as the linear contribution, which is sensitive to the orientation of the radiation electric field vector with respect to the triangles., Comment: 14 pages, 13 figures

This letter presents a non-local study on the electric field tunable edge transport in an hBN-encapsulated dual-gated Bernal stacked (ABA) trilayer graphene across various displacement fields ($D$) and temperatures ($T$). Our measurements revealed that the non-local resistance ($R_{NL}$) surpassed the expected classical ohmic contribution by a factor of at least two orders of magnitude. Through scaling analysis, we found that the non-local resistance scales linearly with the local resistance ($R_{L}$) only when the $D$ exceeds a critical value of $\sim0.2$ V/nm. Additionally, we observed that the scaling exponent remains constant at unity for temperatures below the bulk-band gap energy threshold ($T<25$ K). Further, the value of $R_{NL}$ decreases in a linear fashion as the channel length ($L$) increases. These experimental findings provide evidence for edge-mediated charge transport in ABA trilayer graphene under the influence of a finite displacement field. Furthermore, our theoretical calculations support these results by demonstrating the emergence of dispersive edge modes within the bulk-band gap energy range when a sufficient displacement field is applied., Comment: Accepted in Physical Review Letters

We report on the mechanism of energy transfer in van der Waals heterostructures of the two-dimensional semiconductor WS$_2$ and graphene with varying interlayer distances, achieved through spacer layers of hexagonal boron nitride (hBN). We record photoluminescence and reflection spectra at interlayer distances between 0.5 nm and 5.8 nm (0-16 hBN layers). We find that the energy transfer is dominated by states outside the light cone, indicative of a F\"orster transfer process, with an additional contribution from a Dexter process at 0.5 nm interlayer distance. We find that the measured dependence of the luminescence intensity on interlayer distances above 1 nm can be quantitatively described using recently reported values of the F\"orster transfer rates of thermalized charge carriers. At smaller interlayer distances, the experimentally observed transfer rates exceed the predictions and furthermore depend on excess energy as well as on excitation density. Since the transfer probability of the F\"orster mechanism depends on the momentum of electron-hole pairs, we conclude that at these distances, the transfer is driven by non-thermalized charge carrier distributions.

Quantum transport properties in molecularly thin perovskite/graphene heterostructure are experimentally investigated by Shubnikov-de Hass (SdH) oscillation and photo-resistance spectroscopy. We find an efficient charge transfer between the perovskite nanosheets and graphene, with a high hole concentration in graphene of up to $\rm \sim 2.8 \times 10^{13}\ cm^{-2}$. The perovskite layer also increases Fermi velocity lowering the effective mass of graphene from expected $\rm \sim 0.12\ m_e$ to $\rm \sim 0.08\ m_e$. Combining magneto-resistance and density functional theory calculations, we find that the carrier density in graphene significantly depends on the perovskite termination at the interface, affecting the charge transfer process and leading to a coexistence of regions with different doping. We also investigate the photo-response of the SdH oscillation under illumination. Using photo-resistance spectroscopy, we find evidence of photo-assisted transport across the perovskite layer between two graphene electrodes mediated by hot carriers in perovskite. Our results provide a picture to understand the transport behavior of 2D perovskite/graphene heterostructure and a reference for the controlled design of interfaces in perovskite optoelectronic devices.

We report intriguing and hitherto overlooked low-field room temperature extremely large magnetoresistance (XMR) patterns in graphene/hexagonal boron nitride (h-BN) superlattices that emerge due to the existence of open orbits within each miniband. This finding is set against the backdrop of the experimental discovery of the Hofstadter butterfly in moir superlattices, which has sparked considerable interest in the fractal quantum Hall regime. To cope with the challenge of deciphering the low magnetic field dynamics of moir minibands, we utilize a novel semi-classical calculation method, grounded in zero-field Fermi contours, to predict the nontrivial behavior of the Landau-level spectrum. This is compared with fully quantum simulations, enabling an in-depth and contrasted analysis of transport measurements in high-quality graphene-hBN superlattices. Our results not only highlight the primary observation of the open-orbit induced XMR in this system but also shed new light on other intricate phenomena. These include the nuances of single miniband dynamics, evident through Lifshitz transitions, and the complex interplay of semiclassical and quantum effects between these minibands. Specifically, we document transport anomalies linked to trigonal warping, a semiclassical deviation from the expected linear characteristics of Landau levels, and magnetic breakdown phenomena indicative of quantum tunneling, all effects jointly contributing to the intricacies of a rich electronic landscape uncovered at low magnetic fields., Comment: 5 figures

We perform infrared magneto-spectroscopy of Landau level (LL) transitions in dual-gated bilayer graphene. At $\nu=4$ when the zeroth LL (octet) is filled, two resonances are observed indicating the opening of a gap. At $\nu=0$ when the octet is half-filled, multiple resonances disperse non-monotonically with increasing displacement field, $D$, perpendicular to the sheet, showing a phase transition at modest displacement fields from a canted anti-ferromagnet (CAFM) to the layer-polarized state, with a gap that opens linearly in $D$. When $D=0$ and $\nu$ is varied, resonances at $\pm\nu$ show an electron-hole asymmetry with multiple line splittings as the octet is progressively filled. The $\nu=4$ data show good agreement with predictions from a mean-field Hartree-Fock calculation when accounting for multiple tight-binding terms in a four-band model of bilayer graphene. However even by incorporating a valley interaction anisotropy tuned to the CAFM ground state, only partial agreement is found at $\nu=0$. Our results suggest additional physics is required to understand bilayer graphene at half-filling.

Twist-controlled moire superlattices (MS) have emerged as a versatile platform in which to realize artificial systems with complex electronic spectra. Bernal-stacked bilayer graphene (BLG) and hexagonal boron nitride (hBN) form an interesting example of the MS that has recently featured a set of unexpected behaviors, such as unconventional ferroelectricity and electronic ratchet effect. Yet, the understanding of the BLG/hBN MS electronic properties has, at present, remained fairly limited. Here we develop a multi-messenger approach that combines standard magnetotransport techniques with low-energy sub-THz excitation to get insights into the properties of this MS. We show that BLG/hBN lattice alignment results in the emergence of compensated semimetals at some integer fillings of the moire bands separated by van Hove singularities where Lifshitz transition occurs. A particularly pronounced semimetal develops when 8 electrons reside in the moire unit cell, where coexisting high-mobility electron and hole systems feature a strong magnetoresistance reaching 2350 % already at B=0.25 T. Next, by measuring the THz-driven Nernst effect in remote bands, we observe valley splitting, pointing to an orbital magnetization characterized by a strongly enhanced effective g-factor of 340. Last, using THz photoresistance measurements, we show that the high-temperature conductivity of the BLG/hBN MS is limited by electron-electron umklapp processes. Our multi-facet analysis introduces THz-driven magnetotransport as a convenient tool to probe the band structure and interaction effects in vdW materials and provides a comprehension of the BLG/hBN MS., Comment: 9 pages, 4 figures

Collective spin-wave excitations-magnons-in a quantum Hall ferromagnet are promising quasi-particles for next-generation spintronics devices, including platforms for information transfer. Detection of these charge-neutral excitations relies on the conversion of magnons into electrical signals in the form of excess electrons and holes, but if these signals are equal the magnon detection remains elusive. In this work, we overcome this shortcoming by measuring the electrical noise generated by magnons. We use the symmetry-broken quantum Hall ferromagnet of the zeroth Landau level in graphene to launch magnons. Absorption of these magnons creates excess noise above the Zeeman energy and remains finite even when the average electrical signal is zero. Moreover, we formulate a theoretical model in which the noise is generated by equilibration (partial or full, depending on the bias voltage) between edge channels and propagating magnons. Our model, which agrees with experimental observations, also allows us to pinpoint the regime of ballistic magnon transport in our device.

Under high electrical current, some materials can emit electromagnetic radiation beyond incandescence. This phenomenon, referred to as electroluminescence, leads to the efficient emission of visible photons and is the basis of domestic lighting devices (e.g., light-emitting diodes). In principle, electroluminescence can lead to mid-infrared (mid-IR) emission of confined light-matter excitations called phonon-polaritons, resulting from the coupling of photons with crystal lattice vibrations (optical phonons). In particular, phonon-polaritons arising in the van der Waals crystal hexagonal boron nitride (hBN) exhibit hyperbolic dispersion, which enhances light-matter coupling. For this reason, electroluminescence of hyperbolic phonon-polaritons (HPhPs) has been proposed as an explanation for the peculiar radiative energy transfer within hBN-encapsulated graphene transistors. However, since HPhPs are confined, they are inaccessible in the far-field, so that any hint of electroluminescence is only based on indirect electronic signatures and needs to be confirmed by direct observation. Here, we demonstrate far-field mid-IR ({\lambda} = 6.5 {\mu}m) electroluminescence of HPhPs excited by strongly biased high-mobility graphene within a van der Waals heterostructure, and we quantify the associated radiative energy transfer through the material. The presence of HPhPs is revealed via far-field mid-IR spectroscopy due to their elastic scattering at discontinuities in the heterostructure. The associated radiative flux is quantified by mid-IR pyrometry of the substrate receiving the energy. This radiative energy transfer is shown to be reduced in hBN with nanoscale inhomogeneities, demonstrating the central role of the electromagnetic environment in this process., Comment: 30 pages including Extended Data and Supplementary Material (Main text: 8 pages, 4 figures)

We have fabricated a 180$^\circ$-twisted bilayer ReSe$_2$ by stacking two centrosymmetric monolayer ReSe$_2$ flakes in opposite directions, which is expected to lose spatial inversion symmetry. By the second harmonic generation and angle-resolved photoemission spectroscopy, we successfully observed spatial inversion symmetry breaking and emergent band dispersions. The band calculation shows the finite lifting of spin degeneracy (~50 meV) distinct from natural monolayer and bilayer ReSe$_2$. Our results demonstrate that the spin-momentum locked state, which leads to spintronic functions and Berry-curvature-related phenomena, can be realized even with the stacking of centrosymmetric monolayers., Comment: 15 pages, 4 figures

Van der Waals (vdW) heterostructures composed of two-dimensional (2D) transition metal dichalcogenides (TMD) and vdW magnetic materials offer an intriguing platform to functionalize valley and excitonic properties in non-magnetic TMDs. Here, we report magneto-photoluminescence (PL) investigations of monolayer (ML) MoSe$_2$ on the layered A-type antiferromagnetic (AFM) semiconductor CrSBr under different magnetic field orientations. Our results reveal a clear influence of the CrSBr magnetic order on the optical properties of MoSe$_2$, such as an anomalous linear-polarization dependence, changes of the exciton/trion energies, a magnetic-field dependence of the PL intensities, and a valley $g$-factor with signatures of an asymmetric magnetic proximity interaction. Furthermore, first principles calculations suggest that MoSe$_2$/CrSBr forms a broken-gap (type-III) band alignment, facilitating charge transfer processes. The work establishes that antiferromagnetic-nonmagnetic interfaces can be used to control the valley and excitonic properties of TMDs, relevant for the development of opto-spintronics devices., Comment: 14 pages, 4 figures

Raman scattering excitation (RSE) is an experimental technique in which the spectrum is made up by sweeping the excitation energy when the detection energy is fixed. We study the low-temperature ($T$=5~K) RSE spectra measured on four high quality monolayers (ML) of semiconducting transition metal dichalcogenides (S-TMDs), $i.e.$ MoS$_2$, MoSe$_2$, WS$_2$, and WSe$_2$, encapsulated in hexagonal BN. The outgoing resonant conditions of Raman scattering reveal an extraordinary intensity enhancement of the phonon modes, which results in extremely rich RSE spectra. The obtained spectra are composed not only of Raman-active peaks, $i.e.$ in-plane E$'$ and out-of-plane A$'_1$, but the appearance of 1$^{st}$, 2$^{nd}$, and higher-order phonon modes is recognised. The intensity profiles of the A$'_1$ modes in the investigated MLs resemble the emissions due to neutral excitons measured in the corresponding PL spectra for the outgoing type of resonant Raman scattering conditions. Furthermore, for the WSe$_2$ ML, the A$'_1$ mode was observed when the incoming light was in resonance with the neutral exciton line. The strength of the exciton-phonon coupling (EPC) in S-TMD MLs strongly depends on the type of their ground excitonic state, $i.e.$ bright or dark, resulting in different shapes of the RSE spectra. Our results demonstrate that RSE spectroscopy is a powerful technique for studying EPC in S-TMD MLs., Comment: 9 pages, 6 figures, ESI

The low-temperature phase diagram of a Bosonic system is predicted to contain an exotic quantum phase, called a supersolid, that is defined by broken translational symmetry and off-diagonal long-range order. This unique combination of properties enables a seemingly paradoxical scenario where a bosonic solid exhibits dissipationless mass flow. However, despite decades of extensive efforts, experimental realization of such a supersolid phase remains elusive. In this work we report experimental observation of a superfluid-to-insulating transition in the bosonic system of spatially indirect excitons in double layer graphene. Utilizing a variety of transport methods to characterize the superfluid-insulator phase boundary as a function of both density and temperature suggests the insulator to be a solid phase driven by repulsive dipole-dipole interactions in the dilute limit. The exciton solid exhibits a unique melting transition, with the high-temperature phase recovering a hallmark transport signature of off-diagonal long-range order, perfect Coulomb drag. The reentrant superfluid-like behaviour could indicate the low temperature solid also corresponds to a quantum coherent phase.

Electroluminescence, a non-thermal radiative process, is ubiquitous in semi-conductors and insulators but fundamentally precluded in metals. We show here that this restriction can be circumvented in high-quality graphene. By investigating the radiative emission of semi-metallic graphene field-effect transistors over a broad spectral range, spanning the near- and mid-infrared, we demonstrate direct far-field electroluminescence from hBN-encapsulated graphene in the mid-infrared under large bias in ambient conditions. Through a series of test experiments ruling out its incandescence origin, we determine that the electroluminescent signal results from the electrical pumping produced by interband tunneling. We show that the mid-infrared electroluminescence is spectrally shaped by a natural quarter-wave resonance of the heterostructure. This work invites a reassessment of the use of metals and semi-metals as non-equilibrium light emitters, and the exploration of their intriguing specificities in terms of carrier injection and relaxation, as well as emission tunability and switching speed., Comment: Main text (8 pages , 3 figures ) + Supplementary Information ( 19 pages , 19 figures)

Defect centers in wide-band-gap crystals attracted considerable attention due to the realisations of qubits, sensors, or single photon emitters at room temperature. The family of these centers is constantly growing, including well-known examples such as nitrogen-vacancy centers in diamond, silicon-vacancy in silicon carbide, chromium substitutions in aluminium oxide, and many others. Unfortunately, such defect centers embedded in highly insulating crystals have been notoriously difficult to excite electrically. Herewith, we present a realisation of insulating light-emitting diodes based on carbon centers in hexagonal boron nitride. The rational design of the vertical tunnelling devices via van der Waals technology enabled us to control the charge dynamics related to non-radiative tunelling, defect-to-band electroluminescence, and intradefect electroluminescence. The fundamental understanding of the tunnelling events enabled us to achieve high efficiency of electrical excitation, which exceeded by a few orders of magnitude the efficiency of optical excitation in the sub-band-gap regime. A combination of a Stark effect and screening by band electrons provide a control knob for tuning the energy of emission. With this work, we solve an outstanding problem of creating electrically driven devices realised with defect centers in wide-band-gap crystals, which are relevant in the domain of optoelectronics, telecommunication, computation, or sensing.

Modulation of the Fermi level using an ultraviolet (UV)-assisted photochemical method is demonstrated in tungsten diselenide monolayers. Systematic shifts and relative intensities between charged and neutral exciton species indicate a progressive and controllable decrease of the electron density and switch tungsten diselenide from n-type to a p-type semiconductor. The presence of chlorine in the 2D crystal shifts the Fermi level closer to the valence band while the effect can be only partially reversible via continuous wave laser rastering process. The presence of chlorine species in the lattice is validated by X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations predict that adsorption of chlorine on the selenium vacancy sites leads to p-type doping. The results of our study indicate that photochemical techniques have the potential to enhance the performance of various 2D materials, making them suitable for potential applications in optoelectronics., Comment: 15 pages, 13 figures

Employing the original, all-optical method, we quantify the magnetic susceptibility of a two-dimensional electron gas (2DEG) confined in the MoSe$_2$ monolayer in the range of low and moderate carrier densities. The impact of electron-electron interactions on the 2DEG magnetic susceptibility is found to be particularly strong in the limit of, studied in detail, low carrier densities. Following the existing models, we derive the value of $g_0 = 2.5 \pm 0.4$ for the bare (in the absence of the interaction effects) $g$-factor of the ground state electronic band in the MoSe$_2$ monolayer. The derived value of this parameter is discussed in the context of estimations from other experimental approaches. Surprisingly, the conclusions drawn differ from theoretical ab-initio studies.

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

We have investigated the exciton fine structure in atomically thin WSe2 -based van der Waals heterostructures where the density of optical modes at the location of the semiconductor monolayer can be tuned. The energy splitting $\Delta$ between the bright and dark exciton has been measured by photoluminescence spectroscopy. We demonstrate that $\Delta$ can be tuned by a few meV, as a result of a significant Lamb shift of the optically active exciton which arises from emission and absorption of virtual photons triggered by the vacuum fluctuations of the electromagnetic field. We also measured strong variations of the bright exciton radiative linewidth, as a result of the Purcell effect. All these experimental results illustrate the strong sensitivity of the excitons to local vacuum field. We found a very good agreement with a model that demonstrates the equivalence, for our system, of a classical electrodynamical transfer matrix formalism and quantum-electrodynamical approach. The bright-dark splitting control demonstrated here should apply to any semiconductor structures.

Semiconducting transition metal dichalcogenides (TMDCs) are very promising materials for quantum dots and spin-qubit implementation. Reliable operation of spin qubits requires the knowledge of Land\'e g-factor, which can be measured by exploiting the discrete energy spectrum on a quantum dot. However, the quantum dots realized in TMDCs has yet to reach the required quality for reliable measurement of g-factor. Quantum dot sizes reported in TMDCs so far are not small enough to observe discrete energy levels on them. Here, we report on electron transport through discrete energy levels of quantum dot in a single layer MoS2. The quantum dot energy levels are separated by few (5-6) meV such that the ground state and the excited state transitions are clearly visible. This well resolved energy separation allows us to accurately measure the ground state g-factor of ~5 in MoS2 quantum dots. We observe a spin filling sequence in our quantum dot under perpendicular magnetic field. Such a system offers an excellent testbed to measure the key parameters for evaluation and implementation of spin-valley qubits in TMDCs, thus accelerating the development of quantum systems in two dimensional semiconducting TMDCs., Comment: 17 pages, 10 figures

Excitons in bilayer transition metal dichalcogenides (2L-TMDs) are Coulomb-bound electron/hole pairs that can be viewed as broadly tunable analogs of atomic or molecular systems. Here, we study the properties of 2L-TMD excitons under strong electric field. To overcome the field limit, reached in previous experiments, we developed a new organic/inorganic molecular gating technique. Our approach allows reaching the field > 0.27 V nm-1, about twice higher than previously available. Under this field inter and intra-layer excitonic are brought into an energetic resonance, allowing us to discover new emergent properties of the resulting hybridized states. First, as the result of hybridization, intralayer excitons acquire an interlayer character. Second, the same hybridization allows us to detect new excitonic species. Third, we observe an ultra-strong Stark splitting of > 380 meV with exciton energies tunable over a large range of the optical spectrum, with potential implications for optoelectronics. Our work creates new possibilities for using strong electric fields to unlock new physical regimes and control exciton hybridization in 2D heterostructures and other systems., Comment: 11 pages, 4 figures

We demonstrate gate-tunable giant field-dependent nonreciprocal transport (magnetochiral anisotropy) in a noncentrosymmetric superconductor $T_{\rm d}$-MoTe$_2$ in the thin limit. Giant magnetochiral anisotropy (MCA) with a rectification coefficient $\gamma$ = $3.1 \times 10^6$ T$^{-1}$ A$^{-1}$, is observed at 230 mK, below the superconducting transition temperature ($T_c$). This is one of the largest values reported so far and is likely attributed to the reduced symmetry of the crystal structure. The temperature dependence of $\gamma$ indicates that the ratchet-like motion of magnetic vortices is the origin of the MCA, as supported by our theoretical model. For bilayer $T_{\rm d}$-MoTe$_2$, we successfully perform gate control of the MCA and realize threefold modulation of $\gamma$. Our experimental results provide a new route to realizing electrically controllable superconducting rectification devices in a single material., Comment: 14 pages, 12 figures

One of the intrinsic drift velocity limit of the quantum Hall effect is the collective magneto-exciton (ME) instability. It has been demonstrated in bilayer graphene (BLG) using noise measurements. We reproduce this experiment in monolayer graphene (MLG), and show that the same mechanism carries a direct relativistic signature on the breakdown velocity. Based on theoretical calculations of MLG- and BLG-ME spectra, we show that Doppler-induced instabilities manifest for a ME phase velocity determined by a universal value of the ME conductivity, set by the Hall conductance., Comment: 27 pages, 11 figures including supplementary information (14 pages and 3 figures for the main text alone)

Low-frequency 1/f noise in electronics is a conductance fluctuation, that has been expressed in terms of a mobility "$\alpha$-noise" by Hooge and Kleinpenning. Understanding this noise in graphene is a key towards high-performance electronics. Early investigations in diffusive graphene have pointed out a deviation from the standard Hooge formula, with a modified expression where the free-carrier density is substituted by a constant density $n_\Delta\sim10^{12}\;\mathrm{cm^{-2}}$. We investigate hBN-encapsulated graphene transistors where high mobility gives rise to the non-linear velocity-saturation regime. In this regime, the $\alpha$-noise is accounted for by substituting conductance by differential conductance $G$, ressulting in a bell-shape dependence of flicker noise with bias voltage $V$. The same analysis holds at larger bias in the Zener regime, with two main differences: the first one is a strong enhancement of the Hooge parameter reflecting the hundred-times larger coupling of interband excitations to the hyperbolic phonon-polariton (HPhP) modes of the mid-infrared Reststrahlen (RS) bands of hBN. The second is an exponential suppression of this coupling at large fields, which we attribute to decoherence effects. We also show that the HPhP bands control the amplitude of flicker noise according to the graphene-hBN thermal coupling estimated with microwave noise thermometry. The phenomenology of $\alpha$-noise in graphene supports a quantum-coherent bremsstrahlung interpretation of flicker noise., Comment: v2, main + SI, added reference to open data on Zenodo repository

Recently, magic-angle twisted bilayer graphene (MATBLG) has shown the emergence of various interaction-driven novel quantum phases at the commensurate fillings of the moir'e superlattice, while the charge neutrality point (CNP) remains mostly a vanilla insulator. Here, we show an emerging phase of nearly compensated semimetallicity at the CNP of twisted double bilayer graphene (TDBLG), a close cousin of MATBLG, with signatures of electronic correlation. Using electrical and thermal transport, we find almost two orders of magnitude enhancement of the thermopower in magnetic fields much smaller than the extreme quantum limit, accompanied by a large magnetoresistance($\sim 2500\%$) at CNP. This provides indisputable experimental evidence that TDBLG near CNP is a compensated semimetal. Moreover, at low temperatures, we observe an unusual sublinear temperature dependence of resistance. A recent theory predicts the formation of an excitonic metal near CNP, where small electron and hole pockets coexist. We understand the sublinear temperature dependence in terms of critical fluctuations in this theory.

New phases of matter can be stabilized by a combination of diverging electronic density of states, strong interactions, and spin-orbit coupling. Recent experiments in magic-angle twisted bilayer graphene (TBG) have uncovered a wealth of novel phases as a result of interaction-driven spin-valley flavour polarization. In this work, we explore correlated phases appearing due to the combined effect of spin-orbit coupling-enhanced valley polarization and large density of states below half filling ($\nu \lesssim 2$) of the moir\'e band in a TBG coupled to tungsten diselenide. We observe anomalous Hall effect, accompanied by a series of Lifshitz transitions, that are highly tunable with carrier density and magnetic field. Strikingly, the magnetization shows an abrupt sign change in the vicinity of half-filling, confirming its orbital nature. The coercive fields reported are about an order of magnitude higher than previous studies in graphene-based moir\'e systems, presumably aided by a Stoner instability favoured by the van Hove singularities in the malleable bands. While the Hall resistance is not quantized at zero magnetic fields, indicative of a ground state with partial valley polarization, perfect quantization and complete valley polarization are observed at finite fields. Our findings illustrate that singularities in the flat bands in the presence of spin-orbit coupling can stabilize ordered phases even at non-integer moir\'e band fillings., Comment: 17 pages, 15 figures

Quantum Hall edge states are the paradigmatic example of the bulk-boundary correspondence. They are prone to intricate reconstructions calling for their detailed investigation at high spatial resolution. Here, we map quantum Hall edge states of monolayer graphene at a magnetic field of 7 T with scanning tunneling microscopy. The graphene sample features a gate-tunable lateral interface between areas of different filling factor. We compare the results with detailed tight-binding calculations quantitatively accounting for the perturbation by the tip-induced quantum dot. We find that the edge state pattern is mapped with little perturbation by adequate choice of gate voltage. We observe extended compressible regions, the antinodal structure of edge states and their meandering along the lateral interface., Comment: 23 pages, 23 figures

The detection of individual quanta of light is important for quantum computation, fluorescence lifetime imaging, single-molecule detection, remote sensing, correlation spectroscopy, and more. Thanks to their broadband operation, high detection efficiency, exceptional signal-to-noise ratio, and fast recovery times, superconducting nanowire single-photon detectors (SNSPDs) have become a critical component in these applications. The operation of SNSPDs based on conventional superconductors, which have a low critical temperature ($T_c$), requires costly and bulky cryocoolers. This motivated exploration of other superconducting materials with higher $T_c$ that would enable single-photon detection at elevated temperatures, yet this task has proven exceedingly difficult. Here we show that with proper processing, high-$T_c$ cuprate superconductors can meet this challenge. We fabricated superconducting nanowires (SNWs) out of thin flakes of Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ and La$_{1.55}$Sr$_{0.45}$CuO$_4$/La$_2$CuO$_4$ (LSCO-LCO) bilayer films and demonstrated their single-photon response up to $25$ and $8$ K, respectively. The single-photon operation is revealed through the linear scaling of the photon count rate (PCR) on the radiation power. Both of our cuprate-based SNSPDs exhibited single-photon sensitivity at the technologically-important $1.5$ ${\mu}$m telecommunications wavelength. Our work expands the family of superconducting materials for SNSPD technology, opens the prospects of raising the temperature ceiling, and raises important questions about the underlying mechanisms of single-photon detection by unconventional superconductors., Comment: 8 pages, 3 figures

Charge-neutral conducting systems represent a class of materials with unusual properties governed by electron-hole (e-h) interactions. Depending on the quasiparticles' statistics, band structure, and device geometry these semimetallic phases of matter can feature unconventional responses to external fields that often defy simple interpretations in terms of single-particle physics. Here we show that small-angle twisted bilayer graphene (SA-TBG) offers a highly-tunable system in which to explore interactions-limited electron conduction. By employing a dual-gated device architecture we tune our devices from a non-degenerate charge-neutral Dirac fluid to a compensated two-component e-h Fermi liquid where spatially separated electrons and holes experience strong mutual friction. This friction is revealed through the T^2 resistivity that accurately follows the e-h drag theory we develop. Our results provide a textbook illustration of a smooth transition between different interaction-limited transport regimes and clarify the conduction mechanisms in charge-neutral SA-TBG., Comment: 11 pages, 4 figures, supplementary information

We report on observation of the infrared photoresistance of twisted bilayer graphene under continuous quantum cascade laser illumination at a frequency of 57.1 THz. The photoresistance shows an intricate sign-alternating behavior under variations of temperature and back gate voltage, and exhibits giant resonance-like enhancements at certain gate voltages. The structure of the photoresponse correlates with weaker features in the dark dc resistance reflecting the complex band structure of twisted bilayer graphene. It is shown that the observed photoresistance is well captured by a bolometric model describing the electron and hole gas heating, which implies an ultrafast thermalization of the photoexcited electron-hole pairs in the whole range of studied temperatures and back gate voltages. We establish that photoresistance can serve a highly sensitive probe of the temperature variations of electronic transport in twisted bilayer graphene., Comment: 8 pages, 10 figures

Strong electric field annihilation by particle-antiparticle pair creation, also known as the Schwinger effect, is a non-perturbative prediction of quantum electrodynamics. Its experimental demonstration remains elusive, as threshold electric fields are extremely strong and beyond current reach. Here, we propose a mesoscopic variant of the Schwinger effect in graphene, which hosts Dirac fermions with an approximate electron-hole symmetry. Using transport measurements, we report on universal 1d-Schwinger conductance at the pinchoff of ballistic graphene transistors. Strong pinchoff electric fields are concentrated within approximately 1 $\mu$m of the transistor's drain, and induce Schwinger electron-hole pair creation at saturation. This effect precedes a collective instability toward an ohmic Zener regime, which is rejected at twice the pinchoff voltage in long devices. These observations advance our understanding of current saturation limits in ballistic graphene and provide a direction for further quantum electrodynamic experiments in the laboratory., Comment: 39 pages, 13 figures, final version with extended discussion of the pinchoff effect in supplementary informations, abstract updated

In two-dimensional (2D) ferromagnets, anisotropy is essential for the magnetic ordering as dictated by the Mermin-Wagner theorem. But when competing anisotropies are present, the phase transition becomes nontrivial. Here, utilizing highly sensitive susceptometry of scanning superconducting quantum interference device microscopy, we probe the spin correlations of ABC-stacked CrBr3 under zero magnetic field. We identify a plateau feature in susceptibility above the critical temperature (Tc) in thick samples. It signifies a crossover regime induced by the competition between easy-plane intralayer exchange anisotropy versus uniaxial interlayer anisotropy. The evolution of the critical behavior from the bulk to 2D shows that the competition between the anisotropies is magnified in the reduced dimension. It leads to a strongly frustrated ferromagnetic transition in the bilayer with fluctuation on the order of Tc, which is distinct from both the monolayer and the bulk. Our observation potentially offers a 2D localized spin system on honeycomb lattice to explore magnetic frustration.

In a strongly correlated system, collective excitations contain key information regarding the electronic order of the underlying ground state. An abundance of collective modes in the spin and valley isospin channels of magic-angle graphene moir\'e bands has been alluded to by a series of recent experiments. However, direct observation of collective excitations has remained elusive due to the lack of a spin probe. In this work, we use a resistively-detected electron spin resonance technique to look for low-energy collective excitations in magic-angle twisted bilayer graphene. We report direct observation of collective modes in the form of microwave-induced resonance near half filling of the moir\'e flatbands. The frequency-magnetic field dependence of these resonance modes sheds light onto the nature of intervalley spin coupling, allowing us to extract parameters such as intervalley exchange interaction and spin stiffness. Two independent observations testify that the generation and detection of the microwave resonance relies on the strong correlation within the flat moir\'e energy band. First, the onset of robust resonance response coincides with the spontaneous flavor polarization at half moir\'e filling, and remains absent in the density range where the underlying Fermi surface is isospin unpolarized. Second, we performed the same resonance measurement on graphene monolayer and bilayer samples, including twisted bilayer with a large twist angle, where flatband physics is absent. We observe no indication of resonance response in these samples across a large range of carrier density, microwave frequency and power. A natural explanation is that the resonance response near the magic angle originates from "Dirac revivals" and the resulting isospin order., Comment: 9 pages, 4 figures and supplementary information; updated discussion and data from 4 additional samples

Van der Waals heterostructures comprised of two-dimensional (2D) materials offer a platform to obtain materials by design with unique electronic properties. Franckeite (Fr) is a naturally occurring van der Waals heterostructure comprised of two distinct alternately stacked semiconducting layers; (i) SnS$_2$ layer and (ii) Pb$_3$SbS$_4$. Though both layers in the heterostructure are semiconductors, the photoluminescence from Franckeite remains elusive. Here, we report the observation of photoluminescence (PL) from Franckeite for the first time. We observed two PL peaks at ~ 1.93 eV and ~ 2.11 eV. By varying the temperature from 1.5 K to 80 K, we found that the PL peak position redshifts and the integrated intensity decreases slowly as we increase the temperature. We observed linear dependence of photoluminescence integrated intensity on excitation laser power indicating that the photoluminescence is originating from free excitons in the SnS$_2$ layer of Fr. By comparing the PL from Fr with the PL from a monolayer MoS$_2$, we determined that the PL quantum efficiency from Fr is an order of magnitude lower than that of a monolayer MoS$_2$. Our study provides a fundamental understanding of the optical behavior in a complex naturally occurring van der Waals heterostructure, and may pave an avenue toward developing nanoscale optical and optoelectronic devices with tailored properties., Comment: 8 pages, 5 Figures, Accepted to Applied Physics Letter