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Register a new userCoexisting 1T/2H polymorphs, reentrant resistivity behavior, and charge distribution in MoS2-hBN 2D/2D composite thin films
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In view of their immensely intriguing properties, two dimensional materials are being intensely researched in search of novel phenomena and diverse application interests, however, studies on the realization of nanocomposites in the application-worthy thin-film platform are rare. Here we have grown MoS2-hBN composite thin films on different substrates by the pulsed laser deposition technique and made comparative studies with the pristine MoS2 and hBN films. The Raman, XPS and HRTEM confirm the concomitant presence of both the 1T (conducting) and 2H (semiconducting) polymorphs of MoS2 in the composite film. Interestingly, a peculiar reentrant semiconductor-metal-insulator transition is seen in the composite film which is absent in the MoS2 film, and it correlates well with the signatures of phonon softening seen in temperature-dependent Raman spectroscopy. Furthermore, electrostatic force microscopy reveals the presence of three distinct regions (metallic, semiconducting, and insulating) in the composite film with differing contact potentials and enhanced propensity for charge transfer with respect to pristine MoS2. A triboelectric nanogenerator device containing biphasic composite film as an electron acceptor exhibits more than twofold (sixfold) enhancement in peak-to-peak output voltage as compared to the pristine MoS2 (hBN) film. These observations bring out the potential of nanocomposite thin films for unfolding emergent phenomena and technological applications.
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Two-dimensional (2D) superconductivity is a fascinating phenomenon packed with rich physics and wide technological application. The vortices and their dynamics arising from classical and quantum fluctuations give rise to Berezinskii-Kosterlitz-Thouless (BKT) transition and 2D Bose metallic phase both of which are of fundamental interest. In 2D, observation of superconductivity and the associated phenomena are sensitive to material disorders. Highly crystalline and inherently 2D van der Waals (vW) systems with carrier concentration and conductivity approaching metallic regime have been a potential platform. The metallic 1T phase of MoS2, a widely explored vW material system controllably, engineered from the semiconducting 2H phase, is a tangible choice. Here, we report the observation of 2D superconductivity accompanied by BKT transition and Bose metallic state in a few-layer 1T-MoS2. Structural characterization shows excellent crystallinity over extended lateral dimension. The electrical characterization confirms the metallic nature down to 4 K and a transition to a superconducting state below 1.2 K with a Tc ~ 920 mK. The 2D nature of the superconducting state is confirmed from the magneto-transport anisotropy against field orientations and the presence of BKT transition. In addition, our sample showcases a manifold increase in the parallel upper-critical-field above the Pauli limit. The inherent two-dimensionality and possibility of scalably engineering semiconducting, metallic and superconducting phases makes MoS2 a potential candidate for hosting monolithic all-two-dimensional hybrid quantum devices.
The correlation between the transport properties and structural degrees of freedom of conducting polymers is a central concern in both practical applications and scientific research. In this study, we demonstrated the existence of mesoscopic two-dimensional (2D) coherent charge transport in poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) film by performing structural investigations and high-field magnetoconductance (MC) measurements in magnetic fields of up to 15 T. We succeeded in observing marked positive MCs reflecting 2D electronic states in a conventional drop-cast film. This low-dimensional feature is surprising, since PEDOT:PSS-a mixture of two different polymers-seems to be significantly different from crystalline 2D materials in the viewpoint of the structural inhomogeneity, especially in popular drop-cast thick films. The results of the structural experiments suggest that such 2D transport originates from the nanometer-scale self-assembled laminated structure, which is composed of PEDOT nanocrystals wrapped by insulating sheets consisting of amorphous PSSs. These results indicate that charge transport in the PEDOT:PSS film can be divided into two regimes: mesoscopic 2D coherent tunneling and macroscopic three-dimensional hopping among 2D states. Our findings elucidate the hieratical nature of charge transport in the PEDOT:PSS film, which could provide new insight into a recent engineering concern, i.e., the anisotropic conductance.
The magnetic properties of a new family of molecular-based quasi-two dimension $S=1/2$ Heisenberg antiferromagnets are reported. Three compounds, ($Cu(pz)_2(ClO_4)_2$, $Cu(pz)_2(BF_4)_2$, and $[Cu(pz)_2(NO_3)](PF_6)$) contain similar planes of Cu$^{2+}$ ions linked into magnetically square lattices by bridging pyrazine molecules (pz = $C_4H_4N_2$). The anions provide charge balance as well as isolation between the layers. Single crystal measurements of susceptibility and magnetization, as well as muon spin relaxation studies, reveal low ratios of N{e}el temperatures to exchange strengths ($4.25 / 17.5 = 0.243$, $3.80/15.3=0.248$, and $3.05/10.8=0.282$, respectively) while the ratio of the anisotropy fields $H_A$ (kOe) to the saturation field $H_mathrm{SAT}$ (kOe) are small ($2.6/490 = 5.3times10^{-3}$, $2.4/430=5.5times10^{-3}$, and $0.07/300=2.3times10^{-4}$, respectively), demonstrating close approximations to a 2D Heisenberg model. The susceptibilities of ClO$_4$ and BF$_4$ show evidence of an exchange anisotropy crossover (Heisenberg to $XY$) at low temperatures; their ordering transitions are primarily driven by the $XY$ behavior with the ultimate 3D transition appearing parasitically. The PF$_6$ compound remains Heisenberg-like at all temperatures, with its transition to the N{e}el state due to the interlayer interactions. Effects of field-induced anisotropy have been observed.
Segregation at surfaces of metal-covalent binary liquids is often non-classical and in extreme cases such as AuSi, the surface crystallizes above the melting point. In this study, we employ atomic-scale computational frameworks to study the surface crystallization of AuSi films and droplets as a function of composition, temperature and size. For temperatures in the range $T_s^ast=765-780$K above the melting point $(T_s^astapprox1.3,T_m)$, both thin film and droplet surfaces undergo a first order transition, from a 2D Au$_2$Si crystalline phase to a laterally disordered yet stratified layer. The thin film surfaces exhibit an effective surface tension that increases with temperature and decreases with Si concentration. On the other hand, for droplets in the size range $10-30$ nm, the bulk Laplace pressure alters the surface segregation as it occurs with respect to a strained bulk. Above $T_s^ast$ the size effect on the surface tension is small, while for $T<T_s^ast$ the surface layer is strained and composed of 2D crystallites separated by extended grain boundary scars that lead to large fluctuations in its energetics. As a specific application, all-atom simulations of AuSi droplets on Si(111) substrate subject to Si surface flux show that the supersaturation dependent surface tension destabilizes the contact line via formation of a precursor wetting film on the solid-vapor interface, and has ramifications for size selection during VLS-based routes for nanowire growth. Our study sheds light on the interplay between stability and energetics of surfaces in these unique class of binary alloys and offers pathways for exploiting their surface structure for varied applications such as catalytic nanocrystal growth, dealloying, and polymer crystallization.
In the context of photoelectron spectroscopy, the $GW$ approach has developed into the method of choice for computing excitation spectra of weakly correlated bulk systems and their surfaces. To employ the established computational schemes that have been developed for three-dimensional crystals, two-dimensional systems are typically treated in the repeated-slab approach. In this work we critically examine this approach and identify three important aspects for which the treatment of long-range screening in two dimensions differs from the bulk: (1) anisotropy of the macroscopic screening (2) $mathbf k$-point sampling parallel to the surface (3) periodic repetition and slab-slab interaction. For prototypical semiconductor (silicon) and ionic (NaCl) thin films we quantify the individual contributions of points (1) to (3) and develop robust and efficient correction schemes derived from the classic theory of dielectric screening.
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