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Register a new userSpin-dependent Tunneling Barriers in CoPc/VSe2 from Many-Body Interactions
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Mixed-dimensional magnetic heterostructures are intriguing, newly available platforms to explore quantum physics and its applications. Using state-of-the-art many-body perturbation theory, we predict the energy level alignment for a self-assembled monolayer of cobalt phthalocyanine (CoPc) molecules on magnetic VSe 2 monolayers. The predicted projected density of states on CoPc agrees with experimental scanning tunneling spectra. Consistent with experiment, we predict a shoulder in the unoccupied region of the spectra that is absent from mean-field calculations. Unlike the nearly spin-degenerate gas phase frontier molecular orbitals, the tunneling barriers at the interface are spin-dependent, a finding of interest for quantum information and spintronics applications. Both the experimentally observed shoulder and the predicted spin-dependent tunneling barriers originate from many-body interactions in the interface-hybridized states. Our results showcase the intricate many-body physics that governs the properties of these mixed-dimensional magnetic heterostructures, and suggests the possibility of manipulating the spin-dependent tunneling barriers through modifications of interface coupling.
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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.
Currents across thin insulators are commonly taken as single electrons moving across classically forbidden regions; this independent particle picture is well-known to describe most tunneling phenomena. Examining quantum transport from a different perspective, i.e., by explicit treatment of electron-electron interactions, we evaluate different single particle approximations with specific application to tunneling in metal-molecule-metal junctions. We find maximizing the overlap of a Slater determinant composed of single particle states to the many-body current-carrying state is more important than energy minimization for defining single particle approximations in a system with open boundary conditions. Thus the most suitable single particle effective potential is not one commonly in use by electronic structure methods, such as the Hartree-Fock or Kohn-Sham approximations.
Many-body interactions in monolayer transition-metal dichalcogenides are strongly affected by their unique band structure. We study these interactions by measuring the energy shift of neutral excitons (bound electron-hole pairs) in gated WSe$_2$ and MoSe$_2$. Surprisingly, while the blueshift of the neutral exciton, $X^0$, in electron-doped samples can be more than 10~meV, the blueshift in hole-doped samples is nearly absent. Taking into account dynamical screening and local-field effects, we present a transparent and analytical model that elucidates the crucial role played by intervalley plasmons in electron-doped conditions. The energy shift of $X^0$ as a function of charge density is computed showing agreement with experiment, where the renormalization of $X^0$ by intervalley plasmons yields a stronger blueshift in MoSe$_2$ than in WSe$_2$ due to differences in their band ordering.
We report on the use of the LaAlO3 (LAO) high-k dielectric as a tunnel barrier in magnetic tunnel junctions. From tunnel magnetoresistance (TMR) measurements on epitaxial La2/3Sr1/3MnO3/LAO/La2/3Sr1/3MnO3 junctions, we estimate a spin polarization of 77% at low temperature for the La2/3Sr1/3MnO3/LAO interface. Remarkably, the TMR of La2/3Sr1/3MnO3/LAO/Co junctions at low bias is negative, evidencing a negative spin polarization of Co at the interface with LAO, and its bias dependence is very similar to that of La2/3Sr1/3MnO3/STO/Co junctions. We discuss possible reasons for this behaviour.
We design dipolar quantum many-body Hamiltonians that will facilitate the realization of exotic quantum phases under current experimental conditions achieved for polar molecules. The main idea is to modulate both single-body potential barriers and two-body dipolar interactions on a spatial scale of tens of nanometers to strongly enhance energy scales and, therefore, relax temperature requirements for observing new quantum phases of engineered many-body systems. We consider and compare two approaches. In the first, nanoscale barriers are generated with standing wave optical light fields exploiting optical nonlinearities. In the second, static electric field gradients in combination with microwave dressing are used to write nanostructured spatial patterns on the induced electric dipole moments, and thus dipolar interactions. We study the formation of inter-layer and interface bound states of molecules in these configurations, and provide detailed estimates for binding energies and expected losses for present experimental setups.
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