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Register a new userSpin selectivity through chiral polyalanine monolayers on semiconductors
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Tianhan Liu
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Electrical generation of polarized spins in nonmagnetic materials is of great interest for the underlying physics and device potential. One such mechanism is chirality-induced spin selectivity (CISS), with which structural chirality leads to different electric conductivities for electrons of opposite spins. The resulting effect of spin filtering has been reported for a number of chiral molecules. However, the microscopic mechanism and manifestation of CISS in practical device structures remain controversial; in particular, the Onsager relation is understood to preclude linear-response detection of CISS by a ferromagnet. Here, we report direct evidence of CISS in two-terminal devices of chiral molecules on the magnetic semiconductor (Ga,Mn)As: In vertical heterojunctions of (Ga,Mn)As/AHPA-L molecules/Au, we observed characteristic linear- and nonlinear-response magnetoconductance, which directly verifies spin filtering by the AHPA-L molecules and spin detection by the (Ga,Mn)As. The results constitute definitive signature of CISS-induced spin valve effect, a core spintronic functionality, in apparent violation of the Onsager reciprocity. The results present a promising route to semiconductor spintronics free of any magnetic material.
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Chiral induced spin selectivity (CISS) describes efficient spin filtering by chiral molecules. This phenomenon has led to nanoscale manipulation of quantum spins with promising applications to spintronics and quantum computing, since its discovery nearly two decades ago. However, its underlying mechanism still remains mysterious for the required spin-orbit interaction (SOI) strength is unexpectedly large. Here we report a multi-orbital theory for CISS, where an effective SOI emerges from spontaneous formation of electron-hole pairing caused by many-body correlation. This mechanism produces a strong SOI to the order of tens of milielectronvolts which could support the large spin polarization observed in CISS at room temperature. One central ingredient of our theory is the Wannier functions of the valence and conduction bands correspond respectively to one- and two-dimensional representation of the spatial rotation symmetry around the molecule elongation direction. The induced SOI strength is found to decrease when the band gap increases. Our theory may provide important guidance for searching other molecules with CISS effects.
Defect-free monolayers of graphene and hexagonal boron nitride were previously shown to be surprisingly permeable to thermal protons, despite being completely impenetrable to all gases. It remains untested whether small ions can permeate through the two-dimensional crystals. Here we show that mechanically exfoliated graphene and hexagonal boron nitride exhibit perfect Nernst selectivity such that only protons can permeate through, with no detectable flow of counterions. In the experiments, we used suspended monolayers that had few if any atomic-scale defects, as shown by gas permeation tests, and placed them to separate reservoirs filled with hydrochloric acid solutions. Protons accounted for all the electrical current and chloride ions were blocked. This result corroborates the previous conclusion that thermal protons can pierce defect-free two-dimensional crystals. Besides importance for theoretical developments, our results are also of interest for research on various separation technologies based on two-dimensional materials.
Understanding chiral induced spin-selectivity (CISS), resulting from charge transport through helical systems, has recently inspired many experimental and theoretical efforts, but is still object of intense debate. In order to assess the nature of CISS, we propose to focus on electron-transfer processes occurring at the single-molecule level. We design simple magnetic resonance experiments, exploiting a qubit as a highly sensitive and coherent magnetic sensor, to provide clear signatures of the acceptor polarization. Moreover, we show that information could even be obtained from time-resolved electron paramagnetic resonance experiments on a randomly-oriented solution of molecules. The proposed experiments will unveil the role of chiral linkers in electron-transfer and could also be exploited for quantum computing applications.
The strength of the spin-orbit interaction relevant to transport in a low dimensional structure depends critically on the relative geometrical arrangement of current carrying orbitals. Recent tight-binding orbital models for spin transport in DNA-like molecules, have surmised that the band spin-orbit coupling arises from the particular angular relations between orbitals of neighboring bases on the helical chain. Such arrangement could be probed by inducing deformations in the molecule in a conductive probe AFM type setup, as it was recently reported by Kiran, Cohen and Naamancite{Kiran}. Here we report deformation dependent spin selectivity when a double strand DNA model is compressed or stretched. We find that the equilibrium geometry is not optimal with respect to the SO coupling strength and thus spin selectivity can be tuned by deformations. The latter can be increased by stretching the helical structure taking into account its elastic properties through the Poisson ratio. The spin filtering gap is also found to be tunable with uniaxial deformations.
Organic materials are known to feature long spin-diffusion times, originating in a generally small spin-orbit coupling observed in these systems. From that perspective, chiral molecules acting as efficient spin selectors pose a puzzle, that attracted a lot of attention during the recent years. Here we revisit the physical origins of chiral-induced spin selectivity (CISS), and propose a simple analytic minimal model to describe it. The model treats a chiral molecule as an anisotropic wire with molecular dipole moments aligned arbitrarily with respect to the wires axes, and is therefore quite general. Importantly, it shows that helical structure of the molecule is not necessary to observe CISS and other chiral non-helical molecules can also be considered as a potential candidates for CISS effect. We also show that the suggested simple model captures the main characteristics of CISS observed in experiment, without the need for additional constraints employed in the previous studies. The results pave the way for understanding other related physical phenomena where CISS effect plays an essential role.
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