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Register a new userAssessing the nature of chiral-induced spin-selectivity by magnetic resonance
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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.
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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.
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.
A new method for detecting the magnetic resonance of electronic spins at low temperature is demonstrated. It consists in measuring the signal emitted by the spins with a superconducting qubit that acts as a single-microwave-photon detector, resulting in an enhanced sensitivity. We implement this new type of electron-spin resonance spectroscopy using a hybrid quantum circuit in which a transmon qubit is coupled to a spin ensemble consisting of NV centers in diamond. With this setup we measure the NV center absorption spectrum at 30mK at an excitation level of thicksim15,mu_{B} out of an ensemble of 10^{11} spins.
The theoretical explanation for the chiral-induced spin selectivity effect, in which electrons passage through a chiral system depends on their spin and the handedness of the system, remains vague. Although most experimental work was performed at room temperature, most of the proposed theories did not include vibrations. Here, we present temperature-dependent experiments and a theoretical model that captures all observations and provides spin polarization values that are consistent with the experimental results. The model includes vibrational contribution to the spin orbit coupling. It shows the importance of dissipation and the relation between the effect and the optical activity.
Magnetic resonance with ensembles of electron spins is nowadays performed in frequency ranges up to 240 GHz and in corresponding magnetic fields of up to 10 T. However, experiments with single electron and nuclear spins so far only reach into frequency ranges of several 10 GHz, where existing coplanar waveguide structures for microwave (MW) delivery are compatible with single spin readout techniques (e.g. electrical or optical readout). Here, we explore the frequency range up to 90 GHz, respectively magnetic fields of up to $approx 3,$T for single spin magnetic resonance in conjunction with optical spin readout. To this end, we develop MW resonators with optical single spin access. In our case, rectangular E-band waveguides guarantee low-loss supply of microwaves to the resonators. Three dimensional cavities, as well as coplanar waveguide resonators enhance MW fields by spatial and spectral confinement with a MW efficiency of $1.36,mathrm{mT/sqrt{W}}$. We utilize single NV centers as hosts for optically accessible spins, and show, that their properties regarding optical spin readout known from smaller fields (<0.65 T) are retained up to fields of 3 T. In addition, we demonstrate coherent control of single nuclear spins under these conditions. Furthermore, our results extend the applicable magnetic field range of a single spin magnetic field sensor. Regarding spin based quantum registers, high fields lead to a purer product basis of electron and nuclear spins, which promises improved spin lifetimes. For example, during continuous single-shot readout the $^{14}$N nuclear spin shows second-long longitudinal relaxation times.
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