Chiral Selective Chemistry Induced by Natural Selection of Spin‐Polarized Electrons

Rosenberg, R. A.; Mishra, Debabrata; Naaman, Ron

doi:10.1002/anie.201501678

Cited by 60 publications

(50 citation statements)

References 29 publications

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“…This finding supports the proposed model that relates the enantiorecognition mechanism to an exchange energy term that is influenced by the spin polarization in chiral molecules. This observation is also consistent with previous studies that found a relation between spin‐selective electron interaction with molecules and the electron‐induced dissociation in those molecules …”

Section: Figuresupporting

confidence: 93%

Magnetless Device for Conducting Three‐Dimensional Spin‐Specific Electrochemistry

et al. 2017

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Electron spin states play an important role in many chemical processes. Most spin-state studies require the application of a magnetic field. Recently it was found that the transport of electrons through chiral molecules also depends on their spin states and may also play a role in enantiorecognition. Electrochemistry is an important tool for studying spin-specific processes and enantioseparation of chiral molecules. A new device is presented, which serves as the working electrode in electrochemical cells and is capable of providing information on the correlation of spin selectivity and the electrochemical process. The device is based on the Hall effect and it eliminates the need to apply an external magnetic field. Spin-selective electron transfer through chiral molecules can be monitored and the relationship between the enantiorecognition process and the spin of electrons elucidated.

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Section: Figuresupporting

confidence: 93%

Magnetless Device for Conducting Three‐Dimensional Spin‐Specific Electrochemistry

et al. 2017

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“…In recent experiments, it was demonstrated that electrons that pass through a layer of dsDNA, and their spin was therefore polarized, induce chiral-selective chemistry. 27 …”

Section: Introductionmentioning

confidence: 99%

Spin-Dependent Transport through Chiral Molecules Studied by Spin-Dependent Electrochemistry

et al. 2016

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ConspectusMolecular spintronics (spin + electronics), which aims to exploit both the spin degree of freedom and the electron charge in molecular devices, has recently received massive attention. Our recent experiments on molecular spintronics employ chiral molecules which have the unexpected property of acting as spin filters, by way of an effect we call “chiral-induced spin selectivity” (CISS). In this Account, we discuss new types of spin-dependent electrochemistry measurements and their use to probe the spin-dependent charge transport properties of nonmagnetic chiral conductive polymers and biomolecules, such as oligopeptides, L/D cysteine, cytochrome c, bacteriorhodopsin (bR), and oligopeptide-CdSe nanoparticles (NPs) hybrid structures. Spin-dependent electrochemical measurements were carried out by employing ferromagnetic electrodes modified with chiral molecules used as the working electrode. Redox probes were used either in solution or when directly attached to the ferromagnetic electrodes. During the electrochemical measurements, the ferromagnetic electrode was magnetized either with its magnetic moment pointing “UP” or “DOWN” using a permanent magnet (H = 0.5 T), placed underneath the chemically modified ferromagnetic electrodes. The spin polarization of the current was found to be in the range of 5–30%, even in the case of small chiral molecules. Chiral films of the l- and d-cysteine tethered with a redox-active dye, toludin blue O, show spin polarizarion that depends on the chirality. Because the nickel electrodes are susceptible to corrosion, we explored the effect of coating them with a thin gold overlayer. The effect of the gold layer on the spin polarization of the electrons ejected from the electrode was investigated. In addition, the role of the structure of the protein on the spin selective transport was also studied as a function of bias voltage and the effect of protein denaturation was revealed. In addition to “dark” measurements, we also describe photoelectrochemical measurements in which light is used to affect the spin selective electron transport through the chiral molecules. We describe how the excitation of a chromophore (such as CdSe nanoparticles), which is attached to a chiral working electrode, can flip the preferred spin orientation of the photocurrent, when measured under the identical conditions. Thus, chirality-induced spin polarization, when combined with light and magnetic field effects, opens new avenues for the study of the spin transport properties of chiral molecules and biomolecules and for creating new types of spintronic devices in which light and molecular chirality provide new functions and properties.

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“…These secondary electrons then react with adsorbed Epi and the reaction kinetics were determined by the following changes in the Cl 2p XPS spectra in a similar fashion to Section 3.1 and quantum yields (QYs) were determined. When the two enantiomers were adsorbed on bare Au, the QYs were the same, but when adsorbed on the dsDNA layer the QY for S-Epi was~16% greater than for R-Epi [45].…”

Section: Chiral-specific Reactions Caused By Natural Selection Of Spimentioning

confidence: 92%

“…A schematic diagram showing how the Au secondary electrons produced by X-ray irradiation become spin polarized, with their spins aligned antiparallel to their velocity, and induce chiral selective chemistry in adsorbed (R)-or (S)-epichlorohdydrin. This figure was originally published in Ref [45]…”

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confidence: 99%

Electrochirogenesis: The Possible Role of Low-Energy Spin-Polarized Electrons in Creating Homochirality

Rosenberg

2019

Symmetry

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Electrochirogenesis deals with the induction of chirality by polarized electrons of which those with low energy (<15 eV) are seen to be the most effective. Possible sources of such electrons in the prebiotic universe are discussed and several examples where chiral induction by these electrons have been demonstrated are given. Finally, some possible scenarios where electrochirogenesis could have played a role in forming a chiral imbalance in a prebiotic setting have been speculated on and some possible future areas of research proposed.

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Chiral Selective Chemistry Induced by Natural Selection of Spin‐Polarized Electrons

Cited by 60 publications

References 29 publications

Magnetless Device for Conducting Three‐Dimensional Spin‐Specific Electrochemistry

Magnetless Device for Conducting Three‐Dimensional Spin‐Specific Electrochemistry

Spin-Dependent Transport through Chiral Molecules Studied by Spin-Dependent Electrochemistry

Electrochirogenesis: The Possible Role of Low-Energy Spin-Polarized Electrons in Creating Homochirality

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