scholarly journals Enantioselective fragmentation of an achiral molecule in a strong laser field

2019 ◽  
Vol 5 (3) ◽  
pp. eaau7923 ◽  
Author(s):  
K. Fehre ◽  
S. Eckart ◽  
M. Kunitski ◽  
M. Pitzer ◽  
S. Zeller ◽  
...  

Chirality is omnipresent in living nature. On the single molecule level, the response of a chiral species to a chiral probe depends on their respective handedness. A prominent example is the difference in the interaction of a chiral molecule with left or right circularly polarized light. In the present study, we show by Coulomb explosion imaging that circularly polarized light can also induce a chiral fragmentation of a planar and thus achiral molecule. The observed enantiomer strongly depends on the orientation of the molecule with respect to the light propagation direction and the helicity of the ionizing light. This finding might trigger new approaches to improve laser-driven enantioselective chemical synthesis.

The differential scattering of right and left circularly polarized light is a manifestation of optical activity. Both naturally optically active systems and fluids in a magnetic field parallel to the direction of propagation exhibit differential scattering. Although there is no electric analogue of Faraday’s effect, a static electric field applied to a fluid perpendicular to the direction of propagation induces a difference in the scattered intensities of right and left circularly polarized light. The difference is linear in the field strength. It is determined by the effect of the field on the polarizabilities producing optical activity and is present in all matter, including monatomic gases. The classical theory of the scattering of electromagnetic waves is used in a formulation of the general theory of light scattering in an electric field. Results are given for some particular symmetries, including spherical, tetrahedral and dipolar molecules, and estimates of the magnitude of the effect are made.


Nanophotonics ◽  
2019 ◽  
Vol 8 (5) ◽  
pp. 909-920 ◽  
Author(s):  
Ranran Zhang ◽  
Qiuling Zhao ◽  
Xia Wang ◽  
Wensheng Gao ◽  
Jensen Li ◽  
...  

AbstractThe ability of chiral media to differentiate circularly polarized light is conventionally characterized by circular dichroism (CD) which is based on the difference in the absorption of the incident light for different polarizations. Thus, CD probes the bulk properties of chiral media. Here, we introduce a new approach termed as circular phase-dichroism that is based on the surface properties and is defined as the difference of the reflection phase for different circularly polarized incident lights in characterizing chiral media. As a demonstration, we measure the reflection phase from planar chiral sawtooth metasurface for circularly polarized light in the visible range using a simple Fabry Perot interference technique. The measured circular phase-dichroism is also crosschecked by conventional CD measurement of the transmitted light and by full-wave simulations. Our results demonstrate the potential applications of circular phase-dichroism in sensing and metasurface characterizations.


1968 ◽  
Vol 46 (4) ◽  
pp. 599-604 ◽  
Author(s):  
D. A. Hutchinson

sRosenfeld's formula, for off-resonance optical rotation, is derived by an alternative approach. The scattering amplitudes are determined for the scattering of right circularly polarized light and left circularly polarized light by a molecule. The calculation is carried out to the order of approximation which includes electric quadrupole and magnetic dipole terms. From the real parts of the forward scattering amplitudes the corresponding indices of refraction are determined for left and right circularly polarized light. Rosenfeld's formula then follows from the difference between the two refractive indices.


Author(s):  
Marcos F. Maestre

Recently we have developed a form of polarization microscopy that forms images using optical properties that have previously been limited to macroscopic samples. This has given us a new window into the distribution of structure on a microscopic scale. We have coined the name differential polarization microscopy to identify the images obtained that are due to certain polarization dependent effects. Differential polarization microscopy has its origins in various spectroscopic techniques that have been used to study longer range structures in solution as well as solids. The differential scattering of circularly polarized light has been shown to be dependent on the long range chiral order, both theoretically and experimentally. The same theoretical approach was used to show that images due to differential scattering of circularly polarized light will give images dependent on chiral structures. With large helices (greater than the wavelength of light) the pitch and radius of the helix could be measured directly from these images.


2021 ◽  
Author(s):  
Zhaoming Zhang ◽  
Takunori Harada ◽  
Adriana Pietropaolo ◽  
Yuting Wang ◽  
Yue Wang ◽  
...  

Preferred-handed propeller conformation was induced by circularly polarized light irradiation to three amorphous molecules with trigonal symmetry, and the molecules with induced chirality efficiently exhibited blue circularly polarized luminescence. In...


2021 ◽  
Vol 11 (8) ◽  
pp. 3317
Author(s):  
C.S. Quintans ◽  
Denis Andrienko ◽  
Katrin F. Domke ◽  
Daniel Aravena ◽  
Sangho Koo ◽  
...  

External electric fields (EEFs) have proven to be very efficient in catalysing chemical reactions, even those inaccessible via wet-chemical synthesis. At the single-molecule level, oriented EEFs have been successfully used to promote in situ single-molecule reactions in the absence of chemical catalysts. Here, we elucidate the effect of an EEFs on the structure and conductance of a molecular junction. Employing scanning tunnelling microscopy break junction (STM-BJ) experiments, we form and electrically characterize single-molecule junctions of two tetramethyl carotene isomers. Two discrete conductance signatures show up more prominently at low and high applied voltages which are univocally ascribed to the trans and cis isomers of the carotenoid, respectively. The difference in conductance between both cis-/trans- isomers is in concordance with previous predictions considering π-quantum interference due to the presence of a single gauche defect in the trans isomer. Electronic structure calculations suggest that the electric field polarizes the molecule and mixes the excited states. The mixed states have a (spectroscopically) allowed transition and, therefore, can both promote the cis-isomerization of the molecule and participate in electron transport. Our work opens new routes for the in situ control of isomerisation reactions in single-molecule contacts.


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