Sensitive Chiral Analysis via Microwave Three-Wave Mixing

Patterson, David; Doyle, John M.

doi:10.1103/physrevlett.111.023008

Cited by 177 publications

(259 citation statements)

References 15 publications

(26 reference statements)

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“…39 Buffer gas cooled molecules have also been used as a continuous source of cold molecules for cavity-enhanced direct frequency comb spectroscopy 40 and enantiomer-specific detection of chiral molecules via microwave spectroscopy. 41,42 The direct observation of conformational relaxation by collisions with He atoms in a cryogenic environment (∼6 K) has also been reported for the 1,2-propanediol molecule. 43 Other direct techniques such as collisional cooling 44 and rotating nozzle slowing and velocity filtering have been implemented.…”

Section: A Methods For Creation Of Cold and Ultracold Moleculesmentioning

confidence: 99%

Perspective: Ultracold molecules and the dawn of cold controlled chemistry

Balakrishnan

2016

The Journal of Chemical Physics

282

271

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Ultracold molecules offer unprecedented opportunities for the controlled interrogation of molecular events, including chemical reactivity in the ultimate quantum regime. The proliferation of methods to create, cool, and confine them has allowed the investigation of a diverse array of molecular systems and chemical reactions at temperatures where only a single partial wave contributes. Here we present a brief account of recent progress on the experimental and theoretical fronts on cold and ultracold molecules and the opportunities and challenges they provide for a fundamental understanding of bimolecular chemical reaction dynamics. Published by AIP Publishing. [http://dx

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Section: A Methods For Creation Of Cold and Ultracold Moleculesmentioning

confidence: 99%

Perspective: Ultracold molecules and the dawn of cold controlled chemistry

Balakrishnan

2016

The Journal of Chemical Physics

282

271

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“…[95] In mixtures of carvone differences of 20 % ee of the R-species and 33 % ee of the S-species could be distinguished when compared to the racemic mixture. [94] In mixtures of 1,2-propanediol, the racemic mixture could be distinguished from a mixture of 2 % ee of the S-species.…”

Section: Pecd On the Bicyclic Ketonesmentioning

confidence: 97%

“…[94] In mixtures of 1,2-propanediol, the racemic mixture could be distinguished from a mixture of 2 % ee of the S-species. [95] We believe that our ionization method on effusive samples delivers at least a similar sensitivity, where substances having the same mass like camphor and fenchone could be distinguished via different excess energies of the released photoelectrons and substances having the same excess energy but different masses could be distinguished with the help of coincidence techniques. A detailed comparison of the approaches has to wait until both approaches are further developed.…”

Section: Pecd On the Bicyclic Ketonesmentioning

confidence: 99%

Photoelectron Circular Dichroism of Bicyclic Ketones from Multiphoton Ionization with Femtosecond Laser Pulses

et al. 2014

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Photoelectron circular dichroism (PECD) is a CD effect up to the ten-percent regime and shows contributions from higher-order Legendre polynomials when multiphoton ionization is compared to single-photon ionization. We give a full account of our experimental methodology for measuring the multiphoton PECD and derive quantitative measures that we apply on camphor, fenchone and norcamphor. Different modulations and amplitudes of the contributing Legendre polynomials are observed despite the similarity in chemical structure. In addition, we study PECD for elliptically polarized light employing tomographic reconstruction methods. Intensity studies reveal dissociative ionization as the origin of the observed PECD effect, whereas ionization of the intermediate resonance is dominating the signal. As a perspective, we suggest to make use of our tomographic data as an experimental basis for a complete photoionization experiment and give a prospect of PECD as an analytic tool.

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“…This is known as chiral discrimination, and is the subject of much present interest, especially in connection with the detection [23][24][25][26][27][28] and optomechanical (or optofluidic) separation [29][30][31][32][33][34][35][36][37][38][39][40] of enantiomers.…”

Section: Chiral Discrimination In An Electromagnetic Trapmentioning

confidence: 99%

Electromagnetic trapping of chiral molecules: orientational effects of the irradiating beam

Andrews¹

2015

J. Opt. Soc. Am. B

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The photonic interaction generally responsible for the electromagnetic trapping of molecules is forward-Rayleigh scattering, a process that is mediated by transition electric dipoles connecting the ground electronic state and virtual excited states. Higher order electric and magnetic multipole contributions to the scattering amplitude are usually negligible. However, on consideration of chiral discrimination effects (in which an input light of left-handed circular polarization can present different observables compared to right-handed polarization, or molecules of opposite enantiomeric form respond differently to a set circular polarization), the mechanism must be extended to specifically accommodate transition magnetic dipoles. Moreover, it is important to account for the fact that chiral molecules are necessarily nonspherical, so that their interactions with a laser beam will have an orientational dependence. Using quantum electrodynamics, this article quantifies the extent of the energetic discrimination that arises when chiral molecules are optically trapped, placing particular emphasis on the orientational effects of the trapping beam. An in-depth description of the intricate ensemble-weighted method used to incorporate the latter is presented. It is thus shown that, when a mixture of molecular enantiomers is irradiated by a continuous beam of circularly polarized light, a difference arises in the relative rates of migration of each enantiomer in and out of the most intense regions of the beam. As a consequence, optical trapping can be used as a means of achieving enantiomer separation.

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Sensitive Chiral Analysis via Microwave Three-Wave Mixing

Cited by 177 publications

References 15 publications

Perspective: Ultracold molecules and the dawn of cold controlled chemistry

Perspective: Ultracold molecules and the dawn of cold controlled chemistry

Photoelectron Circular Dichroism of Bicyclic Ketones from Multiphoton Ionization with Femtosecond Laser Pulses

Electromagnetic trapping of chiral molecules: orientational effects of the irradiating beam

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