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Nonlinear Optics || Molecular Origin of the Nonlinear Optical Response
摘要： In Chapter 3, we presented a general quantum-mechanical theory of the nonlinear optical susceptibility. This calculation was based on time-dependent perturbation theory and led to explicit predictions for the complete frequency dependence of the linear and nonlinear optical susceptibilities. Unfortunately, however, these quantum-mechanical expressions are typically far too complicated to be of use for practical calculations. In this chapter we review some of the simpler approaches that have been implemented to develop an understanding of the nonlinear optical characteristics of various materials. Many of these approaches are based on understanding the optical properties at the molecular level. We also present brief descriptions of the nonlinear optical characteristics of conjugated polymers, chiral molecules, and liquid crystals.
关键词： chiral molecules,nonlinear optical susceptibility,liquid crystals,quantum-mechanical theory,conjugated polymers,time-dependent perturbation theory
更新于2025-09-23 15:21:01
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Asymmetric photoelectron emission from chiral molecules using a high repetition rate laser
摘要： In the chiro-optical phenomenon known as photoelectron circular dichroism, the angular distribution of electrons ionized from chiral molecules by circularly polarized light pulses has been found to be anti-symmetric with respect to the direction of the light propagation. To study this phenomenon, chiral molecules were multiphoton ionized with a femtosecond laser in our laboratory. Using a simple stereo-detection setup, direct measurements of the asymmetry for the exemplar aromatic chiral molecule 1-phenylethanol were made using 260 nm pulses produced at a rate of 1 MHz. It was found that the asymmetry had a linear dependence on Stokes’ S3 parameter indicating that the photoelectron circular dichroism is due to a single photon process from the excited state of the molecule. This is in contrast to previous and new results for camphor where a more complex dependence on S3 suggested that selective excitation of molecules with certain orientations was influential.
关键词： photoelectron circular dichroism,circularly polarized light,asymmetry,Stokes’ S3 parameter,chiral molecules
更新于2025-09-23 15:19:57
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Metamaterials and chiral sensing: a review of fundamentals and applications
摘要： Chirality, a property of broken mirror symmetry, prevails in nature. Chiral molecules show different biochemical behaviors to their mirror molecules. For left or right circularly polarized lights, the fundamental chiral states of electromagnetic fields interact differently with chiral matter, and this effect has been used as a powerful tool for the detection of chiral molecules. This optical sensing, also termed chiral sensing, is not only easy to implement but also non-invasive to the analytes. However, the measurements made by the optical sensing of chiral molecules are challenging, as chiroptical signals are extremely weak. Recent years have seen active research efforts into metamaterial and plasmonic platforms for manipulating local fields to enhance chiroptical signals. This metamaterial approach offers new possibilities of chiral sensing with high sensitivity. Here, we review the recent advances in chiral sensing using metamaterial and plasmonic platforms. In addition, we explain the underlying principles behind the enhancement of chiroptical signals and highlight practically efficient chiral sensing platforms. We also provide perspectives that shed light on design considerations for chiral sensing metamaterials and discuss the possibility of other types of chiral sensing based on resonant metamaterials.
关键词： chiral sensing,chiral molecules,optical rotatory dispersion (ORD),chiroptical spectroscopy,circular dichroism (CD),enantiomers,plasmonics,metamaterials,optical spectroscopy
更新于2025-09-19 17:15:36
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[IEEE 2019 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) - Munich, Germany (2019.6.23-2019.6.27)] 2019 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) - Photoelectron Circular Dichroism at the Few-Cycle Limit in the Tunnel Ionization Regime
摘要： Photoelectron circular dichroism (PECD) is a process that leads to a forward-backward asymmetry (with respect to the laser propagation direction) in photoelectron distributions created upon interaction of a circularly or elliptically polarized laser with a chiral molecule. The PECD effect has been shown in a broad range of ionization mechanisms from direct photoionization through multi-photon regime, above-threshold ionization to the tunnel ionization [1]. The fact that the effects of chirality can be observed in the tunnel ionization regime opens up the possibility to connect this fundamental effect to strong-field science with prospects for studying and driving sub-laser-cycle and attosecond phenomena connected to PECD [2]. However, a thorough understanding of PECD in the tunneling regime is of yet missing. In this study the effect of trajectory related parameters like electron energy or CEP on the PECD is investigated in order to determine the role of the scattering on the chiral potential.
关键词： few-cycle laser pulses,tunnel ionization,Photoelectron circular dichroism,chiral molecules
更新于2025-09-12 10:27:22
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DNA Enabled Chiral Gold Nanoparticle - Chromophore Hybrid Structure with Resonant Plasmon – Exciton Coupling Gives Unusual and Strong Circular Dichroism
摘要： Circular dichroism (CD) from hybrid complexes of plasmonic nanostructures and chiral molecules has recently attracted significant interest. However, the hierarchical chiral self-assembly of molecules on surfaces of metal nanostructures has remained challenging. As a result, a deep understanding of plasmon-exciton coupling between surface plasmons and chiral collective molecular excitations has not been achieved. In particular, the critical impact of resonant plasmon-exciton coupling within the hybrid is unclear. Here, we employed DNA-templated strategies to control the chiral self-assembly of achiral chromophores with rationally tuned exciton transitions on gold nanosphere (AuNP) or gold nanorod (AuNR) surfaces. Unlike many previous chiral plasmonic hybrids utilizing chiral biomolecules with CD signals in the UV range, we designed structure with the chiral excitonic resonances at visible wavelengths. The constructed hybrid complexes displayed strong chiroptical activity that depends on the spectral overlap between the chiral collective molecular excitations and the plasmon resonances. We find that when spectral overlap is optimized, the molecular CD signal originating from the chiral self-assemblies of chromophores was strongly enhanced (maximum enhancement of nearly an order of magnitude) and a plasmonic CD signal was induced. Surprisingly, the sign of the molecular CD was reversed despite different self-assembly mechanisms of the Au nanoparticle-chromophore hybrids. Our results provide new insight into plasmonic CD enhancements and will inspire further studies on chiral light-matter interactions in strongly coupled plasmonic-excitonic systems.
关键词： DNA-templated strategies,gold nanorod,chiral molecules,chiroptical activity,gold nanosphere,Circular dichroism,plasmonic nanostructures
更新于2025-09-12 10:27:22
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Laser-induced persistent orientation of chiral molecules
摘要： We study, both classically and quantum mechanically, enantioselective orientation of gas-phase chiral molecules excited by laser fields with twisted polarization. Counterintuitively, the induced orientation, whose direction is laser controllable, does not disappear after the excitation but stays long after the end of the laser pulses. We computationally demonstrate this long-lasting orientation, using propylene oxide molecules (CH3CHCH2O, or PPO) as an example, and consider two kinds of fields with twisted polarization: a pair of delayed cross-polarized pulses and an optical centrifuge. This chiral effect opens avenues for detecting molecular chirality, measuring enantiomeric excess, and separating enantiomers with the help of inhomogeneous external fields.
关键词： laser-induced orientation,propylene oxide,chiral molecules,optical centrifuge,enantioselective
更新于2025-09-11 14:15:04
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Dissymmetry enhancement in enantioselective synthesis of helical polydiacetylene by application of superchiral light
摘要： Superchiral light, generated by the interference of two counter-propagating circularly polarized light (CPL) with same frequency, opposite handedness and different intensity, exhibits enhanced dissymmetry in its interaction with chiral molecules, and has the potential for ultrasensitive detection and characterization of chiral molecules. It is anticipated that the enhanced optical dissymmetry in superchiral light (SCL) field may be utilized to promote asymmetric photochemical reactions efficiency. Herein we reported SCL impart greater chiral bias to trigger asymmetric photo-polymerization reaction from initially achiral diacetylene (DA) monomer, and the enhanced optical dissymmetry for whole polydiacetylene (PDA) films could be achieved. An explanation based on the chiral transfer and amplification of chiral bias from SCL during the polymerization process has been proposed. Moreover, thus formed chiral PDA films polymerized by SCL exhibited enhanced enantioselective recognition ability, and can serve as a direct visual probe for the discrimination of some specific enantiomers.
关键词： polydiacetylene,asymmetric photochemical reactions,chiral molecules,enantioselective recognition,Superchiral light
更新于2025-09-10 09:29:36
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Real single-loop cyclic three-level configuration of chiral molecules
摘要： Single-loop cyclic three-level ((cid:2)-type) con?guration of chiral molecules was used for enantio-separation in many theoretical works. Considering the effect of molecular rotation, this simple single-loop con?guration is generally replaced by a complicated multiple-loop con?guration containing multiple degenerate magnetic sublevels and the ability of the enantio-separation methods is suppressed. For chiral asymmetric top molecules, we propose a scheme to construct a real single-loop (cid:2)-type con?guration with no connections to other states by applying three microwave ?elds with appropriate polarization vectors and frequencies. With our scheme, the previous theoretical proposals for enantio-separation based on single-loop (cid:2)-type con?gurations can be experimentally realized when the molecular rotation is considered.
关键词： single-loop (cid:2)-type con?guration,chiral molecules,enantio-separation,asymmetric top molecules,microwave ?elds
更新于2025-09-09 09:28:46
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Chiral Analysis || Raman Optical Activity
摘要： Raman optical activity (ROA) has many advantages over conventional Raman spectroscopy for investigation of chiral molecules, in general, and biological molecules, in particular, on account of their homochirality. Since it is a manifestation of vibrational optical activity [1], being complementary to vibrational circular dichroism (VCD), ROA is more sensitive to the 3D structures of chiral molecules through its dependence on their absolute handedness, which has led to its development as an incisive probe of the structure and behavior of biomolecules in aqueous solution. For example, ROA spectra obtained from proteins can provide detailed information on the secondary and tertiary structures adopted by polypeptide backbones. Additionally, ROA can probe the tautomers of side chains. In common with other vibrational spectroscopies, there is no restriction on the size of molecules, or in their type, that can be investigated by ROA, broadening its application to unfolded proteins, viruses, and carbohydrates.
关键词： vibrational circular dichroism,proteins,Raman optical activity,aqueous solution,carbohydrates,vibrational optical activity,biological molecules,biomolecules,viruses,chiral molecules
更新于2025-09-09 09:28:46
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Real-time determination of enantiomeric and isomeric content using photoelectron elliptical dichroism
摘要： The fast and accurate analysis of chiral chemical mixtures is crucial for many applications but remains challenging. Here we use elliptically-polarized femtosecond laser pulses at high repetition rates to photoionize chiral molecules. The 3D photoelectron angular distribution produced provides molecular fingerprints, showing a strong forward-backward asymmetry which depends sensitively on the molecular structure and degree of ellipticity. Continuously scanning the laser ellipticity and analyzing the evolution of the rich, multi-dimensional molecular signatures allows us to observe real-time changes in the chemical and chiral content present with unprecedented speed and accuracy. We measure the enantiomeric excess of a compound with an accuracy of 0.4% in 10 min acquisition time, and follow the evolution of a mixture with an accuracy of 5% with a temporal resolution of 3 s. This method is even able to distinguish isomers, which cannot be easily distinguished by mass-spectrometry.
关键词： real-time monitoring,isomer distinction,photoelectron elliptical dichroism,enantiomeric excess,chiral molecules
更新于2025-09-04 15:30:14