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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Cavity Ring-Down Polarimetry (CRDP): A New Scheme for Probing Circular Birefringence and Circular Dichroism in the Gas Phase
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Cavity Ring-Down Polarimetry (CRDP): A New Scheme for Probing Circular Birefringence and Circular Dichroism in the Gas Phase

机译：腔衰荡极化（CRDP）：探测气相中的双折射和圆二色性的新方案

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摘要

Cavity ring-down polarimetry (CRDP), a new, ultrasensitive method for probing circular birefriengence and circular dichroism, has been developed by extending the well-established technique of pulsed cavity ring-own spectroscopy (CRDS). The concurrent incorporation of polarization elements into the stable resonator, injection optics, and detection train of a conventional CRDS apparatus is found to permit the quantitative measurement of optical rotation and differential absorption induced by the presence of chiral compounds. The sensitivity of this novel scheme is sufficient to allow (low-pressure) gas-phase species to be interrogated under ambient conditions, a fact highlighted by the direct determination of specific rotation at 355 nm ([α]_(355nm)~(25 ℃)) for gaseous samples of α-pinene, β-pinene, cis-pinane, limonene, fenchone, and propylene oxide. Although usually precluded by the signal discrimination limits imposed upon traditional polarimeters, such gas-phase studies of nonresonant optical activity in the visible and near-ultraviolet regions of the electromagnetic spectrum can serve to calibrate ab initio theoretical predictions and to examine the roles of solvent-solute interactions. Comparison of the CRDP-measured specific rotation angles for isolated (gaseous) chiral molecules with analogous solution-phase results reveals that solvent effects can be significant and nonintuitive, often leading to solvent-mediated [α]_(355nm)~(25 ℃) values that differ significantly from their gas-phase counterparts in both magnitude and sign.
机译：腔环衰荡极化法（CRDP）是探测圆形双折射和圆二色性的一种新的超灵敏方法，它是通过扩展已建立的脉冲腔环拥有光谱法（CRDS）来开发的。发现将偏振元件同时并入常规CRDS设备的稳定谐振器，注入光学器件和检测列中可以定量测量由手性化合物的存在引起的旋光度和吸收差。这种新颖方案的灵敏度足以允许在环境条件下对（低压）气相物质进行讯问，这一事实在直接确定355 nm（[α] _（355nm）〜（25 ℃））用于α-pine烯，β-pine烯，顺式pin烷，li烯，fenchone和环氧丙烷的气态样品。尽管通常不受传统旋光仪施加的信号辨别限制的限制，但这种在电磁波谱的可见光和近紫外光区域的非共振光学活性的气相研究可用于校准从头开始的理论预测并检验溶剂的作用。溶质相互作用。将CRDP测量的分离的（气态）手性分子的比旋角与类似的溶液相结果进行比较表明，溶剂的作用可能是显着且非直觉的，通常导致溶剂介导的[α] _（355nm）〜（25℃）在气相的大小和符号上均明显不同于气相色谱。

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