A versatile ultrastable platform for optical multidimensional Fourier-transform spectroscopy

A versatile ultrastable platform for optical multidimensional Fourier-transform spectroscopy
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DOI:
10.1063/1.3184103
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发表时间:
2009-07-01
影响因子:
1.6
通讯作者:
Cundiff, S. T.
Cundiff, S. T.
中科院分区:
工程技术4区
文献类型:
--
作者:
Bristow, A. D.;Karaiskaj, D.;Cundiff, S. T.

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JILA 多维光学非线性光谱仪 (JILA-MONSTR) 是一个坚固、超稳定的平台,由嵌套和折叠式迈克尔逊干涉仪组成,可以主动进行相位稳定。该平台生成方形相同的激光脉冲,可以对其进行调整以在它们之间具有任意时间延迟,同时保持相位稳定性。 JILA-MONSTR 提供用于材料非线性激励的输出脉冲和用于感应信号的外差检测的相位稳定参考脉冲。这种布置非常适合执行相干光学实验,例如多维傅里叶变换光谱,它将非线性信号的相位记录为几个激发脉冲之间的时间延迟的函数。所得到的多维频谱是通过傅立叶变换获得的。该光谱可以解析、分离和隔离对与光学频率下的电子激发相关的光-物质相互作用的相干贡献。为了展示 JILA-MONSTR 的多功能性,提供了几个二维傅里叶变换光谱的演示,包括降低噪声的相位循环方案的示例。还显示了访问双量子相干性的频谱,其中所有激励脉冲都需要锁相来检测信号。
The JILA multidimensional optical nonlinear spectrometer (JILA-MONSTR) is a robust, ultrastable platform consisting of nested and folded Michelson interferometers that can be actively phase stabilized. This platform generates a square of identical laser pulses that can be adjusted to have arbitrary time delay between them while maintaining phase stability. The JILA-MONSTR provides output pulses for nonlinear excitation of materials and phase-stabilized reference pulses for heterodyne detection of the induced signal. This arrangement is ideal for performing coherent optical experiments, such as multidimensional Fourier-transform spectroscopy, which records the phase of the nonlinear signal as a function of the time delay between several of the excitation pulses. The resulting multidimensional spectrum is obtained from a Fourier transform. This spectrum can resolve, separate, and isolate coherent contributions to the light-matter interactions associated with electronic excitation at optical frequencies. To show the versatility of the JILA-MONSTR, several demonstrations of two-dimensional Fourier-transform spectroscopy are presented, including an example of a phase-cycling scheme that reduces noise. Also shown is a spectrum that accesses two-quantum coherences, where all excitation pulses require phase locking for detection of the signal.