Autry Travis M, Moody Galan, Fraser James, McDonald Corey, Mirin R P, Silverman Kevin
National Institute of Standards and Technology, Boulder, Colorado 80305, USA.
Queen's University, Kingston, Ontario ONK7L3N6, Canada.
Optica. 2019;6(6). doi: 10.1364/optica.6.000735.
Multidimensional coherent spectroscopy is a powerful tool for understanding the ultrafast dynamics of complex quantum systems. To fully characterize the nonlinear optical response of a system, multiple pulse sequences must be recorded and quantitatively compared. We present a new single-scan method that enables rapid and parallel acquisition of all unique pulse sequences corresponding to first- and third-order degenerate wave-mixing processes. Signals are recorded with shot-noise limited detection, enabling acquisition times of ~2 minutes with ~100 zs phase stability and ~8 orders of dynamic range, in a collinear geometry, on a single-pixel detector. We demonstrate this method using quantum well excitons, and quantitative analysis reveals new insights into the bosonic nature of excitons. This scheme may enable rapid and scalable analysis of unique chemical signatures, metrology of optical susceptibilities, nonperturbative coherent control, and the implementation of quantum information protocols using multidimensional spectroscopy.
多维相干光谱学是理解复杂量子系统超快动力学的有力工具。为了全面表征系统的非线性光学响应，必须记录多个脉冲序列并进行定量比较。我们提出了一种新的单扫描方法，该方法能够快速并行采集与一阶和三阶简并波混频过程对应的所有独特脉冲序列。信号通过散粒噪声受限检测进行记录，在共线几何结构下，使用单像素探测器，可实现约2分钟的采集时间，具有约100 zeptosecond的相位稳定性和约8个数量级的动态范围。我们用量子阱激子演示了该方法，定量分析揭示了激子玻色子性质的新见解。该方案可能实现对独特化学特征的快速可扩展分析、光学磁化率的计量、非微扰相干控制以及使用多维光谱学实现量子信息协议。
