Yang Lijun, Mukamel Shaul
Chemistry department, University of California, Irvine, California, 92697-2025, United States.
Proc SPIE Int Soc Opt Eng. 2010;7600:76001G1-76001G9. doi: 10.1117/12.840993.
Multidimensional analysis of coherent signals is commonly used in nuclear magnetic resonance to study correlations among spins. These techniques were recently extended to the femtosecond regime and applied to chemical, biological and semiconductor systems. In this work, we apply a two-dimensional correlation spectroscopy technique which employs double-quantum-coherence to investigate many-body effects in a semiconductor quantum well. The signal is detected along the direction k(1)+ k(2)- k(3), where k(1), k(2) and k(3) are the pulse wave vectors in chronological order. We show that this signal is particularly sensitive to many-body correlations which are missed by time-dependent Hartree-Fock approximation. The correlation energy of two-exciton can be probed with a very high resolution arising from a two-dimensional correlation spectrum, where two-exciton couplings spread the cross peaks along both axes of the 2D spectrum to create a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo (-k(1)+ k(2)+ k(3)).
相干信号的多维分析常用于核磁共振中以研究自旋之间的相关性。这些技术最近已扩展到飞秒领域,并应用于化学、生物和半导体系统。在这项工作中,我们应用一种二维相关光谱技术,该技术采用双量子相干来研究半导体量子阱中的多体效应。信号沿着k(1)+ k(2)- k(3)方向检测,其中k(1)、k(2)和k(3)是按时间顺序排列的脉冲波矢。我们表明,该信号对多体相关性特别敏感,而这些相关性是含时哈特里 - 福克近似所遗漏的。二维相关光谱产生的高分辨率可用于探测双激子的相关能,其中双激子耦合使二维光谱的交叉峰沿两个轴展开,从而形成特征性的高分辨率图案。传统的一维四波混频或其他二维相关光谱信号(如光回波(-k(1)+ k(2)+ k(3)))无法提供这种详细程度的信息。