Phase-cycling schemes for pump–probe beam geometry two-dimensional electronic spectroscopy

• Published in: Chemical physics letters Vol. 550; pp. 156 - 161
• Main Authors: Zhang, Zhengyang, Wells, Kym Lewis, Hyland, Edward William James, Tan, Howe-Siang
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 22.10.2012
• ISSN: 0009-2614; 1873-4448
• DOI: 10.1016/j.cplett.2012.08.037

[Display omitted] ► Theoretical explanation and Experimental demonstration of phase cycling schemes for 2D pump probe spectroscopy. ► 1×2 Phase cycling recovers both rephasing and nonrephasing 2D spectra under certain experimental situations. ► 1×3 Phase cycling recovers all 2D spectra that has been shown hitherto to be only obtained with a 1×4 phase cycling scheme. ► Experimental studies performed with excellent agreement with theory. Experimental demonstrations and detailed theoretical explanations are provided for a thorough understanding of the various phase-cycling schemes in an optical pulse shaper assisted two-dimensional electronic spectroscopy (2DES) in a pump–probe beam geometry. We show that two and three-step phase-cycling schemes can be employed to retrieve both rephasing and nonrephasing 2D spectra. The studies were performed on the Qy transition of chlorophyll a.