Passively phase-stable monolithic all-reflective two

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Passively phase-stable monolithic all-reflective two-dimensional electronic spec-troscopy based on a 4-quadrant mirror

This content has been downloaded from IOPscience. Please scroll down to see the full text. 2014 J. Phys.: Conf. Ser. 488 142001 (http://iopscience.iop.org/1742-6596/488/14/142001) View the table of contents for this issue, or go to the journal homepage for more

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XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013) IOP Publishing Journal of Physics: Conference Series 488 (2014) 142001 doi:10.1088/1742-6596/488/14/142001

Passively phase-stable monolithic all-reflective two-dimensional electronic spectroscopy based on a 4-quadrant mirror Yizhu Zhang*† 1, Kristina Meyer*, Christian Ott* and Thomas Pfeifer* 2 *

†

Max-Planck Institute for Nuclear Physics, 69117 Heidelberg, Germany Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210, China

Synopsis A new design for a passively phase-stable two-dimensional electronic spectroscopy experiment, based on a 4-quadrant mirror concept, is introduced. The new setup, which is particularly simple and robust, is suitable for few-cycle laser pulses and ultrabroad-bandwidth light in the ultraviolet, visible and near-infrared (IR) region, with the capability to be used under grazing incidence for soft-x-ray or x-ray light at Free-Electron Lasers.

Two-dimensional (2D) electronic spectroscopy is a versatile tool to track electronic dynamics in complex quantum systems. Compared to traditional (onedimensional) spectroscopy, it allows to uncover quantum-state coupling and energy-transfer pathways in complex overlapping spectral line shapes. 2D electronic spectroscopy has already been successfully applied to investigate ultrafast dynamics in complex systems, e.g. photosynthesis [1] and semiconductor materials [2]. The current designs [3] of 2D electronic spectroscopy involve transmissions through optical components, or routing beams via significantly different optical paths. Here, we introduce a new passively phasestable 2D spectroscopy setup based on a fourquadrant mirror [4], shown in Fig. 1. A spatial mask creates the box geometry by splitting the beam into four parallel beamlets. These beamlets are then reflected by a home-built four-quadrant split mirror. The split-mirror arrangement is composed of four square mirrors. The two lower mirrors, which are fixed on independent piezo stages, can rapidly scan the pulses k1 and k2 (inset of Figure 1) with subwavelength resolution. The upper right mirror acts as the third excitation beam k3, while the upper left beam plays the role of the local oscillator (LO). All four mirrors are fixed on independent micrometer translation stages, which can be used not only for micrometer alignment, but also for introducing the waiting time T within the pulse sequence with femtosecond accuracy. Then, the beams are reflected and focused onto the sample by a f=100 mm concave mirror. The incidence angles on both the split-mirror and the focusing †1 2

mirror are optimized to be less than 10º, to avoid the angular deviation in the focal plane. Before the sample, a second mask is inserted to spatially filter out the diffraction caused by the small holes on the first mask.

Figure 1. The design of the four-quadrant splitmirror 2D spectroscopy setup.

The new design is tested by the benchmark dye sample IR144 in methanol around 800 nm. A step-to-step phase error lower than ʌ/6 is achieved, which clearly demonstrates the passive sub-wavelength stability of the setup. Y. Z. Z. is grateful for support from the NSFC (Grant NO. 11274232), the National Basic Research Program of China (973 Program) (grant 2013CB922200) References [1] T. Brixner et al 2005 Nature 434 625. G. S. Engel et al 2007 Nature 446 782. [2] X. Li et al 2006 Phys. Rev. Lett. 96 057406. K. W. Stone et al 2009 Science 324 1169. [3] A. D. Bristow et al 2009 Rev. Sci. Instrum. 80 073108. T. Brixner et al 2004 Opt. Lett. 29 884. J. C. Vaughan et al 2007 J. Phys. Chem. A 111 4873. [4] Y. Zhang et al 2013 Opt. Lett. 38 356.

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E-mail: [email protected]

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