The Earliest Stage of Photoinduced Phase Transition in a Strongly Correlated Organic System Using a 10-fs Pulse

Onda, Ken; Matsubara, Y.; Ishikawa, Tadaharu; Okimoto, Y.; Koshihara, Shin‐ya; Hiramatsu, Takeshi; Saito, Gunzi; Nakano, Yoshiaki; Yamochi, Hideki

doi:10.1051/epjconf/20134103001

EPJ Web of Conferences

2013

DOI: 10.1051/epjconf/20134103001

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The Earliest Stage of Photoinduced Phase Transition in a Strongly Correlated Organic System Using a 10-fs Pulse

Ken Onda

Y. Matsubara

Tadaharu Ishikawa

et al.

Abstract: Abstract. We examined the initial excited state before photoinduced phase transition in a charge transfer complex (EDO-TTF) 2 PF 6 and revealed the conversion process to the photoinduced phase and the electronic coherence at the excited state.

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“…The first step takes place within 100 fs and the photoinduced phase is assigned to the (1010) charge disproportionate phase, as shown in the lower panel of Fig. 1(a) [17][18][19][20][21][22][23][24][25][26][27][28]. The time required for the emergence of the metallic phase is 100 ps [22,23].…”

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Coherent dynamics of photoinduced phase formation in a strongly correlated organic crystal

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The photoinduced phase formation in a strongly correlated crystal (EDO-TTF) 2 PF 6 (EDO-TTF: 4,5ethylenedioxytetrathiafulvalene) is investigated using a 12 fs laser pulse. The formation time is determined as 40 fs with observation of coherence of electron-phonon coupled excited states prior to formation. The temperature-independent dephasing time is determined as ß22 fs up to 180 K and the frequency of phonon oscillation is ß38 THz, corresponding to the intramolecular vibrations in EDO-TTF. The phase formation is coherently controlled by relative-phase-controlled two-pulse excitation.Strongly correlated materials exhibit intriguing phases such as superconductor, Mott insulator, spin liquid, and charge density wave [1]. Competitions between electrons, phonons, and spins in the materials play a key role in creating these phases. Photoexcitation controls this competition and initiates cooperative response resulting in a macroscopic ordering, called photoinduced phase transition (PIPT). In PIPT, electronphonon interactions lead to significant changes in dynamics. Thus, not only pure electronic but also electron-phonon dynamics have attracted considerable attention. Time-resolved optical spectroscopy has been widely used to study the electronic and vibrational dynamics and subsequent PIPT by monitoring the transient changes in optical constants on a femtosecond time scale [2][3][4][5][6]. However, the interactions dominating electronic phases are often inferred indirectly from these measurements.Coherent nonlinear spectroscopy utilizing third-order nonlinear response is a powerful tool to directly investigate interactions and has been applied to reveal ultrafast dynamics in semiconductors [7,8], light-harvesting protein complexes [9][10][11][12], and other functional materials [13,14]. However, this spectroscopy has been applied only to a few strongly correlated materials [15] because their electronic coherence is considered to be too short owing to their strong electron-electron interaction. In this Rapid Communication we have investigated 10-fs time scale dynamics of the strongly correlated organic chargetransfer (CT) complex (EDO-TTF) 2 PF 6 (EDO-TTF: 4,5ethylenedioxytetrathiafulvalene) [16], which exhibits unique PIPT due to strong electron-phonon interactions. We also revealed the formation process of the photoinduced phase * onda.k.aa@m.titech.ac.jp from the phonon-coupled excited state as well as the role of coherences in the excited state.(EDO-TTF) 2 PF 6 undergoes metal-insulator phase transition at 280 K because of its strong electron-electron and electron-phonon interactions and shows (0110)-type charge ordering below the transition temperature [16], where the number in parentheses represent the order of charge for EDO-TTF molecules, as shown in the upper panel of Fig. 1(a). This material exhibits a two-step phase transition triggered by photoexcitation in the low-temperature phase, that is, "insulator"-"photoinduced phase"-"metal" transition. The first step takes place within 100 fs and the photoinduced ph...

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Coherent dynamics of photoinduced phase formation in a strongly correlated organic crystal

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The Earliest Stage of Photoinduced Phase Transition in a Strongly Correlated Organic System Using a 10-fs Pulse

Abstract: Abstract. We examined the initial excited state before photoinduced phase transition in a charge transfer complex (EDO-TTF) 2 PF 6 and revealed the conversion process to the photoinduced phase and the electronic coherence at the excited state.

Cited by 1 publication

References 8 publications

Coherent dynamics of photoinduced phase formation in a strongly correlated organic crystal

Coherent dynamics of photoinduced phase formation in a strongly correlated organic crystal

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