All-optical control and visualization of ultrafast two-dimensional atomic motions in a single crystal of bismuth

Katsuki, Hirohiko; Delagnes, Jean-Christophe; Hosaka, K.; Ishioka, Kunie; Chiba, H.; Zijlstra, Eeuwe S.; Garcia, Martín E.; Takahashi, Hiroshi; Watanabe, Keiji; Kitajima, Masahiro; Matsumoto, Yoshiyasu; Nakamura, Kazutaka G.; Ohmori, Kenji

doi:10.1038/ncomms3801

Cited by 65 publications

(48 citation statements)

References 41 publications

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“…Remarkably, due to the low photon energies required, THz SFE provides a unique tool to steer chemical reactions [1] or phase transitions [7,8] in the electronic ground state, solely driven by Raman-active lattice vibrations. Shaping of THz pulses [48] to multicolor sequences could enable independent phase and amplitude control of the lattice trajectory along multiple normal coordinates, which is challenging with optical pulses accompanied by parasitic electronic excitations [49].…”

Section: Prl 119 127402 (2017) P H Y S I C a L R E V I E W L E T T Ementioning

confidence: 99%

Terahertz Sum-Frequency Excitation of a Raman-Active Phonon

et al. 2017

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In stimulated Raman scattering, two incident optical waves induce a force oscillating at the difference of the two light frequencies. This process has enabled important applications such as the excitation and coherent control of phonons and magnons by femtosecond laser pulses. Here, we experimentally and theoretically demonstrate the so far neglected up-conversion counterpart of this process: THz sumfrequency excitation of a Raman-active phonon mode, which is tantamount to two-photon absorption by an optical transition between two adjacent vibrational levels. Coherent control of an optical lattice vibration of diamond is achieved by an intense terahertz pulse whose spectrum is centered at half the phonon frequency of 40 THz. Remarkably, the carrier-envelope phase of the THz pulse is directly transferred into the phase of the lattice vibration. New prospects in general infrared spectroscopy, action spectroscopy, and lattice trajectory control in the electronic ground state emerge.

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Section: Prl 119 127402 (2017) P H Y S I C a L R E V I E W L E T T Ementioning

confidence: 99%

Terahertz Sum-Frequency Excitation of a Raman-Active Phonon

et al. 2017

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“…Very recently, we have reported that the degrees of excitation between two different bulk phonon modes of Bi can be controlled by using the optical phase of pump pulses. [40] …”

Section: Coherent Phonons Of Alkali Metal Layers At Metal Surfacesmentioning

confidence: 97%

Applications of Time‐Domain Spectroscopy to Electron–Phonon Coupling Dynamics at Surfaces

Matsumoto

2014

The Chemical Record

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Photochemistry is one of the most important branches in chemistry to promote and control chemical reactions. In particular, there has been growing interest in photoinduced processes at solid surfaces and interfaces with liquids such as water for developing efficient solar energy conversion. For example, photoinduced charge transfer between adsorbates and semiconductor substrates at the surfaces of metal oxides induced by photogenerated holes and electrons is a core process in photovoltaics and photocatalysis. In these photoinduced processes, electron-phonon coupling plays a central role. This paper describes how time-domain spectroscopy is applied to elucidate electron-phonon coupling dynamics at metal and semiconductor surfaces. Because nuclear dynamics induced by electronic excitation through electron-phonon coupling take place in the femtosecond time domain, the pump-and-probe method with ultrashort pulses used in time-domain spectroscopy is a natural choice for elucidating the electron-phonon coupling at metal and semiconductor surfaces. Starting with a phenomenological theory of coherent phonons generated by impulsive electronic excitation, this paper describes a couple of illustrative examples of the applications of linear and nonlinear time-domain spectroscopy to a simple adsorption system, alkali metal on Cu(111), and more complex photocatalyst systems.

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“…At high fluence, semiconductors may become unstable in the direction of certain phonon coordinates leading to an initially exponential increase of Q qλ , resulting in nonthermal melting. and used to visualize the real-space laser-induced atomic motions from an all-optical experiment [23].…”

Section: A Coherent Phononsmentioning

confidence: 99%

Ultrafast structural phenomena: theory of phonon frequency changes and simulations with code for highly excited valence electron systems

et al. 2014

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When a femtosecond-laser pulse excites a solid it may, among other ultrafast processes, induce coherent phonons, phonon frequency changes, thermal phonon squeezing, and nonthermal melting. Using our in-house code for highly excited valence electron systems, where laser-induced interatomic forces are computed "on the fly" from ab initio theory, we performed molecular dynamics simulations of supercells with up to 800 atoms. For Si we found that thermal phonon squeezing precurses nonthermal melting as a function of fluence. Furthermore, our molecular dynamics trajectories showed that nonthermal melting includes a stage during which the atoms move fractionally diffusive. We also simulated femtosecond-laser-excited Ge. In addition, we explain the electronic origin of laser-induced phonon frequency redshifts and blueshifts in Mg.

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All-optical control and visualization of ultrafast two-dimensional atomic motions in a single crystal of bismuth

Cited by 65 publications

References 41 publications

Terahertz Sum-Frequency Excitation of a Raman-Active Phonon

Terahertz Sum-Frequency Excitation of a Raman-Active Phonon

Applications of Time‐Domain Spectroscopy to Electron–Phonon Coupling Dynamics at Surfaces

Ultrafast structural phenomena: theory of phonon frequency changes and simulations with code for highly excited valence electron systems

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