Real-time observation of phonon-polariton dynamics in ferroelectric LiNbO3 in time-frequency space

Ikegaya, Yuki; Sakaibara, Hiroyuki; Minami, Yasuo; Katayama, Ikufumi; Takeda, Jun

doi:10.1063/1.4928480

Cited by 22 publications

(29 citation statements)

References 24 publications

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“…1b, to avoid 800 nm pump light reaching the detectors, the pump and probe pulses crossed the sample at a small angle, allowing spatial filtering of the pump beam. propagating phonon-polaritons [18]. The backward propagating phonon-polariton contributes a larger signal at 2.9 THz, which may obscure the signal from the 3.9 THz mode.…”

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confidence: 99%

“…A number of ISRS studies have been performed on LiNbO 3 , mainly in an effort to map out the phonon-polariton dispersion [14][15][16][17]. A recent study showed radiative control over vibrational modes in lithium niobate using ISRS in an optical Kerr effect measurement scheme to simultaneously excite and probe both forward and backward propagating phonon-polaritons [18].…”

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confidence: 99%

“…Pump and probe pulses were focused and overlapped spatially on the sample. The (THz or ISRS) excitation induces the lattice vibration, and the probe pulse interrogates the phonon-polariton vibration via a Raman scattering process [18] (this mode is necessarily both IR and Raman active). Polarization changes to the probe beam are recorded by directing the probe beam through a quarter-wave plate (QWP) with fast axis set at 45° to the initial probe polarization, followed by a Wollaston prism (WP) to split it into separate vertically and horizontally polarized beams (identical to a standard electrooptic sampling configuration [19]).…”

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Experimental determination of the interatomic potential in LiNbO3 via ultrafast lattice control

Dastrup

Hall

Johnson

2017

Applied Physics Letters

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We present a direct comparison between resonant terahertz (THz) and nonresonant impulsive stimulated Raman scattering (ISRS) excitation of phonon-polaritons in ferroelectric lithium niobate. THz excitation offers advantages of selectively driving only the forward propagating phonon-polariton mode to exceedingly high amplitudes, without complications due to nonlinear processes at the high 800 nm pump fluences used in Raman excitation. At peak-to-peak THz electric field strengths exceeding 1 MV/cm, the ferroelectric lattice is driven into the anharmonic regime, allowing experimental determination of the shape of the potential energy surface.Ultrafast control over a crystalline lattice is of interest in developing a basic understanding of how light can influence material properties, as well as potential practical applications such as the development of ultrafast switches and a variety of optoelectronic applications [1][2][3][4]. Strong THz radiation, with frequencies resonant to the modes of interest, has been promoted as a preferred means of lattice control [1] over two common routes: displacive excitation [5,6] and nonresonant Raman excitation of vibrations [7][8][9]. In typical displacive-type excitation, energy is deposited into the material's electronic subsystem, transiently distorting the lattice. Such excitation may coherently drive many modes simultaneously, but potentially leaves large amounts of (unwanted) incoherent thermal energy. Nonresonant ultrafast Raman excitation, termed impulsive stimulated Raman scattering (ISRS) [7-9], can coherently excite lattice modes without the excess thermal energy, but it is an inefficient process and thus extremely high-fluence laser pulses are required to a

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Experimental determination of the interatomic potential in LiNbO3 via ultrafast lattice control

Dastrup

Hall

Johnson

2017

Applied Physics Letters

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“…15 Therefore, performing observations of lightinduced lattice vibrations located in the THz-frequency region (so-called phonon-polaritons) over a wide range of temperatures remains an important task. Although the dynamic behaviors of ferroelectric phonon-polaritons have been studied using ultrafast measurements, [16][17][18] most of these experiments were conducted at room temperature. Obtaining measurements at temperatures lower than $170 K was quite difficult because of the long-lived photorefractive effects.…”

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confidence: 99%

Anharmonic phonon-polariton dynamics in ferroelectric LiNbO3 studied with single-shot pump-probe imaging spectroscopy

Kuribayashi

Motoyama

Arashida

et al. 2018

Journal of Applied Physics

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We demonstrate that single-shot pump-probe imaging spectroscopy with an echelon mirror enables us to disclose the ferroelectric phonon-polariton dynamics across a wide temperature range from 10 K to 375 K while avoiding the photorefractive effects that appear prominently at low temperatures. The E-mode phonon-polaritons corresponding to the two transverse optical modes, TO 1 and TO 3 , up to $7 THz were induced in LiNbO 3 through an impulsive stimulated Raman scattering process. Subsequently, using single-shot pump-probe imaging spectroscopy over a minimal cumulative time, we successfully visualized the phonon-polariton dynamics in time-wavelength space even at low temperatures. We found that the phase-matching condition significantly affected the observed temperature-dependent phonon-polariton frequency shift. The anharmonicity of the TO 1 and TO 3 modes was then evaluated based on an anharmonic model involving higher-order interactions with acoustic phonons while eliminating the influence of the frequency shift due to the phase-matching condition. The observed wavenumber-dependent damping rate was analyzed by considering the bilinear coupling of the TO 1 or TO 3 modes with the thermally activated relaxation mode. We found that the phonon-polariton with a higher frequency and wavenumber had a higher damping rate at high temperatures because of its frequent interaction with the thermally activated relaxation mode and acoustic phonons. The TO 3 mode displayed greater bilinear coupling than the TO 1 mode, which may also have contributed to the observed high damping rate. Thus, using our unique single-shot spectroscopy technique, we could reveal the overall anharmonic characteristics of the E-mode phonon-polaritons arising from both the acoustic phonons and the relaxation mode.

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“…The loss of inversion symmetry allows and enhances the optical nonlinearities such as sum and difference frequency generation, the optical Kerr effect, and excitation of polaritons with ultrafast near-infrared (NIR) laser pulses222324. These nonlinearities are important ingredients in designing future optoelectronic devices.…”

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High-Acquisition-Rate Single-Shot Pump-Probe Measurements Using Time-Stretching Method

Kobayashi

Minami

Johnson

et al. 2016

Sci Rep

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Recent advances of ultrafast spectroscopy allow the capture of an entire ultrafast signal waveform in a single probe shot, which greatly reduces the measurement time and opens the door for the spectroscopy of unrepeatable phenomena. However, most single-shot detection schemes rely on two-dimensional detectors, which limit the repetition rate of the measurement and can hinder real-time visualization and manipulation of signal waveforms. Here, we demonstrate a new method to circumvent these difficulties and to greatly simplify the detection setup by using a long, single-mode optical fiber and a fast photodiode. Initially, a probe pulse is linearly chirped (the optical frequency varies linearly across the pulse in time), and the temporal profile of an ultrafast signal is then encoded in the probe spectrum. The probe pulse and encoded temporal dynamics are further chirped to nanosecond time scales using the dispersion in the optical fiber, thus, slowing down the ultrafast signal to time scales easily recorded with fast detectors and high-bandwidth electronics. We apply this method to three distinct ultrafast experiments: investigating the power dependence of the Kerr signal in LiNbO3, observing an irreversible transmission change of a phase change material, and capturing terahertz waveforms.

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Real-time observation of phonon-polariton dynamics in ferroelectric LiNbO3 in time-frequency space

Cited by 22 publications

References 24 publications

Experimental determination of the interatomic potential in LiNbO3 via ultrafast lattice control

Experimental determination of the interatomic potential in LiNbO3 via ultrafast lattice control

Anharmonic phonon-polariton dynamics in ferroelectric LiNbO3 studied with single-shot pump-probe imaging spectroscopy

High-Acquisition-Rate Single-Shot Pump-Probe Measurements Using Time-Stretching Method

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