Ladder Climbing on the Anharmonic Intermolecular Potential in an Amino Acid Microcrystal via an Intense Monocycle Terahertz Pulse

Jewariya, Mukesh; Nagai, Masaya; Tanaka, Kōichiro

doi:10.1103/physrevlett.105.203003

Cited by 94 publications

(54 citation statements)

References 28 publications

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“…[6][7][8][9][10][11][12] Since Hebling et al 13 ͑2002͒ proposed a tilted-pumppulse-front scheme for efficient phase-matched THz pulse generation using LiNbO 3 crystals, the technique has been rapidly developing. This technique has demonstrated the possibility of THz pulse generation with energies on the scale of 10 J by using an amplified Ti:sapphire laser with low repetition frequencies.…”

mentioning

confidence: 99%

Single-cycle terahertz pulses with amplitudes exceeding 1 MV/cm generated by optical rectification in LiNbO3

Hirori

Doi

Blanchard

et al. 2011

Applied Physics Letters

786

501

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Using the tilted-pump-pulse-front scheme, we generate single-cycle terahertz ͑THz͒ pulses by optical rectification of femtosecond laser pulses in LiNbO 3 . In our THz generation setup, the condition that the image of the grating coincides with the tilted-optical-pulse front is fulfilled to obtain optimal THz beam characteristics and pump-to-THz conversion efficiency. By using an uncooled microbolometer-array THz camera, it is found that the THz beam leaving the output face of the LN crystal can be regarded as a collimated rather than point source. The designed focusing geometry enables tight focus of the collimated THz beam with a spot size close to the diffraction limit, and the maximum THz electric field of 1.2 MV/cm is obtained. © 2011 American Institute of Physics. ͓doi:10.1063/1.3560062͔Recent successful developments in efficient high-power terahertz ͑THz͒ pulse generation has created many promising applications such as in large-scale object imaging, medical diagnosis and treatment, and remote sensing techniques for security issues.1,2 In addition, intense THz pulses allow for study of unexplored nonlinear phenomena such as coherent THz manipulation of quantum states, 3,4 high-order harmonic generation, 5 nonlinear optical processes, and nonlinear transport phenomena in solids. [6][7][8][9][10][11][12] Since Hebling et al.13 ͑2002͒ proposed a tilted-pumppulse-front scheme for efficient phase-matched THz pulse generation using LiNbO 3 crystals, the technique has been rapidly developing. This technique has demonstrated the possibility of THz pulse generation with energies on the scale of 10 J by using an amplified Ti:sapphire laser with low repetition frequencies.14,15 To make the technique versatile for applications and useful for study of unexplored nonlinear phenomena, a generation setup to obtain optimal THz beam characteristics and a maximized THz peak field is required. A recent detailed analysis of the scheme predicted that the imaging errors in the setup consisting of a grating and lenses can lead to distortion in THz intensity profile after the LiNbO 3 output surface. 16 This distortion could create strong and ambiguous divergence in the THz beam, causing inaccuracy in optimal optis design for THz measurement, thereby limiting its applications.In this paper, we report the generation of single-cycle THz pulses using the tilted-pump-pulse-front scheme with a 1.3 mol % MgO-doped stoichiometric LiNbO 3 ͑LN͒ crystal. In the THz generation setup, the condition that the image of the grating coincides with the tilted-optical-pulse front is fulfilled to obtain optimal THz beam characteristics and pumpto-THz conversion efficiency. The propagation characteristics of the THz beam leaving the output face of the LN crystal were measured by an uncooled microbolometer-array THz camera. The results show that the THz beam had divergence of 52Ϯ 5 mrad in the horizontal direction for 1 THz.The designed focusing geometry for the collimated THz beam enables tight focus onto the electro-optic ͑EO͒ crystal with a spot size ...

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mentioning

confidence: 99%

Single-cycle terahertz pulses with amplitudes exceeding 1 MV/cm generated by optical rectification in LiNbO3

Hirori

Doi

Blanchard

et al. 2011

Applied Physics Letters

786

501

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“…Ladder climbing in a phonon mode of the crystalline amino acid excited by a single cycle THz pulse has been reported recently by Jewariya et al [129]. In amino acids and other hydrogen bonded crystalline substances like sugars, the dielectric properties in the THz range are determined by low-lying vibrations which are an admixture of inter-and intramolecular degrees of freedom.…”

Section: Vibrational Excitationmentioning

confidence: 99%

Intense ultrashort terahertz pulses: generation and applications

Hoffmann¹,

Fülöp²

2011

J. Phys. D: Appl. Phys.

332

215

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Ultrashort terahertz pulses derived from femtosecond table-top sources have become a valuable tool for time-resolved spectroscopy during the last two decades. Until recently, the pulse energies and field strengths of these pulses have been generally too low to allow for the use as pump pulses or the study of nonlinear effects in the terahertz range. In this review article we will describe methods of generation of intense single cycle terahertz pulses with emphasis on optical rectification using the tilted-pulse-front pumping technique. We will also discuss some applications of these intense pulses in the emerging field of nonlinear terahertz spectroscopy.

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“…This onephoton absorption (1PA) process requires an infrared-active transition and a pump spectrum that covers the phonon frequency Ω=2π, typically between ∼1 and 40 THz [ Fig. 1(a)] [10][11][12][13]. To date, most works have implemented lattice excitation using stimulated Raman scattering (SRS) of a light pulse containing frequencies ω 0 1 and ω 0 2 ¼ ω 0 1 þ Ω, both at roughly 2π × 500 THz [ Fig.…”

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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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Ladder Climbing on the Anharmonic Intermolecular Potential in an Amino Acid Microcrystal via an Intense Monocycle Terahertz Pulse

Cited by 94 publications

References 28 publications

Single-cycle terahertz pulses with amplitudes exceeding 1 MV/cm generated by optical rectification in LiNbO3

Single-cycle terahertz pulses with amplitudes exceeding 1 MV/cm generated by optical rectification in LiNbO3

Intense ultrashort terahertz pulses: generation and applications

Terahertz Sum-Frequency Excitation of a Raman-Active Phonon

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