Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation

Zalden, Peter; Song, Liwei; Wu, Xiaojun; Huang, Haoyu; Ahr, Frederike; Mücke, Oliver D.; Reichert, Joscha; Thorwart, Michael; Mishra, Pankaj Kr.; Welsch, Ralph; Santra, Robin; Kärtner, Franz X.; Bressler, Christian

doi:10.1038/s41467-018-04481-5

Cited by 73 publications

(92 citation statements)

References 59 publications

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“…[165,166] By comparing optically driven with THz-driven alignment, it was determined whether or whether not rotational molecular degrees of freedom make a dominant contribution to the dielectric function of polar solvents such as methanol. Accordingly, it was shown that intense THz pulses align solvent molecules more efficiently than optical fields do.…”

Section: Properties Of Driven Modesmentioning

confidence: 99%

Laser‐Driven Strong‐Field Terahertz Sources

Fülöp

Tzortzakis

Kampfrath

2019

Advanced Optical Materials

284

147

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reason for this interest relies on the fact that THz radiation can couple resonantly to numerous fundamental motions of ions, electrons, and electron spins in all phases of matter. For example, in solids, the THz range overlaps with the frequency of lattice vibrations (phonons), the collision rates of conduction electrons, the binding energy of bound electron-hole pairs (excitons), and the precession frequency of spin waves (magnons). Consequently, THz radiation, both continuous-wave and pulsed, has been used for characterization of and gaining insight into elementary processes in complex materials. The majority of these studies used relatively weak THz fields and, thus, probed the linear response of the material, without inducing notable material modifications.Only recently, however, completely new avenues in THz science were opened up by triggering nonlinear THz responses of materials. [3][4][5][6][7][8][9][10][11][12][13] Instead of using weak fields to primarily observe selected THz modes such as phonons or magnons, strong fields allow one to actively drive them to unprecedentedly large amplitudes, potentially thereby resulting in novel states of matter. [6,8,11] For example, simulations suggest that exciting matter with intense THz transients may lead to massive modifications of electrically [14] or magnetically [15] ordered domains and enable the acceleration of free ions to ≈1 MeV, [16] and postacceleration to 50-100 MeV energies. [17] Remarkable experimental results such as switching of magnetic order, [18,19] parametric amplification of optical phonons, [20] novel insights into spin-lattice coupling, [21,22] and acceleration of free electrons in a THz linear accelerator [23] were achieved only recently. This progress has been made possible by the development of laser-driven table-top THz sources routinely providing pulses with unprecedented energies and peak electric and magnetic field strengths throughout the entire THz spectral range. Different laser-based THz pulse generation techniques can be used to access different parts of the spectral range extending from 0.1 to 10 THz. Some of the recently developed technologies enable the generation of radiation with even larger bandwidth or tuning range up to 100 THz and beyond, which lead to an extension of what is called the THz spectral range. An overview of the approximate spectral coverage and the achieved highest pulse energies and peak electric-field strengths of various laserdriven technologies is given in Figure 1. ScopeIn this work, the basic principles of femtosecond-laser-driven intense pulsed THz sources and their recent development are reviewed. These sources are capable of delivering peak electric field strengths on the MV cm −1 scale. Corresponding typical THz pulse energies are on the µJ-to-mJ level, depending on A review on the recent development of intense laser-driven terahertz (THz) sources is provided here. The technologies discussed include various types of sources based on optical rectification (OR), spintronic emitters, and laserfilame...

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Section: Properties Of Driven Modesmentioning

confidence: 99%

Laser‐Driven Strong‐Field Terahertz Sources

Fülöp

Tzortzakis

Kampfrath

2019

Advanced Optical Materials

284

147

View full text Add to dashboard Cite

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“…The pump intensity required to drive liquid water into the nonlinear response regime depends on the wavelength. Based on the third-order responses reported previously, we tentatively estimate to 50 GW/cm 2 , 5 TW/cm 2 , 1 GW/cm 2 , and 5 TW/cm 2 , the peak power required to induce a pump-probe signal of roughly 1% at the frequency of~1 MHz [127,128],~1 THz [72], 10 THz [54], and~200 THz [129][130][131][132][133][134][135][136][137][138][139][140], respectively.…”

Section: Discussionmentioning

confidence: 68%

“…OR typically allows us to generate intense THz radiation below 5 THz (sketched in light green and light red in Figure 1c), while DFG covers higher frequencies (dark green and dark red in Figure 1c). Both inorganic (LiNbO 3 [66][67][68][69][70][71][72][73][74][75][76][77], GaSe [78][79][80], ZnTe [81,82], LiGaS 2 [83], GaP [84][85][86][87][88][89]) as well as organic (DSTMS [89][90][91][92], OH1 [93][94][95][96][97], DAST [98,99], DPFO [100], HMQ-TMS [101], OHQ-N2S [102]) crystals are phase-matched in the NIR and can emit pulsed THz fields with peak amplitudes in excess of 1 MV/cm. The approximate spectrum of the strongest THz pulses generated to date by non-linear optical methods in inorganic [62,64] and organic [63,65] crystals are shown in green and in red in Figure 1c, respectively.…”

Section: Introductionmentioning

confidence: 99%

Towards Intense THz Spectroscopy on Water: Characterization of Optical Rectification by GaP, OH1, and DSTMS at OPA Wavelengths

2020

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Water is the most prominent solvent. The unique properties of water are rooted in the dynamical hydrogen-bonded network. While TeraHertz (THz) radiation can probe directly the collective molecular network, several open issues remain about the interpretation of these highly anharmonic, coupled bands. In order to address this problem, we need intense THz radiation able to drive the liquid into the nonlinear response regime. Firstly, in this study, we summarize the available brilliant THz sources and compare their emission properties. Secondly, we characterize the THz emission by Gallium Phosphide (GaP), 2–{3–(4–hydroxystyryl)–5,5–dimethylcyclohex–2–enylidene}malononitrile (OH1), and 4–N,N–dimethylamino–4′–N′–methyl–stilbazolium 2,4,6–trimethylbenzenesulfonate (DSTMS) crystals pumped by an amplified near-infrared (NIR) laser with tunable wavelength. We found that both OH1 as well as DSTMS could convert NIR laser radiation between 1200 and 2500 nm into THz radiation with high efficiency (> 2 × 10−4), resulting in THz peak fields exceeding 0.1 MV/cm for modest pump excitation (~ mJ/cm2). DSTMS emits the broadest spectrum, covering the entire bandwidth of our detector from ca. 0.5 to ~7 THz, also at a laser wavelength of 2100 nm. Future improvements will require handling the photothermal damage of these delicate organic crystals, and increasing the THz frequency.

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“…Terahertz science has shown great potential in different applications such as security, medical imaging, and communications [1][2][3][4][5][6]. One of the main reasons for such interest in this field is the exclusive interaction of terahertz waves with some specific molecules [7][8][9]. Additionally, due to the low photon energy of terahertz radiation, it is a good candidate for non-destructive test (NDT) applications.…”

Section: Introductionmentioning

confidence: 99%

Numerical Performance Analysis of Terahertz Spectroscopy Using an Ultra-Sensitive Resonance-Based Sensor

et al. 2020

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A terahertz sensor structure is proposed that can sense any variations in analyte permittivity. The sensor essentially works according to the shifts in the resonance frequencies of its propagated spoof surface plasmonic modes. The proposed structure shows great support for surface plasmon oscillations, which is proved by the calculated dispersion diagram. To achieve this in terahertz frequencies, a metamaterial structure is presented in the form of a structure with two-dimensional periodic elements. Afterward, it is shown that the performance of the sensor can be affected by different parameters such as metal stripe thickness, length of metal stripe, and width of metal stripe as the most influential parameters. Each of the parameters mentioned can directly influence on the electric field confinement in the metal structure as well as the strength of propagation modes. Therefore, two propagation modes are compared, and the stronger mode is chosen for sensing purposes. The primary results proved that the quality factors of the resonances are substantially dependent on certain physical parameters. To illustrate this, a numerical parametric sweep on the thickness of the metal stripe is performed, and the output shows that only for some specific dimensions the electromagnetic local field binds strongly with the metal part. In a similar way, a sweeping analysis is run to reveal the outcome of the variation in analyte permittivity. In this section, the sensor demonstrates an average sensitivity value, ∼1,550 GHz/Permittivity unit, for a permittivity range between 1 and 2.2, which includes the permittivity of many biological tissues in the terahertz spectrum. Following this, an analysis is presented, in the form of two contour plots, for two electrical parameters, maximum electric field and maximum surface current, based on 24 different paired values of metal thickness and metal width as the two most critical physical parameters. Using the plotted contour diagrams, which are estimated using the bi-harmonic fitting function, the best physical dimension for the maximum capability of the proposed sensor is achieved. As mentioned previously, the proposed sensor can be applied for biological sensing due to the simplicity of its fabrication and its performance.

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Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation

Cited by 73 publications

References 59 publications

Laser‐Driven Strong‐Field Terahertz Sources

Laser‐Driven Strong‐Field Terahertz Sources

Towards Intense THz Spectroscopy on Water: Characterization of Optical Rectification by GaP, OH1, and DSTMS at OPA Wavelengths

Numerical Performance Analysis of Terahertz Spectroscopy Using an Ultra-Sensitive Resonance-Based Sensor

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