Strong Anisotropy in Liquid Water upon Librational Excitation Using Terahertz Laser Fields

Novelli, Fabio; Pestana, Luis Ruiz; Bennett, Kochise; Sebastiani, Federico; Adams, Ellen M.; Stavrias, N.; Ockelmann, Thorsten; Colchero, Alejandro; Hoberg, Claudius; Schwaab, Gerhard; Head‐Gordon, Teresa; Havenith, Martina

doi:10.1021/acs.jpcb.0c02448

Cited by 23 publications

(77 citation statements)

References 111 publications

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“…This is especially challenging in the THz range due to lack of brilliant sources [4]. To this aim, a variety of nonlinear laser techniques have been used [16][17][18][19][20][21][22][23][24].…”

Section: Introductionmentioning

confidence: 99%

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Novelli

Adhlakha

et al. 2020

Applied Sciences

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The solvation properties of liquid water originate from the transient network of hydrogen-bonded molecules. In order to probe the coupling between the different modes of this network, nonlinear terahertz (THz) spectroscopy techniques are required. Ideally, these techniques should use a minimal volume and capitalize on sensitive field-resolved detection. Here we performed open aperture z-scan transmission experiments on static liquid cells, and detect the THz fields with electro-optical techniques. We show that it is possible to quantify the nonlinear response of liquid water at ~1 THz even when large signals originate from the sample holder windows.

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Section: Introductionmentioning

confidence: 99%

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Novelli

Adhlakha

et al. 2020

Applied Sciences

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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: 67%

“…For example, as sketched in orange in Figure 1c, single color pump-probe experiments at the free electron laser (FEL) facility FELIX in Nijmegen can currently be performed only between ca. 5 and 25 THz [54]. The severe beam time restrictions at the few available facilities, and the limited tunability in polarization and pulse length constrain the applicability of these sources.…”

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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“…Recently, researchers have successfully used THz pulses to drive liquids, such as dimethyl sulfoxide (DMSO), chloroform and liquid water, and tracked the molecular dynamics by detecting transient birefringence 24,[27][28][29][30][31][32][33] . In particular, in 2018, Zalden et al used a low-frequency single-cycle THz pulse (centre frequency of 0.25 THz) generated by optical rectification in a LiNbO 3 crystal to stimulate liquid water and observed the time-resolved birefringent signal induced by the transient orientation of dipole moments.…”

Section: Introductionmentioning

confidence: 99%

“…However, only the polarizability anisotropy caused by the orientational relaxation of liquid water was investigated in this study, which is limited by the relatively low-power and narrowband properties of the applied THz excitation. In the latest research, Novelli et al presented a narrowband THz pump/THz probe experiment using a free electron laser to induce strong anisotropy of liquid water through librational excitation 33 . A very large third-order response of liquid water at 12.3 THz was observed, which was three to five orders of magnitude larger than the previously reported values.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast hydrogen bond dynamics of liquid water revealed by terahertz-induced transient birefringence

et al. 2020

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The fundamental properties of water molecules, such as their molecular polarizability, have not yet been clarified. The hydrogen bond network is generally considered to play an important role in the thermodynamic properties of water. The terahertz (THz) Kerr effect technique, as a novel tool, is expected to be useful in exploring the low-frequency molecular dynamics of liquid water. Here, we use an intense and ultrabroadband THz pulse (peak electric field strength of 14.9 MV/cm, centre frequency of 3.9 THz, and bandwidth of 1-10 THz) to resonantly excite intermolecular modes of liquid water. Bipolar THz field-induced transient birefringence signals are observed in a free-flowing water film. We propose a hydrogen bond harmonic oscillator model associated with the dielectric susceptibility and combine it with the Lorentz dynamic equation to investigate the intermolecular structure and dynamics of liquid water. We mainly decompose the bipolar signals into a positive signal caused by hydrogen bond stretching vibration and a negative signal caused by hydrogen bond bending vibration, indicating that the polarizability perturbation of water presents competing contributions under bending and stretching conditions. A Kerr coefficient equation related to the intermolecular modes of water is established. The ultrafast intermolecular hydrogen bond dynamics of water revealed by an ultrabroadband THz pump pulse can provide further insights into the transient structure of liquid water corresponding to the pertinent modes.

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Strong Anisotropy in Liquid Water upon Librational Excitation Using Terahertz Laser Fields

Cited by 23 publications

References 111 publications

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

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

Ultrafast hydrogen bond dynamics of liquid water revealed by terahertz-induced transient birefringence

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