Infrared Spectroscopy on Equilibrated High-Density Amorphous Ice

Karina, Aigerim; Eklund, Tobias; Tonauer, Christina Maria; Li, Hailong; Loerting, Thomas; Amann‐Winkel, Katrin

doi:10.1021/acs.jpclett.2c02074

Cited by 7 publications

(8 citation statements)

References 56 publications

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“…38 The hydrogen bonds of ice I h is slightly stronger than that of I sd . The average O−O distance between hydrogen-bonded water molecules in ice I h (0.2752 nm at 123 K 39 ) is slightly smaller than that in I sd (0.2755 nm at >120 K 34 ). In the case of the transition from pure I c to I h , the O−H stretching band shifts to a higher wavenumber.…”

Section: Phase Transition With Heatingmentioning

confidence: 77%

“…This indicates that the purity of HDA ice in this sample is higher than that of another sample denoted by the blue line because the wavenumber of the O−H symmetric stretching mode of HDA ice is higher than that of LDA ice. 34 The large surface area caused by pores and cracks might affect the formation of pure HDA ice to defuse tension from the distorted structure of HDA ice. 43…”

Section: Effects Of Depositionmentioning

confidence: 99%

“…The wavenumber of the O−H symmetric stretching mode gradually decreases from 23 to 95 K. This indicates that the transition from HDA to LDA ice begins at around 23 K. The O−H symmetric stretching mode of LDA ice is lower than that of HDA ice because the hydrogen bond in LDA ice is stronger. 34 HDA ice transforms into LDA ice owing to the relaxation of the collapsed structure. 15 The beginning temperature of the transition from HDA to LDA ice (i.e., 23 K) is close to the temperature of the pore collapse in the porous amorphous solid water (pASW).…”

Section: Phase Transition With Heatingmentioning

confidence: 99%

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Effects of Deposition Temperature on Phase Transition of Amorphous Ice

Kina,

Ono,

Yoshida

et al. 2024

J. Phys. Chem. C

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To investigate the effects of deposition temperature, T d , on the phase transition of amorphous ice with heating, the infrared spectra of ice deposited at temperatures of 6−160 K were measured. From the changing rate of the wavenumber of the O−H symmetric stretching mode with heating, the transition processes from high-density amorphous (HDA) ice to crystalline hexagonal ice I h via low-density amorphous (LDA) ice and ice I c were analyzed. The results show that the structure of the deposited ice depends on T d and is classified into six types: (i) HDA ice at T d < 20 K, (ii) a mixture of HDA and LDA ice at 20 K < T d < 80 K, (iii) LDA ice at 80 K < T d < 130 K, (iv) a mixture of LDA ice and I c at 130 K < T d < 140 K, (v) I c at 140 K < T d < 150 K, and (vi) a mixture of I c and I h at T d > ∼150 K. Furthermore, the processes of the structural transitions from the deposited ice with heating reflect T d . These results have important implications for the chemical evolution processes in interstellar molecular clouds.

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Section: Phase Transition With Heatingmentioning

confidence: 77%

Section: Effects Of Depositionmentioning

confidence: 99%

Section: Phase Transition With Heatingmentioning

confidence: 99%

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Effects of Deposition Temperature on Phase Transition of Amorphous Ice

Kina,

Ono,

Yoshida

et al. 2024

J. Phys. Chem. C

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“…Red and blue colors are results from PIMD and classical MD simulations using the q-TIP4P/F model for water. Experimental values of d OO HB ( T ) in LDA from IR spectroscopy experiments are indicated by black squares (from ref ). (b) Average HOO angle formed between two hydrogen-bonded water molecules, ⟨ θ HOO HB false( T false) ⟩ , as a function of temperature at P = 0.1 MPa.…”

Section: Resultsmentioning

confidence: 99%

The Importance of Nuclear Quantum Effects on the Thermodynamic and Structural Properties of Low-Density Amorphous Ice: A Comparison with Hexagonal Ice

2023

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We study the nuclear quantum effects (NQE) on the thermodynamic properties of low-density amorphous ice (LDA) and hexagonal ice (I h ) at P = 0.1 MPa and T ≥ 25 K. Our results are based on path-integral molecular dynamics (PIMD) and classical MD simulations of H 2 O and D 2 O using the q-TIP4P/F water model. We show that the inclusion of NQE is necessary to reproduce the experimental properties of LDA and ice I h . While MD simulations (no NQE) predict that the density ρ(T) of LDA and ice I h increases monotonically upon cooling, PIMD simulations indicate the presence of a density maximum in LDA and ice I h . MD and PIMD simulations also predict a qualitatively different Tdependence for the thermal expansion coefficient α P (T) and bulk modulus B(T) of both LDA and ice I h . Remarkably, the ρ(T), α P (T), and B(T) of LDA are practically identical to those of ice I h . The origin of the observed NQE is due to the delocalization of the H atoms, which is identical in LDA and ice I h . H atoms delocalize considerably (over a distance ≈ 20−25% of the OH covalent-bond length) and anisotropically (preferentially perpendicular to the OH covalent bond), leading to less linear hydrogen bonds HB (larger HOO angles and longer OO separations) than observed in classical MD simulations.

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“…Instead of a powdered sample, we use a compact, free-standing piece of ice, which is 10 times thinner than that in the previous study . We now observe a previously hidden heterodyne signal in a one-component system, which allows us to shed light on the nucleation and growth process during the phase transition from HDA to LDA. ,− …”

mentioning

confidence: 83%

Intrinsic Dynamics of Amorphous Ice Revealed by a Heterodyne Signal in X-ray Photon Correlation Spectroscopy Experiments

Li,

Ladd-Parada,

Karina

et al. 2023

J. Phys. Chem. Lett.

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Unraveling the mechanism of water’s glass transition and the interconnection between amorphous ices and liquid water plays an important role in our overall understanding of water. X-ray photon correlation spectroscopy (XPCS) experiments were conducted to study the dynamics and the complex interplay between the hypothesized glass transition in high-density amorphous ice (HDA) and the subsequent transition to low-density amorphous ice (LDA). Our XPCS experiments demonstrate that a heterodyne signal appears in the correlation function. Such a signal is known to originate from the interplay of a static component and a dynamic component. Quantitative analysis was performed on this heterodyne signal to extract the intrinsic dynamics of amorphous ice during the HDA–LDA transition. An angular dependence indicates non-isotropic, heterogeneous dynamics in the sample. Using the Stokes–Einstein relation to extract diffusion coefficients, the data are consistent with the scenario of static LDA islands floating within a diffusive matrix of high-density liquid water.

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Infrared Spectroscopy on Equilibrated High-Density Amorphous Ice

Cited by 7 publications

References 56 publications

Effects of Deposition Temperature on Phase Transition of Amorphous Ice

Effects of Deposition Temperature on Phase Transition of Amorphous Ice

The Importance of Nuclear Quantum Effects on the Thermodynamic and Structural Properties of Low-Density Amorphous Ice: A Comparison with Hexagonal Ice

Intrinsic Dynamics of Amorphous Ice Revealed by a Heterodyne Signal in X-ray Photon Correlation Spectroscopy Experiments

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