Experimental evidence of a liquid-liquid critical point in supercooled water
Data files
Jan 29, 2026 version files 364.54 KB
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main_figure_data_fig2.xlsx
214.42 KB
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main_figure_data_fig3.xlsx
29.55 KB
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main_figure_data_fig4.xlsx
116.81 KB
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README.md
3.76 KB
Abstract
Dataset DOI: 10.5061/dryad.pc866t23j
Description of the data and file structure
Pump-probe measurements using infrared and x-ray laser beams were performed on high-density amorphous (HDA) ice and low-density amorphous (LDA) ice samples. The samples were isochorically heated by the IR laser and then decompressed. The X-ray scattering patterns were measured along the decompression process.
Files and variables
File: main_figure_data_fig2.xlsx
Description: X-ray scattering during the decompression process of HDA at different laser fluences. Wide angle x-ray scattering (WAXS) intensities around the first peak and small angle x-ray scattering (SAXS) intensities at different delays after laser pumping.
(A) 3 J/cm2 WAXS (B) 3 J/cm2 SAXS
(C) 11 J/cm2 WAXS (D) 11 J/cm2 SAXS
(E) 15 J/cm2 WAXS (F) 15 J/cm2 SAXS
(G) 20 J/cm2 WAXS (H) 20 J/cm2 SAXS
Variables
- q in Å-1 unit
- I (q) in arbitrary unit (a. u.)
- After the pump pulse, the scattering intensity changes as a function of time.
- The changes are q-dependent, meaning they reflect structural rearrangements at specific length scales.
- Early times (13–50 ns) already differ from the “before pump” curve represents the system responds very fast.
- Later times (200 ns–1 µs) show partial relaxation or evolution toward a new state.
- The pump excites the system (laser, thermal, electronic, etc.).
- This causes short-range structural changes that modify how the sample scatters.
- The persistence of changes up to 1 µs suggests non-instantaneous recovery.
File: main_figure_data_fig3.xlsx
Description: Determination of temperature reached after laser heating of LDA.
(A) The shift of the ice Bragg peaks after crystallization as a function of laser fluence. Mean values and standard deviations from approximately 10 measurements.
(B_data) Laser energy versus the average of estimated temperatures.
(B_fit) The power-law fit results for the average temperature data shown in Fig. 3B.
Variables
- Pump laser power in J/cm2 unit
- Difference of peak position in Å-1 unit
- Estimated temperature in K unit
- As pump fluence increases, the peak position shifts.
- The shift increases rapidly at low power and then saturates at higher power.
- The decreasing standard deviation at higher fluence suggests more reproducible structural response.
- The peak shift indicates a change in characteristic spacing (e.g., lattice spacing, intermolecular distance).
- Saturation implies:
- A maximum achievable structural distortion, or
- A phase/state that cannot be further driven by higher fluence.
This figure supports the idea that the response is nonlinear but bounded.
File: main_figure_data_fig4.xlsx
Description: X-ray scattering during the densification and decompression processes of LDA at different laser fluences.
(A) 4 J/cm2 WAXS (B) 11 J/cm2 WAXS (C) 15 J/cm2 WAXS
(D) selected scattering shots from 15 J/cm2
(E) LDA 15 J/cm2 25 ns WAXS, HDA 15 J/cm2 200 ns WAXS
Variables
- q in Å-1 unit
- I (q) in arbitrary unit (a. u.)
- Overall intensities are higher than Fig. 2 (note the larger baseline values).
- Time-dependent changes are still present, but:
- The relative magnitude
- The relaxation behavior
differ from Fig. 2.
- This corresponds to:
- A different sample
- A different pump fluence
- Or a different experimental condition (temperature, environment, composition)
- Comparing Fig. 2 and Fig. 4 shows how initial structure or excitation strength affects dynamics.
