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How are Heterogeneous Nucleation Rate Observations Influenced by Instrument Resolution?
Jiahui You1, Ke Yuan1, Nikhil Rampal2
1Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.
ACS Applied Materials & Interfaces
|March 10, 2025
Summary
Instrument resolution significantly affects measured nucleation rates. This study shows how to correct for resolution limits to find intrinsic nucleation parameters, crucial for understanding material formation.
Area of Science:
- Materials Science
- Physical Chemistry
- Chemical Engineering
Background:
- Heterogeneous nucleation rate measurements are vital for understanding material formation processes.
- Small nuclei (few nanometers) are often below the detection limit of experimental techniques.
- Finite instrument resolution complicates capturing early-stage nucleation and density evolution.
Purpose of the Study:
- To demonstrate the impact of instrument resolution on observed nucleation densities.
- To compare numerical modeling results with experimental data for nucleation rates.
- To evaluate the influence of resolution on classical nucleation theory (CNT) parameters.
Main Methods:
- Implemented heterogeneous nucleation in a pore-scale reactive transport model.
- Utilized classical nucleation theory (CNT) for modeling.
- Applied artificial resolution limits (15-500 nm) to simulated nuclei counts.
- Compared modeling results with X-ray nanotomography (XnT) experimental data.
Main Results:
- Instrument resolution significantly impacts apparent prefactor and interfacial energy values in CNT.
- Both apparent prefactor and interfacial energy decrease as instrument resolution decreases.
- Unexpected deviations in interfacial energy were observed due to resolution limits.
Conclusions:
- The study provides a method to correct nucleation rates affected by instrument resolution.
- This approach enables the derivation of intrinsic CNT parameters for prefactor and interfacial energy.
- Understanding resolution effects is critical for accurate nucleation studies.
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