Vibrationally excited ultrafast thermodynamic phase transitions at the water/air interface
Literature Information
Kresimir Franjic, R. J. Dwayne Miller
The extraordinary ability of the hydrogen-bond network of water in the condensed phase to thermalize vibrational excitations within several picoseconds, even under supercritical conditions, offers the possibility of creating highly excited thermodynamic states at water surfaces on ultrafast time scales using vibrationally resonant short infrared laser pulses. We experimentally and numerically studied such states created by depositing ∼100 ps long pulses tuned to the 3400 cm−1 O–H stretch vibration at the water/air interface using time-resolved dark-field imaging and time-resolved optical reflectivity. The results are reasonably well described by using a hydrodynamic ablation model under the assumption of impulsive heat deposition. The large thermoelastic stress amplitudes on the order of 1 GPa created within 100 ps by depositing laser pulses with ∼1 J cm−2 fluence were inferred from the numerical simulations. Stresses of this magnitude drive the excited water layer into a very fast expansion resulting in rapid adiabatic cooling and thorough vaporization within a few nanoseconds. The spatial and temporal lengths scales of the ablation plume are nearly ideal for ejecting molecules into the gas phase with minimum perturbation for applications ranging from mass spectrometry and laser surgery to the development of extremely high pressure molecular beams.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.














