Issue 20, 2010

Vibrationally excited ultrafast thermodynamic phase transitions at the water/air interface

Abstract

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.

Graphical abstract: Vibrationally excited ultrafast thermodynamic phase transitions at the water/air interface

Article information

Article type
Paper
Submitted
07 Jan 2010
Accepted
30 Mar 2010
First published
29 Apr 2010

Phys. Chem. Chem. Phys., 2010,12, 5225-5239

Vibrationally excited ultrafast thermodynamic phase transitions at the water/air interface

K. Franjic and R. J. D. Miller, Phys. Chem. Chem. Phys., 2010, 12, 5225 DOI: 10.1039/C000359J

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements