Investigation of the wavelength dependence (725 -1025 nm) of the threshold for nanosecond optical breakdown in water revealed steps consistent with breakdown initiation by multiphoton ionization, with an initiation energy of about 6.6 eV. This value is considerably smaller than the autoionization threshold of about 9.5 eV, which can be regarded as band gap relevant for avalanche ionization. Breakdown initiation is likely to occur via excitation of a valence band electron into a solvated state, followed by rapid excitation into the conduction band. Theoretical analysis based on these assumptions suggests that the seed electron density required for initiating avalanche ionization drops from 2.5×10 15 cm -3 at 725 nm to 1.1×10 12 cm -3 at 1025 nm. These results demand changes of future breakdown modeling for water including the use of a larger band gap than previously employed, the introduction of an intermediate energy level for initiation, and consideration of the wavelength dependence of seed electron density.

The wavelength dependence of the threshold for femtosecond optical breakdown in water provides information on the interplay of multiphoton, tunneling and avalanche ionization, and is of interest for parameter selection in laser surgery. We measured the bubble threshold from UV to near-IR wavelengths and found a continuous decrease of the irradiance threshold with increasing wavelength λ. Results are compared to the predictions of a numerical model that assumes a bandgap of 9.5 eV and considers the existence of a separate initiation channel via excitation of valence band electrons into a solvated state followed by rapid upconversion into the conduction band. Fits to experimental data yield an electron collision time of ≈ 1 fs, and an estimate for the capacity of the initiation channel. Using that collision time, the breakdown dynamics was explored up to λ = 2 µm. The irradiance threshold first continues to decrease but levels out for wavelengths longer than 1.3 µm. This opens promising perspectives for laser surgery at wavelengths around 1.3 µm and 1.7 µm, which are attractive because of their large penetration depth into scattering tissues.

The dynamics of spherical laser-induced cavitation bubbles in water is investigated by plasma photography, time-resolved shadowgraphs and sensitive single-shot probe beam scattering that portrays the transition from initial nonlinear to late linear oscillations. The frequency of late oscillations yields the bubble's gas content. Numerical simulations with an extended Gilmore model using plasma size as input and oscillation times as fit parameter provide insights into experimentally not accessible bubble parameters and shock wave emission. Model extensions include a term covering the initial shock-driven acceleration of the bubble wall, an automated method determining shock front position and pressure decay and a complete energy balance for the partitioning of absorbed laser energy into vaporization, bubble and shock wave energy and dissipation through viscosity and condensation. These tools are used for analysing a scattering signal covering 102 oscillation cycles from a bubble with 36 μm maximum radius produced by a plasma with 1550 K average temperature. Predicted bubble wall velocities during expansion agree well with experimental data. Upon first collapse, most energy was stored in the compressed liquid around the bubble and radiated away acoustically. The collapsed bubble contained more vapour than gas and had a pressure of 13.5 GPa. The decay of the rebound shock wave pressure with radius r was initially $\mathrm{\ \propto }{r^{ - 1.8}}$ , and energy dissipation at the shock front heated the liquid near the bubble wall to temperatures above the superheat limit. The shock-induced temperature rise reduces damping during late bubble oscillations. Damping in first collapse increases significantly for small bubbles with less than 10 μm radius.

High-resolution imaging techniques capable of detecting identifiable endogenous fluorophores in the eye along with genetic testing will dramatically improve diagnostic capabilities in the ophthalmology clinic and accelerate the development of new treatments for blinding diseases. Two-photon excitation (TPE)-based imaging overcomes the filtering of ultraviolet light by the lens of the human eye and thus can be utilized to discover defects in vitamin A metabolism during the regeneration of the visual pigments required for the detection of light. Combining TPE with fluorescence lifetime imaging (FLIM) and spectral analyses offers the potential of detecting diseases of the retina at earlier stages before irreversible structural damage has occurred. The main barriers to realizing the benefits of TPE for imaging the human retina arise from concerns about the high light exposure typically needed for informative TPE imaging and the requirement to correlate the ensuing data with different states of health and disease. To overcome these hurdles, we improved TPE efficiency by controlling temporal properties of the excitation light and employed phasor analyses to FLIM and spectral data in mouse models of retinal diseases. Modeling of retinal photodamage revealed that plasma-mediated effects do not play a role and that melanin-related thermal effects are mitigated by reducing pulse repetition frequency. By using noninvasive TPE imaging we identified molecular components of individual granules in the retinal pigment epithelium and present their analytical characteristics.