Far-field lithography through saturated resonance energy transfer.

A method based on resonance energy transfer in a donor-acceptor pair is proposed for writing three-dimensional features in the far field. The saturation of the energy transfer between the donor-acceptor pair induces a nonlinear intensity response in the radical population. This optical nonlinearity can enable three-dimensional nanofabrication without requiring the use of the ultrafast excitation that is compulsory for non-resonant multiphoton excitation.

Elucidating complex triplet-state dynamics in the model system isopropylthioxanthone.

We introduce techniques for probing the dynamics of triplet states. We employ these tools, along with conventional techniques, to develop a detailed understanding of a complex chemical system: a negative-tone, radical photoresist for multiphoton absorption polymerization in which isopropylthioxanthone (ITX) is the photoinitiator. This work reveals that the same color of light used for the 2-photon excitation of ITX, leading to population of the triplet manifold through intersystem crossing, also depletes this triplet population via linear absorption followed by reverse intersystem crossing (RISC).

Probing Multiphoton Photophysics Using Two-Beam Action Spectroscopy.

Multiphoton absorption (MPA) is an enabling technology for many applications. However, due to the low probability of MPA processes, their accurate characterization remains a challenge. Here we introduce a new technique, two-beam constant emission intensity (2-BCEIn) spectroscopy, that offers substantial advantages over other existing methods that use the generation of optical emission for the characterization of absorptive nonlinearities.

Determination of the contributions of two simultaneous absorption orders using 2-beam action spectroscopy.

The concept of a 2-beam action (2-BA) spectroscopy was recently introduced as a method for determining the order of effective nonlinear absorption in multiphoton photoresists. Here we demonstrate that the 2-BA approach can be extended to any measureable observable generated by linear and/or nonlinear absorption. As an example, 2-beam constant-amplitude photocurrent spectroscopy is used to study absorption of a tightly focused, mode-locked or continuous-wave, 800 nm laser by a GaAsP photodiode.

NLO response of photoswitchable azobenzene-based materials.

The nonlinear optical (NLO) response of three π-conjugated azobenzene (AB) derivatives was investigated under picosecond laser excitation by means of the Z-scan technique to evaluate the effect of an ethynyl-based conjugated spacer on the NLO properties of ABs. All modules possessed large third-order nonlinearity, but unexpectedly it was the less extended AB derivative that exhibited the largest NLO response. This finding has been confirmed by means of DFT calculations and was attributed to a higher cis/trans ratio of the particular AB derivative in its investigated photoequilibrated state.