Tabletop imaging of structural evolutions in chemical reactions

The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using VUV light from a Free Electron Laser [Phys. Rev. Lett. 105, 263002 (2010)]. Here we show that 266 nm ultrashort laser pulses are capable of initiating rich dynamics through multiphoton ionization. With our generally applicable tabletop approach that can be used for other small organic molecules, we have investigated two basic chemical reactions simultaneously: proton migration and C=C bond-breaking, triggered by multiphoton ionization. The experimental results are in excellent agreement with the timescales and relaxation pathways predicted by new and definitively quantitative ab initio trajectory simulations

Isotope Effect in the three Break-up Channels of the Acetylene Cation

International audienc

Coulomb imaging of the concerted and stepwise break up processes of OCS ions in intense femtosecond laser radiation

International audienceWe study the break up of OCS in intense femtosecond laser radiation using the FEMPULS technique to vary the laser pulse duration from 7 fs to 200 fs. Newton and Dalitz plots show the progression of molecular deformation and break up for OCS$^{3+}$ and OCS$^{4+}$. For increasing pulse length, the concerted three body dissociation exhibits increasing bending, and the amount of stepwise dissociation decreases. For the longest pulses however the stepwise process increases again. Both phenomena can be interpreted in terms of the effect of the laser field on lower charge states and the behaviour of a wave packet on a saddle point potential. The experiment illustrates the ability of the Coulomb imaging method to track molecular geometry and dynamics and indicates a new path to laser control of molecular parameters

Tabletop imaging using 266nm femtosecond laser pulses, for characterization of structural evolution in, single molecule, chemical reactions

We have demonstrated a generally applicable tabletop approach utilizing a 266nm femtosecond laser pulse pump, 800nm pulse probe, coupled with Coulomb explosion imaging (CEI). We have investigated two simple chemical reactions in C2H2 + simultaneously: proton transfer and C=C bond-breaking, triggered by multiphoton ionization to excited states. Too and fro proton migration results are in excellent agreement with new ab initio trajectory simulations which predict isomerization timescales and pathways.Peer reviewed: YesNRC publication: Ye

Tabletop imaging of structural evolutions in chemical reactions

The first high-resolution molecular movie of proton migration in the acetylene cation is obtained using a tabletop multiphoton pump-probe approach - an alternative to demanding free-electron-lasers and other VUV light sources when ionizing from the HOMO-1Peer reviewed: YesNRC publication: Ye

Tabletop imaging using 266nm femtosecond laser pulses, for characterization of structural evolution in, single molecule, chemical reactions

We have demonstrated a generally applicable tabletop approach utilizing a 266nm femtosecond laser pulse pump, 800nm pulse probe, coupled with Coulomb explosion imaging (CEI). We have investigated two simple chemical reactions in C2H2 + simultaneously: proton transfer and C=C bond-breaking, triggered by multiphoton ionization to excited states. Too and fro proton migration results are in excellent agreement with new ab initio trajectory simulations which predict isomerization timescales and pathways.Peer reviewed: YesNRC publication: Ye

Tabletop Imaging of Structural Evolutions in Chemical Reactions

The first high-resolution molecular movie of proton migration in the acetylene cation is obtained using a tabletop multiphoton pump-probe approach\u2014an alternative to demanding free-electron-lasers and other VUV light sources when ionizing from the HOMO-1.Peer reviewed: YesNRC publication: Ye

Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation

The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging, we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using vacuum ultraviolet light from a free-electron laser. Here we show that 266 \u2030nm ultrashort laser pulses are capable of initiating rich dynamics through multiphoton ionization. With our generally applicable tabletop approach that can be used for other small organic molecules, we have investigated two basic chemical reactions simultaneously: proton migration and C=C bond breaking, triggered by multiphoton ionization. The experimental results are in excellent agreement with the timescales and relaxation pathways predicted by new and quantitative ab initio trajectory simulations.Peer reviewed: YesNRC publication: Ye