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TECH SPACE
Watching bonds form using femtosecond X-ray liquidography
by Staff Writers
Daejeon, Korea (SPX) Feb 27, 2015


a, The photochemical reaction of solutes supplied by a liquid-flowing system is triggered by a femtosecond optical laser pulse. Subsequently, a time-delayed X-ray pulse synchronized with the laser pulse probes the structural dynamics of the reaction. The scattering pattern is detected by a fast two-dimensional charge-coupled device detector as shown at the bottom. We measure time-resolved scattering patterns while varying the time delay between the laser and X-ray pulses. b, By integrating the two-dimensional scattering pattern azimuthally, subtracting solvent contributions, performing a Fourier transform and compensating for the depletion of the initial solute contribution due to photochemical reaction, we obtain one-dimensional RDFs in real space as shown in the plot at the top left. These display the interatomic distances of transient species and products. In this way, Au-Au bond lengths of the [Au(CN)2-]3 complex can be identified with sub-angstrom accuracy, and the time-dependent structural changes of the metal complex can be determined in real time. Image courtesy Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS). For a larger version of this image please go here.

The research team of the Center for Nanomaterials and Chemical Reactions at the Institute for Basic Science (IBS) has successfully visualized the entire process of bond formation in solution by using femtosecond time-resolved X-ray liquidography (femtosecond TRXL) for the first time in the world.

Every researcher's longstanding dream to observe real-time bond formation in chemical reactions has come true. Since this formation takes less than one picosecond, researchers have not been able to visualize the birth of molecules.

The research team has used femtosecond TRXL in order to visualize the formation of a gold trimer complex in real time without being limited by slow diffusion.

They have focused on the process of photoinduced bond formation between gold (Au) atoms dissolved in water. In the ground (S0) state, Au atoms are weakly bound to each other in a bent geometry by van der Waals interactions. On photoexcitation, the S0 state rapidly converts into an excited (S1) state, leading to the formation of covalent Au-Au bonds and bent-to-linear transition.

Then, the S1 state changes to a triplet (T1) state with a time constant of 1.6 picosecond, accompanying further bond contraction by 0.1 A. Later, the T1 state of the trimer transforms to a tetramer on nanosecond time scale, and Au atoms return to their original bent structure.

"By using femtosecond TRXL, we will be able to observe molecular vibration and rotation in the solution phase in real time," says Hyotcherl Ihee, the group leader of the Center for Nanomaterials at IBS, as well as the professor of the Department of Chemistry at Korea Advanced Institute of Science and Technology.


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