Experimental evidence for ultrafast intermolecular relaxation processes in hydrated biomolecules

Spatial separation of pyrrole and pyrrole-water clusters

“…In a bottom-up approach, spectroscopic and theoretical investigations were performed for micro-solvated clusters to get fundamental insights into their photophysical and photochemical properties [7,10,11]. Recently performed experiments have provided evidence for ultrafast intermolecular relaxation processes in electronicallyexcited microsolvated tetrahydrofuran-water [12] and indole-water [13] clusters. This reflects one of the proposed efficient mechanisms for radiation damage processes of biomolecules via auto-ionization caused by secondary electrons [14].…”

Damaging Intermolecular Energy and Proton Transfer Processes in Alpha‐Particle‐Irradiated Hydrogen‐Bonded Systems

“…Ionic states with inner-valence vacancies deserve special attention owing to the possibility of intermolecular Coulombic decay (ICD), [5][6][7][8] an onlocal electronic decay process of as ystem embedded in an environment. [13,14,17] While most of the existing experiments have been performed using electromagnetic radiation, ICD was also identified after collisions with charged particles such as electrons, [13,[18][19][20] alpha particles, [21][22][23] and heavy ions. [13,14,17] While most of the existing experiments have been performed using electromagnetic radiation, ICD was also identified after collisions with charged particles such as electrons, [13,[18][19][20] alpha particles, [21][22][23] and heavy ions.…”

“…Like in ICD,s uch double ionization will be followed by Coulomb explosion of the C 2 H 2 + fragments.A lthough ICD and SI can hardly be separated unambiguously,w eb elieve that the latter is only am inor channel here.O ur belief is partially based on the estimates made in the recent electron impact ionization experiments [13,19] indicating that the SI Figure 1. Like in ICD,s uch double ionization will be followed by Coulomb explosion of the C 2 H 2 + fragments.A lthough ICD and SI can hardly be separated unambiguously,w eb elieve that the latter is only am inor channel here.O ur belief is partially based on the estimates made in the recent electron impact ionization experiments [13,19] indicating that the SI Figure 1.…”

“…Ionic states with inner-valence vacancies deserve special attention owing to the possibility of intermolecular Coulombic decay (ICD), [5][6][7][8] an onlocal electronic decay process of as ystem embedded in an environment. [9,10] Since ICD may happen between biologically relevant molecules, [11] in biomolecule-water pairs, [12,13] or between two water monomers, [14,15] it contributes to both direct and indirect damaging events.Indeed, through ICD,the initially deposited energy is converted into ap roduction of al ow energy electron and two cationic species [16] among which water cations cause perhaps the biggest concern because of their fast transformation to reactive hydroxyl radicals.I ti sa lso noteworthy that ICD-induced charge separation may lead to bond-breaking Coulomb explosion of energetic fragments. [13,14,17] While most of the existing experiments have been performed using electromagnetic radiation, ICD was also identified after collisions with charged particles such as electrons, [13,[18][19][20] alpha particles, [21][22][23] and heavy ions.…”

“…Thesame delocalized dicationic states can also be created through SI of two different molecular centers in the dimer. Like in ICD,s uch double ionization will be followed by Coulomb explosion of the C 2 H 2 + fragments.A lthough ICD and SI can hardly be separated unambiguously,w eb elieve that the latter is only am inor channel here.O ur belief is partially based on the estimates made in the recent electron impact ionization experiments [13,19] indicating that the SI…”