Properties of Resonant Interatomic Coulombic Decay in Ne Dimers

Aoto, Tomohiro; Ito, Kenji; Hikosaka, Y.; Shigemasa, E.; Penent, F.; Lablanquie, P.

doi:10.1103/physrevlett.97.243401

Cited by 84 publications

(44 citation statements)

References 27 publications

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“…Other intermolecular or interatomic ionization mechanisms, for example electron impact ionization after photoionization, are typically one order of magnitude less probable. It occurs after ionization of an appropriate atomic shell (that is, an inner valence shell) [11][12][13] , after excitation [14][15][16] and especially as a terminal step after Auger decay [17][18][19] and therefore after ionization of the cluster compound with high-energy particles or photons. Most recently the main characteristic of ICD, ionization of nearest-neighbour molecules by energy transfer, was also seen in the core-hole relaxation of OH − dissolved in water 20 .…”

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Ultrafast energy transfer between water molecules

et al. 2010

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At the transition from the gas to the liquid phase of water, a wealth of new phenomena emerge, which are absent for isolated H 2 O molecules. Many of those are important for the existence of life, for astrophysics and atmospheric science. In particular, the response to electronic excitation changes completely as more degrees of freedom become available. Here we report the direct observation of an ultrafast transfer of energy across the hydrogen bridge in (H 2 O) 2 (a so-called water dimer). This intermolecular coulombic decay leads to an ejection of a low-energy electron from the molecular neighbour of the initially excited molecule. We observe that this decay is faster than the proton transfer that is usually a prominent pathway in the case of electronic excitation of small water clusters and leads to dissociation of the water dimer into two H 2 O , the observed decay channel might contribute as a source of electrons that can cause radiation damage in biological matter.The water molecule is, as a triatomic molecule, rather simple in structure and its geometry is well known. In contrast to that, the interplay of compounds of water molecules or other atoms and molecules with water, for example in a solution, is very rich and far from being fully understood. At the very onset of condensation when two water molecules are combined to form a water dimer a new dimension of complexity arises: electronic excitation of this complex spawns nuclear dynamics leading to fragmentation into a protonated fragment (that is, H 3 O + ) and an OH group 3,4 . For this fragmentation, first a proton migrates from one of the molecules to its neighbour, usually along a distance that is larger than the bond lengths found in the water molecule itself. Such fragmentation dynamics are characteristic for larger clusters, as well 5 . Typical mass spectra of fragments of water droplets show a break-up into protonated cluster fragments (H 2 O) n H + of different sizes and into OH groups. A reason for this is the absence of direct transitions within the Franck-Condon region to break-up channels that do not involve proton migration [6][7][8] . Furthermore, the migration itself is highly efficient and occurs on a timescale of <60 fs (ref. 9).The response of condensed water to electronic excitation has far-reaching consequences for biological systems. Radiation damage to cells naturally depends sensitively on the routes by which energy deposited into the cells is finally distributed and which fragmentation and de-excitation pathways are favoured. Experiments have shown that the constituents of DNA are highly vulnerable to low-energy electrons 1 . These studies revealed that not only does primary ionization by high-energy particles or photons cause damage, but also that low-energy electrons in particular break-up biomolecules efficiently 2 . ). The red oval shows an internuclear distance of 2.9 Å with a corresponding KER of 4.9 eV after the photo reaction. b,c, The process observed in this experiment: an electron from the inner valence shell of one...

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Ultrafast energy transfer between water molecules

et al. 2010

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“…Since that time a wealth of experimental and theoretical studies have shown that ICD is a rather common decay path in nature, as it occurs almost everywhere in loosely bound matter. It has been proven to occur after a manifold of initial excitation schemes such as innervalence shell ionization, after Auger cascades [4,5], resonant excitation [6,7], shakeup ionization [8] and resonant Auger decay. ICD has also been observed in many systems as rare gas clusters [9], even on surfaces [10] and small water droplets [11,12].…”

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Evolution of Interatomic Coulombic Decay in the Time Domain

et al. 2013

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During the last 15 years a novel decay mechanism of excited atoms has been discovered and investigated. This so called "Interatomic Coulombic Decay" (ICD) involves the chemical environment of the electronically excited atom: the excitation energy is transferred (in many cases over long distances) to a neighbor of the initially excited particle usually ionizing that neighbor. It turned out that ICD is a very common decay route in nature as it occurs across van-der-Waals and hydrogen bonds. The time evolution of ICD is predicted to be highly complex, as its efficiency strongly depends on the distance of the atoms involved and this distance typically changes during the decay. Here we present the first direct measurement of the temporal evolution of ICD using a novel experimental approach.In 1997 Cederbaum and coworkers realized that the presence of loosely bound atomic or molecular neighbors opens a new relaxation pathway to an electronically excited atom or molecule. In the decay mechanism they proposed -termed Intermolecular Coulombic Decay (ICD) -the excited particle relaxes efficiently by transferring its excitation energy to a neighboring atom or molecule [1]. As a consequence the atom or molecule receiving the energy emits an electron of low kinetic energy. The occurrence of ICD was proven in experiments in the mid 2000s by means of electron spectroscopy [2] and multi-coincidence techniques [3]. Since that time a wealth of experimental and theoretical studies have shown that ICD is a rather common decay path in nature, as it occurs almost everywhere in loosely bound matter. It has been proven to occur after a manifold of initial excitation schemes such as innervalence shell ionization, after Auger cascades [4,5], resonant excitation [6,7], shakeup ionization [8] and resonant Auger decay. ICD has also been observed in many systems as rare gas clusters [9], even on surfaces [10] and small water droplets [11,12]. The latter suggested that ICD might play a role in radiation damage of living tissue [13], as it creates low energy electrons, which are known to be genotoxic [14,15]. More recently that scenario was reversed as it was suggested to employ ICD in treatment of tagged malignant cells [16]. Apart from these potential applications the elementary process of ICD is under investigation, as the decay is predicted to have a highly complex temporal * Electronic address: jahnke@atom.uni-frankfurt.de behavior. The efficiency and thus the decay times of ICD depend strongly on the size of the system, i.e. the number of neighboring particles and the distance between them and the excited particle. However, even for most simple possible model systems consisting of only two atoms the temporal evolution of the decay is non-trivial and predicted theoretically to exhibit exciting physics [17]: as ICD happens on a timescale that is fast compared to relaxation via photon emission, but comparable to the typical times of nuclear motion in the system, the dynamics of the decay is complicated and so far only theoretically explored...

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“…Upon core level photoionization, the created hole state undergoes ultrafast relaxation due to energy transfer to a neighbouring atom, and emits an electron from that neighbouring site. [11][12][13] The first successful attempt to measure non-protonated (H 2 O) n + (2≤n≤10) clusters was by Shinohara et al 14 who used the argon emission lines at 11.62 and 11.83 eV to ionize a mixed argon/water molecular beam. Since protonated water clusters and mixed (H 2 O) n Ar m + clusters were also observed, it was suggested that electron emission and Ar evaporation from these clusters led to the formation of the non-protonated species.…”

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Ionization of Water Clusters Mediated by Exciton Energy Transfer from Argon Clusters

Golan

Ahmed

2012

J. Phys. Chem. Lett.

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The exciton energy deposited in an argon cluster (Ar n , ⟨n = 20⟩) using VUV radiation is transferred to softly ionize doped water clusters ((H2O) n , n = 1–9), leading to the formation of nonfragmented clusters. Following the initial excitation, electronic energy is channeled to ionize the doped water cluster while evaporating the Ar shell, allowing identification of fragmented and complete water cluster ions. Examination of the photoionization efficiency curve shows that cluster evaporation from excitons located above 12.6 eV is not enough to cool the energized water cluster ion and leads to their dissociation to (H2O) n−2H+ (protonated) clusters.

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Properties of Resonant Interatomic Coulombic Decay in Ne Dimers

Cited by 84 publications

References 27 publications

Ultrafast energy transfer between water molecules

Ultrafast energy transfer between water molecules

Evolution of Interatomic Coulombic Decay in the Time Domain

Ionization of Water Clusters Mediated by Exciton Energy Transfer from Argon Clusters

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