Ultrafast Dynamics in the DNA Building Blocks Thymidine and Thymine Initiated By Ionizing Radiation

Understanding how energetic charged particles damage DNA is crucial for improving radiotherapy techniques such as hadron therapy and for the development of new radiosensitizer drugs. In the present study, the damage caused by energetic particles was simulated by measuring the action of extreme ultraviolet (XUV) attosecond pulses on the DNA building blocks thymine and thymidine. This allowed the ultrafast processes triggered by direct ionization to be probed with an optical pulse with a time resolution of a few femtoseconds. By measuring the yields of fragment ions as a function of the delay between the XUV pulse and the probe pulse, a number of transient processes typically lasting 100 femtoseconds or less were observed. These were particularly strong in thymidine which consists of the thymine base attached to a deoxyribose sugar. This dynamics was interpreted as excited states of the cation, formed by the XUV pulse, rapidly decaying via non-adiabatic coupling between electronic states. This provides the first experimental insight into the mechanisms which immediately proceed from the action of ionizing radiation on DNA and provides a basis on which further theoretical and experimental studies can be conducted

Double ionization probed on the attosecond timescale

Double ionization following the absorption of a single photon is one of the most fundamental processes requiring interaction between electrons. Information about this interaction is usually obtained by detecting emitted particles without access to real-time dynamics. Here, attosecond light pulses, electron wave packet interferometry and coincidence techniques are combined to measure electron emission times in double ionization of xenon using single ionization as a clock, providing unique insight into the two-electron ejection mechanism. Access to many-particle dynamics in real time is of fundamental importance for understanding processes induced by electron correlation in atomic, molecular and more complex systems

Probing electron correlation on the attosecond time scale

We present experimental measurements and theoretical calculations of single and double ionization time delays in various noble gases using an interferometric method. The measured delays allow us to extract information on the electron correlation

Correlation-driven sub-3 fs charge migration in ionised adenine

Sudden ionisation of a relatively large molecule can initiate a correlation-driven process dubbed charge migration, where the electron density distribution is expected to rapidly change. Capturing this few-femtosecond/attosecond charge redistribution represents the real-time observation of the electron correlation in the molecule. So far, there has been no experimental evidence of this process. Here we report on a time-resolved study of the correlation-driven charge migration process occurring in the bio-relevant molecule adenine after ionisation by a 15-35 eV attosecond pulse. We find that, the production of intact doubly charged adenine - via a shortly-delayed laser-induced second ionisation event - represents the signature of a charge inflation mechanism resulting from the many-body excitation. This conclusion is supported by first-principles time-dependent simulations. Our findings opens new important perspectives for the control of the molecular reactivity at the electronic timescale

Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine

Sudden ionisation of a relatively large molecule can initiate a correlation-driven process dubbed charge migration, where the electron density distribution is expected to rapidly move along the molecular backbone. Capturing this few-femtosecond or attosecond charge redistribution would represent the real-time observation of electron correlation in a molecule with the enticing prospect of following the energy flow from a single excited electron to the other coupled electrons in the system. Here, we report a time-resolved study of the correlation-driven charge migration process occurring in the nucleic-acid base adenine after ionisation with a 15–35 eV attosecond pulse. We find that the production of intact doubly charged adenine – via a shortly-delayed laser-induced second ionisation event – represents the signature of a charge inflation mechanism resulting from many-body excitation. This conclusion is supported by first-principles time-dependent simulations. These findings may contribute to the control of molecular reactivity at the electronic, few-femtosecond time scale

Analysis of Outcomes in Ischemic vs Nonischemic Cardiomyopathy in Patients With Atrial Fibrillation A Report From the GARFIELD-AF Registry

IMPORTANCE Congestive heart failure (CHF) is commonly associated with nonvalvular atrial fibrillation (AF), and their combination may affect treatment strategies and outcomes