Login / Signup

A localized view on molecular dissociation via electron-ion partial covariance.

Felix AllumValerija MusicLudger InhesterRebecca BollBenjamin ErkPhilipp SchmidtThomas M BaumannGünter BrennerMichael BurtPhilipp V DemekhinSimon DörnerArno EhresmannAndreas GallerPatrik GrychtolDavid HeathcoteDenis KarginMats LarssonJason W L LeeZheng LiBastian ManschwetusLutz MarderRobert MasonMichael MeyerHuda OttoChristopher PassowRudolf PietschnigDaniel RammKaja SchubertLucas SchwobRichard D ThomasClaire VallanceIgor VidanovićClemens von Korff SchmisingRené WagnerPeter WalterVitali ZhaunerchykDaniel RollesSadia BariMark BrouardMarkus Ilchen
Published in: Communications chemistry (2022)
Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of the prototypical chiral molecule 1-iodo-2-methylbutane, probed by extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we employ electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d 3/2 and 4d 5/2 atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site.
Keyphrases
  • electron transfer
  • solar cells
  • electron microscopy
  • single molecule
  • high resolution
  • density functional theory
  • transcription factor
  • quantum dots
  • binding protein
  • molecular dynamics
  • energy transfer