OPEN IN READ APP
JOURNAL ARTICLE

Measurement of electron-electron interactions and correlations using two-dimensional electronic double-quantum coherence spectroscopy

Jeongho Kim, Vanessa M Huxter, Carles Curutchet, Gregory D Scholes
Journal of Physical Chemistry. A 2009 November 5, 113 (44): 12122-33
19817401
A two-dimensional (2D) optical coherent spectroscopy that correlates the double excited electronic states to constituent single excited states is described. The technique, termed two-dimensional double-quantum coherence spectroscopy (2D-DQCS), makes use of multiple, time-ordered ultrashort coherent optical pulses to create double and single quantum coherences over the time intervals between the pulses. The resulting 2D electronic spectra map out the energy correlation between the first excited state and two-photon-allowed double-quantum states. Measurements of organic dye molecules show that the near-resonant energy offset for adding a second electronic excitation to the system relative to the first excitation is on the order of tens of millielectronvolts. Simulations of DQC spectra show that vibronic transitions add rich features to the 2D spectra. The results of quantum chemical calculations on model systems provide insight into the many-body origin of the energy shift measured in the experiment. These results demonstrate the potential of 2D-DQCS for elucidating quantitative information about electron-electron interactions, many-electron wave functions, and electron correlation in electronic excited states and excitons.

Full Text Links

Find Full Text Links for this Article

Discussion

You are not logged in. Sign Up or Log In to join the discussion.

Related Papers

Available on the App Store

Available on the Play Store
Remove bar
Read by QxMD icon Read
19817401
×

Search Tips

Use Boolean operators: AND/OR

diabetic AND foot
diabetes OR diabetic

Exclude a word using the 'minus' sign

Virchow -triad

Use Parentheses

water AND (cup OR glass)

Add an asterisk (*) at end of a word to include word stems

Neuro* will search for Neurology, Neuroscientist, Neurological, and so on

Use quotes to search for an exact phrase

"primary prevention of cancer"
(heart or cardiac or cardio*) AND arrest -"American Heart Association"