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000598130 1001_ $$0P:(DE-H253)PIP1007576$$aKurta, Ruslan$$b0$$eCorresponding author
000598130 245__ $$aExploring fingerprints of ultrafast structural dynamics in molecular solutions with an X-ray laser
000598130 260__ $$aCambridge$$bRSC Publ.$$c2023
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000598130 520__ $$aWe apply ultrashort X-ray laser pulses to track optically excited structural dynamics of [Ir$_2$(dimen)$_4$]$^{2+}$ molecules in solution. In our exploratory study we determine angular correlations in the scattered X-rays, which comprise a complex fingerprint of the ultrafast dynamics. Model-assisted analysis of the experimental correlation data allows us to elucidate various aspects of the photoinduced changes in the excited molecular ensembles. We unambiguously identify that in our experiment the photoinduced transition dipole moments in [Ir$_2$(dimen)$_4$]$^{2+}$ molecules are oriented perpendicular to the Ir–Ir bond. The analysis also shows that the ground state conformer of [Ir$_2$(dimen)$_4$]$^{2+}$ with a larger Ir–Ir distance is mostly responsible for the formation of the excited state. We also reveal that the ensemble of solute molecules can be characterized with a substantial structural heterogeneity due to solvent influence. The proposed X-ray correlation approach offers an alternative path for studies of ultrafast structural dynamics of molecular ensembles in the liquid and gas phases.
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000598130 7001_ $$avan Driel, Tim B.$$b1
000598130 7001_ $$aDohn, Asmus O.$$b2
000598130 7001_ $$0P:(DE-H253)PIP1092139$$aBerberich, Tim$$b3
000598130 7001_ $$aNelson, Silke$$b4
000598130 7001_ $$0P:(DE-H253)PIP1014884$$aZaluzhnyy, Ivan A.$$b5
000598130 7001_ $$0P:(DE-H253)PIP1023113$$aMukharamova, Nastasia$$b6
000598130 7001_ $$aLapkin, Dmitry$$b7
000598130 7001_ $$0P:(DE-H253)PIP1081580$$aZederkof, Diana$$b8
000598130 7001_ $$aSeaberg, Matthew$$b9
000598130 7001_ $$aPedersen, Kasper S.$$b10
000598130 7001_ $$00000-0002-5580-7851$$aKjær, Kasper S.$$b11
000598130 7001_ $$aRippy, Geoffery Ian$$b12
000598130 7001_ $$aBiasin, Elisa$$b13
000598130 7001_ $$aMøller, Klaus B.$$b14
000598130 7001_ $$0P:(DE-H253)PIP1028523$$aGelisio, Luca$$b15
000598130 7001_ $$aHaldrup, Kristoffer$$b16
000598130 7001_ $$0P:(DE-H253)PIP1003481$$aVartanyants, Ivan A.$$b17
000598130 7001_ $$0P:(DE-H253)PIP1007352$$aNielsen, Martin Meedom$$b18$$eCorresponding author
000598130 773__ $$0PERI:(DE-600)1476244-4$$a10.1039/D3CP01257C$$gVol. 25, no. 35, p. 23417 - 23434$$n35$$p23417 - 23434$$tPhysical chemistry, chemical physics$$v25$$x1463-9076$$y2023
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