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Ultrafast Structural Dynamics of (EDO-TTF)2X

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Chemistry in Action: Making Molecular Movies with Ultrafast Electron Diffraction and Data Science

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Abstract

In this chapter, I will present two studies on the photoinduced structural dynamics of the crystalline material (EDO-TTF)2X. For context, a general overview of this molecular system will be given. This is followed by a description of the experimental procedure and a discussion of the results from the studies.

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Notes

  1. 1.

    Albert Szent-Györgyi (1893–1986) is a Hungarian biochemist who won the Nobel Prize in Physiology or Medicine in 1937 for his work in vitamin C and the chemistry of cellular respiration [191].

  2. 2.

    ‘Organic’ originally refers to that which is solely derived from living organisms; it has now been generalized to describe chemistry that involves the element carbon, often in association with other nonmetals.

  3. 3.

    This work netted the 2000 Nobel Prize in Chemistry for Alan J. Heeger (1936–present), Alan G. MacDiarmid (1927–2007), and Hideki Shirakawa (1936–present) [186].

  4. 4.

    A molecule is said to be aromatic when it has a flat ring of atoms bound together by an set of overlapping p orbitals.

  5. 5.

    Rudolf E. Peierls (1907–1995) noted in 1954 that one-dimensional periodic arrangements of atoms with delocalized electrons tend to dimerize due to electron–phonon coupling [437].

  6. 6.

    Named for Danish chemist Klaus Bechgaard (1945–2017) and French chemist Jean-Marc Fabre (1943–present) who respectively first synthesized the selenium (TMTSF) and sulfur (TMTTF) derivatives of TMTCF [444].

  7. 7.

    Chalcogens are chemical elements in group 16 of the periodic table, e.g. sulfur and selenium; pnictogens are those in group 15, e.g. phosphorus and antimony.

  8. 8.

    German physicist Paul Drude (1863–1906) studied optical phenomena from the perspective of electromagnetism and introduced a classical model of metals to explain their transport properties [274].

  9. 9.

    Hole-wise, \(\frac {1}{4}\)-filled; each of the two EDO-TTF molecules has two valence electrons and one of the four in total is transferred to the PF6 molecule.

  10. 10.

    The curvature of the EDO-TTF molecule refers to the sum of the dihedral angles of the atom chain O–C–S–C and C=C–S–C; ‘flat’: 1.87∘, ‘nearly flat’: 2.08∘, ‘bent’: 13.42∘.

  11. 11.

    More precisely, nearly flat: + (0.6 ± 0.1)e, flat: + (0.8 ± 0.1)e, and bent: + (0.2 ± 0.1)e [9].

  12. 12.

    Hungarian physicist and Nobel laureate Eugene P. Wigner (1902–1995) predicted in 1934 that a free electron gas would crystallize in the limit of zero kinetic energy [337, 557].

  13. 13.

    American physicist Theodore D. Holstein (1915–1985) [141] introduced in a series of papers [228] an eponymous electron–phonon coupling Hamiltonian that describes electrons hopping around a fixed lattice of local oscillators; British physicist John Hubbard (1931–1980) [454] also introduced around the same time [233] a now-classic Hamiltonian that models a system of hopping electrons that experience short- (on-site) and intermediate- (nearest-neighbour) range Coulomb repulsion.

  14. 14.

    A third CT band (CT3) at 6150 cm−1 (= 0.76 eV), more clearly seen on shoulder of CT1 below 100 K, is assigned to an excitation to a mixture of the (1010) and (2000) states [135].

  15. 15.

    Dutch physicist Hendrik A. Kramers (1894–1952) and German physicist Ralph de L. Kronig (1904–1995) independently showed that the dispersive and absorptive properties of a medium are related from one to another and can be calculated using a set of mathematical equations now known as the Kramers-Kronig relations [306, 308, 515].

  16. 16.

    French engineer Étienne-Louis Malus (1775–1812) discovered that transmission of polarized light through a dichroic material varies as \(\cos ^2(\theta )\), where θ is the polarization angle of the light [100].

  17. 17.

    The R-factor is a measure of agreement between the structure factor values calculated from a crystallographic model and those which are experimentally observed; it is defined as .

  18. 18.

    Named for Wolfgang Pauli (1900–1958) and his eponymous exclusion principle, Pauli paramagnetism refers to the tendency of a ‘metal’ to become weakly magnetized under an applied magnetic field as its free electrons align with the field [13, 181].

  19. 19.

    dmit = dimercaptoisotrithione or 1,3-dithiol-2-thione-4,5-dithiolate, Et = C2H5, and Me = CH3.

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    Lai Chung Liu

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Liu, L.C. (2020). Ultrafast Structural Dynamics of (EDO-TTF)2X. In: Chemistry in Action: Making Molecular Movies with Ultrafast Electron Diffraction and Data Science. Springer Theses. Springer, Cham. https://doi.org/10.1007/978-3-030-54851-3_3

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