Stability and Symmetry Properties for the General Quadrupolar Interaction between Biaxial Molecules
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1 Stability and Symmetry Properties for the General Quadrupolar Interaction between Biaxial Molecules Epifanio G. Virga SMMM Soft Matter Mathematical Modelling Department of Mathematics University of Pavia, Italy Summary Molecular Biaxiality Interaction Potential Stability Symmetry Ordered Phases Phase Diagrams 1
2 Molecular Biaxiality molecular tensors We think of the molecules as being described by a biaxial tensor that can be decomposed into two traceless, irreducible orthogonal components. q := m m 1 3 I b := e e e e m long molecular axis m m,e,e tensor axes of any molecular polarizability e e 2
3 Interaction Potential The most general quadratic pair-potential was introduced by Straley (1974) V = U 0 { ξq q + γ ( q b + b q ) + λb b } U 0 typical interaction energy ξ, λ, γ dimensionless parameters alternative representation V = U 0 { (λ ξ) + (ξ λ)(m m ) 2 +2(λ + γ)(e e ) 2 + 2(λ γ)(e e ) 2 } Romano (2004), Longa (2005) 3
4 Stability The local stability of the ground state of V, where all three molecular axes are equally oriented, is guaranteed by the following conditions ξ = 1 λ > 0 λ 2γ + 1 > 0 ξ = 1 λ 2γ 1 > 0 λ γ 4
5 symmetric attraction For ξ = 1 and λ = γ 2 the interaction potential V can be given the dispersion form V = U 0 (q + γb) (q + γb ) By superimposing superposition V 1 = U 1 (q + γ 1 b) (q + γ 1 b ) we obtain V 2 = U 2 (q + γ 2 b) (q + γ 2 b ) V = V 1 + V 2 = U 0 {q q + γ (q b + b q ) + λb b } where U 0 = U 1 + U 2, γ = U 1γ 1 + U 2 γ 2 U 1 + U 2, λ = U 1γ U 2 γ 2 2 U 1 + U 2 5
6 The point (γ, λ) lies on the segment joining the points (γ 1, λ 1 ) and (γ 2, λ 2 ), within the dispersion parabola λ > γ 2 λ γ 6
7 potential extrema The stability region can be further characterized by identifying all extrema of V V attains its absolute minimum at (q,b) = (q,b ) (q,b) and (q,b ) have one and the same eigenframe at all extrema of V 7
8 maxima chart strongest attraction The inner triangle, where V attains its maxima when all corresponding molecular axes are mutually orthogonal, is interpreted as the region of strongest molecular attraction. 8
9 mild repulsion The interactions within the stability region that fall outside the dispersion parabola are called mildly repulsive. 9
10 Symmetry V -invariant transformations V = U 0 {ξ q q + γ (q b + q b ) + λ b b } e = e ξ 1 = 9λ + 6γ + 1 γ 1 = 1 3λ + 2γ λ 1 = 1 + λ 2γ e = e ξ 2 = 9λ 6γ + 1 γ 2 = 1 3λ 2γ λ 2 = 1 + λ + 2γ m = m ξ 3 = 1 γ 3 = γ λ 3 = λ Longa(2005), De Matteis (2005) 10
11 rescaling Provided that ξ 0, we can set either ξ = 1 or ξ = 1, depending on whether ξ > 0 or ξ < 0. Correspondingly, the pairs (γ 1, λ 1) and (γ 2, λ 2) become γ 1 = γ 2 = 1 3λ + 2γ 9λ + 6γ λ 2γ 9λ 6γ + 1 λ 1 = 1 + λ 2γ 9λ + 6γ + 1 λ 2 = 1 + λ + 2γ 9λ 6γ
12 symmetry properties We denote by τ 1, τ 2, and τ 3 the scaled transformations. They enjoy the following properties: τ i τ i = 1 τ i τ j τ k = 1 for i j k lines 1 + λ + 2γ = 0, 1 + λ 2γ = 0, and γ = 0 are conjugated parabola λ = γ 2 is self-conjugated De Matteis (2005) 12
13 conjugation charts λ γ ξ = 1 13
14 λ γ ξ = 1 14
15 Ordered Phases order tensors Q := q B := b ensemble average We assume that both Q and B have one and the same eigenframe {e x,e y,e z }. conjugation The conjugations involving q and b are clearly conveyed on the corresponding order tensors. Conjugated macroscopic states are physically equivalent. 15
16 general representation The most general representation of a completely biaxial state employs four order parameters Straley (1974): Q = S (e z e z 13 ) I + T (e x e x e y e y ) B = S ( e z e z 1 3 I ) + T (e x e x e y e y ) 16
17 terminology uniaxial phase occurs whenever both Q and B are uniaxial: T = T = 0 phase biaxiality compatible with cylindrical molecules occurs when S = T = 0 intrinsic biaxiality emerges when T 0. 17
18 order parameter manifold Let (ϑ, ϕ, ψ) be the Euler angles that represent the rotation taking {e x,e y,e z } into {m,e,e }. S = 3 2 cos2 ϑ 1 3 T = sin2 ϑ cos 2ϕ 2 S (1 S) T 1 3 (1 S) S = 3 2 sin2 ϑ cos 2ψ (1 S) S (1 S) T = 1 2 ( 1 + cos 2 ϑ ) cos 2ϕ cos 2ψ 2 cos ϑ sin2ϕ sin2ψ 1 T 1 18
19 Phase Diagrams Within a mean-field approximation the following diagram has recently been established for γ = ISOTROPIC C /β UNIAXIAL C 1 M BIAXIAL Sonnet, Durand & Virga (2003) De Matteis & Virga (2005) λ 19
20 educated guesses Preliminary numerical explorations suggest that within the attractive parabola there are only two qualitatively different phase diagrams. λ γ 20
21 1/β I U B γ M γ For λ constant above the tricritical trajectory 21
22 1/β I U B γ M γ For λ constant below the tricritical trajectory 22
23 Acknowledgements Co-Authors Fulvio Bisi Giovanni De Matteis Georges Durand Chuck Gartland Silvano Romano Riccardo Rosso Institutions Royal Society of London Sothampton-Pavia Collaborative Project Italian MIUR PRIN Grant No
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