Abstract
Magneto-electric (M-E) response at the molecular level arises from the interaction of matter with the electric and magnetic fields of light, and can manifest itself as nonlinear M-E magnetization (MNL) or M-E rectification (PNL). However, there is presently a limited understanding of how molecular material properties impact M-E response. Here we investigate the relationship between M-E nonlinear coefficients and the third-order electric susceptibility, χ(3), finding that MNL is proportional to χxxxx (3) while PNL scales with χzzxx (3) due to a cascaded nonlinearity. By applying a sum-over-states (SOS) expression for the elements of χ(3) to valence-bond charge-transfer (VB-CT) models, we formulate practical guidelines for the design of materials expected to exhibit enhanced M-E properties. On this basis, we predict that many conventional nonlinear optical chromophores with large values of χxxxx (3) may be suitable for generating optical magnetism at low intensities. In the case of M-E rectification, analysis of Λ-shaped, X-shaped, and octupolar VB-CT models suggests that their molecular structures can be tuned to enhance the response by maximizing χzzxx (3). In particular, octupolar molecules with a predominantly CT character ground state and Λ-shaped chromophores with weakly conjugated bridges between donor and acceptor moieties should promote off-diagonal nonlinearity and M-E rectification.
| Original language | English |
|---|---|
| Pages (from-to) | 16491-16500 |
| Number of pages | 10 |
| Journal | Journal of Physical Chemistry C |
| Volume | 121 |
| Issue number | 30 |
| DOIs | |
| Publication status | Published - Aug 3 2017 |
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ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Energy(all)
- Physical and Theoretical Chemistry
- Surfaces, Coatings and Films
Cite this
Molecular Design Principles for Magneto-Electric Materials : All-Electric Susceptibilities Relevant to Optimal Molecular Chromophores. / Lou, Alexander J.T.; Dreyer, Elizabeth F.C.; Rand, Stephen C.; Marks, Tobin J.
In: Journal of Physical Chemistry C, Vol. 121, No. 30, 03.08.2017, p. 16491-16500.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Molecular Design Principles for Magneto-Electric Materials
T2 - All-Electric Susceptibilities Relevant to Optimal Molecular Chromophores
AU - Lou, Alexander J.T.
AU - Dreyer, Elizabeth F.C.
AU - Rand, Stephen C.
AU - Marks, Tobin J
PY - 2017/8/3
Y1 - 2017/8/3
N2 - Magneto-electric (M-E) response at the molecular level arises from the interaction of matter with the electric and magnetic fields of light, and can manifest itself as nonlinear M-E magnetization (MNL) or M-E rectification (PNL). However, there is presently a limited understanding of how molecular material properties impact M-E response. Here we investigate the relationship between M-E nonlinear coefficients and the third-order electric susceptibility, χ(3), finding that MNL is proportional to χxxxx (3) while PNL scales with χzzxx (3) due to a cascaded nonlinearity. By applying a sum-over-states (SOS) expression for the elements of χ(3) to valence-bond charge-transfer (VB-CT) models, we formulate practical guidelines for the design of materials expected to exhibit enhanced M-E properties. On this basis, we predict that many conventional nonlinear optical chromophores with large values of χxxxx (3) may be suitable for generating optical magnetism at low intensities. In the case of M-E rectification, analysis of Λ-shaped, X-shaped, and octupolar VB-CT models suggests that their molecular structures can be tuned to enhance the response by maximizing χzzxx (3). In particular, octupolar molecules with a predominantly CT character ground state and Λ-shaped chromophores with weakly conjugated bridges between donor and acceptor moieties should promote off-diagonal nonlinearity and M-E rectification.
AB - Magneto-electric (M-E) response at the molecular level arises from the interaction of matter with the electric and magnetic fields of light, and can manifest itself as nonlinear M-E magnetization (MNL) or M-E rectification (PNL). However, there is presently a limited understanding of how molecular material properties impact M-E response. Here we investigate the relationship between M-E nonlinear coefficients and the third-order electric susceptibility, χ(3), finding that MNL is proportional to χxxxx (3) while PNL scales with χzzxx (3) due to a cascaded nonlinearity. By applying a sum-over-states (SOS) expression for the elements of χ(3) to valence-bond charge-transfer (VB-CT) models, we formulate practical guidelines for the design of materials expected to exhibit enhanced M-E properties. On this basis, we predict that many conventional nonlinear optical chromophores with large values of χxxxx (3) may be suitable for generating optical magnetism at low intensities. In the case of M-E rectification, analysis of Λ-shaped, X-shaped, and octupolar VB-CT models suggests that their molecular structures can be tuned to enhance the response by maximizing χzzxx (3). In particular, octupolar molecules with a predominantly CT character ground state and Λ-shaped chromophores with weakly conjugated bridges between donor and acceptor moieties should promote off-diagonal nonlinearity and M-E rectification.
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U2 - 10.1021/acs.jpcc.7b04307
DO - 10.1021/acs.jpcc.7b04307
M3 - Article
VL - 121
SP - 16491
EP - 16500
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 30
ER -