Giant intrinsic circular dichroism of prolinol-derived squaraine thin films

Schulz, Matthias; Zablocki, Jennifer; Abdullaeva, Oliya S.; Brück, Stefanie; Balzer, Frank; Lützen, Arne; Arteaga, Oriol; Schiek, Manuela

doi:10.1038/s41467-018-04811-7

Cited by 86 publications

(134 citation statements)

References 59 publications

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“…The CD spectrum is conservative, meaning that the spectral integral over the CD signal including the wider side peaks approaches zero. This is indicative for an excitonic CD‐response further supporting the idea of supramolecular aggregation within the thin films . Most importantly, the excitonic coupling was not disrupted by intermixing with the fullerene acceptor.…”

Section: Resultssupporting

confidence: 69%

“…We quantified the circular dichroic properties by Mueller matrix ellipsometry of the active layer thin films. Complete exemplary differential Mueller matrices are plotted in Figures S2–S4 in the Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

“…Only very recently, we discovered that the CD response can be greatly enhanced by supramolecular aggregation in chiral squaraine thin films due to the nature of its excitonic coupling . Importantly, the excitonic interactions are not disrupted in a BHJ blend allowing photovoltaic device operation under short circuit conditions without external power supply.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Chiral Excitonic Organic Photodiodes for Direct Detection of Circular Polarized Light

Schulz

Balzer

Scheunemann

et al. 2019

Adv Funct Materials

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105

108

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A facile route to soft matter self-powered bulk heterojunction photodiode detectors sensitive to the circular polarization state of light is shown based on the intrinsic excitonic circular dichroism of the photoactive layer blend. As light detecting materials, enantiopure semiconducting small molecular squaraine derivates of opposite handedness are employed. Via Mueller matrix ellipsometry, the circular dichroism is proven to be of H-type excitonic nature and not originating from mesoscopic structural ordering. Within the green spectral range, the photodiodes convert circular polarized light into a handedness-dependent photocurrent with a maximum dissymmetry factor of ±0.1 corresponding to 5% overall efficiency for the polarization discrimination under short circuit conditions. On the basis of transfer matrix optical simulations, it is rationalized that the optical dissymmetry fully translates into a photocurrent dissymmetry for ease of device design. Thereby, the photodiode's ability to efficiently distinguish between left and right circularly polarized light without the use of external optical elements and voltage bias is demonstrated. This allows a straightforward and sustainable future design of flexible, lightweight, and compact integrated platforms for chiroptical imaging and sensing.

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Section: Resultssupporting

confidence: 69%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Chiral Excitonic Organic Photodiodes for Direct Detection of Circular Polarized Light

Schulz

Balzer

Scheunemann

et al. 2019

Adv Funct Materials

Self Cite

105

108

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“…From symmetry considerations, we have used a valid method based on measurements with sample illumination from the metastructures side (Front-F) or from the substrate side (Back-B) [29,30]. This allows, for example, to discern the different contributions of the system to the circular differential extinction [26,31]. The sample was mounted on a rotational stage which allows changing the in-plane orientation of the sample.…”

Section: Resultsmentioning

confidence: 99%

“…(1) is a valid approximation in the range of values of CDE that we are studying. The real values of the CDE can be extracted from the differential Mueller matrix elements [31,[35][36][37]. It should be mentioned that the sources of the optical anisotropy are the preferential in plane ordering of the structures in the array configuration, as well as effects to the overlapping dimer.…”

Section: Resultsmentioning

confidence: 99%

Mueller matrix study of the dichroism in nanorods dimers: rod separation effects

Dios¹,

Jiménez²,

García³

et al. 2019

Opt. Express

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We have studied the optical response of chiral metastructures composed of a disordered array of couples of plasmonic Au nanorods helically piled along the vertical direction. The fabrication is based on the use of multiaxial and multimaterial evaporation of the different metastructure building blocks through nanohole masks. From the analysis of the Mueller Matrix elements of the system, obtained both experimentally and from dedicated numerical simulations in forward and backward illumination conditions, we have been able to determine the linear and circular dichroic response of the system, as well as to sort out the optical anisotropy and intrinsic circular dichroism contributions to the circular differential extinction. We have also analyzed the dependence of the optical properties as a function of the angle between the rods and of the thickness of the dielectric separator. The study of quasiplanar as well as three-dimensional structures allows unraveling the role played by interactions between the constituting building blocks and, in particular, the distance between rods. We have experimentally and theoretically observed a decrease of the circular dichroic contribution and a change of the optical anisotropic contribution when the structures evolve from non-planar to planar.

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Broadband Enhanced Chirality with Tunable Response in Hybrid Plasmonic Helical Metamaterials

Kılıç

Hilfiker

Ruder

et al. 2021

Adv Funct Materials

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Designing broadband enhanced chirality is of strong interest to the emerging fields of chiral chemistry and sensing, or to control the spin orbital momentum of photons in recently introduced nanophotonic chiral quantum and classical optical applications. However, chiral light‐matter interactions have an extremely weak nature, are difficult to control and enhance, and cannot be made tunable or broadband. In addition, planar ultrathin nanophotonic structures to achieve strong, broadband, and tunable chirality at the technologically important visible to ultraviolet spectrum still remain elusive. Here, these important problems are tackled by experimentally demonstrating and theoretically verifying spectrally tunable, extremely large, and broadband chiroptical response by nanohelical metamaterials. The reported new designs of all‐dielectric and dielectric‐metallic (hybrid) plasmonic metamaterials permit the largest and broadest ever measured chiral Kuhn's dissymmetry factor achieved by a large‐scale nanophotonic structure. In addition, the strong circular dichroism of the presented bottom‐up fabricated optical metamaterials can be tuned by varying their dimensions and proportions between their dielectric and plasmonic helical subsections. The currently demonstrated ultrathin optical metamaterials are expected to provide a substantial boost to the developing field of chiroptics leading to significantly enhanced and broadband chiral light‐matter interactions at the nanoscale.

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Giant intrinsic circular dichroism of prolinol-derived squaraine thin films

Cited by 86 publications

References 59 publications

Chiral Excitonic Organic Photodiodes for Direct Detection of Circular Polarized Light

Chiral Excitonic Organic Photodiodes for Direct Detection of Circular Polarized Light

Mueller matrix study of the dichroism in nanorods dimers: rod separation effects

Broadband Enhanced Chirality with Tunable Response in Hybrid Plasmonic Helical Metamaterials

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