A T‐Matrix Based Approach to Homogenize Artificial Materials

Zerulla, Benedikt; Venkitakrishnan, Ramakrishna; Beutel, Dominik; Krstić, Marjan; Holzer, Christof; Rockstuhl, Carsten; Fernandez‐Corbaton, Ivan

doi:10.1002/adom.202201564

Cited by 18 publications

(29 citation statements)

References 75 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Therefore, it differs from the effective T-matrix defined in Equation (3) of Ref. [48], which is defined for a three-dimensional lattice and does not depend on the propagation direction of the incident light. For the calculation of the effective material parameters of the MOF, the effective T-matrix from Equation (3) of Ref.…”

Section: Appendix: T-matrix Formalismmentioning

confidence: 90%

“…Indeed, these lines of high absorption can be traced to the excitation of standing wave resonances in the Fabry-Pérot cavity filled with a dispersive material [42]. The modes of the cavity, depicted as colored lines in Figure 6(a), are calculated based on the effective refractive index of the MOF, which is computed with the homogenization method from [48]. For the calculation of the cavity modes, the chirality of the MOF is neglected.…”

Section: A Optical Cavity Filled With Uio-67-r-binol Mof Thin Filmmentioning

confidence: 99%

“…The main advantage of our multiscale ansatz is the representation of this complexity by the T-matrix. From the rotationally averaged T-matrix, the effective material parameters can be extracted that describe the optical properties of the material at the macroscopic scale [48]. The material properties that matter to the problem at hand are the permittivity and chirality.…”

Section: B Metasurface Made From Uio-67-r-binol Mof Cylindersmentioning

confidence: 99%

“…The negative real part of the electric-magnetic coupling term of the T-matrix, −Re(T em ) is proportional to the imaginary part of the chirality. This can be seen by the formulas for the effective parameters in Equation (17) of [48]. The imaginary part of the chirality is the quantity determining the circular dichroism.…”

Section: B Metasurface Made From Uio-67-r-binol Mof Cylindersmentioning

confidence: 99%

“…For the calculation of the effective material parameters of the MOF, the effective T-matrix from Equation (3) of Ref. [48] is used.…”

Section: Appendix: T-matrix Formalismmentioning

confidence: 99%

See 4 more Smart Citations

Exploring Functional Photonic Devices made from a Chiral Metal-Organic Framework Material by a Multiscale Computational Method

Zerulla¹,

Li²,

Beutel³

et al. 2023

Preprint

View full text Add to dashboard Cite

Section: Appendix: T-matrix Formalismmentioning

confidence: 90%

Section: A Optical Cavity Filled With Uio-67-r-binol Mof Thin Filmmentioning

confidence: 99%

Section: B Metasurface Made From Uio-67-r-binol Mof Cylindersmentioning

confidence: 99%

Section: B Metasurface Made From Uio-67-r-binol Mof Cylindersmentioning

confidence: 99%

“…For the calculation of the effective material parameters of the MOF, the effective T-matrix from Equation (3) of Ref. [48] is used.…”

Section: Appendix: T-matrix Formalismmentioning

confidence: 99%

See 3 more Smart Citations

Exploring Functional Photonic Devices made from a Chiral Metal-Organic Framework Material by a Multiscale Computational Method

Zerulla¹,

Li²,

Beutel³

et al. 2023

Preprint

View full text Add to dashboard Cite

Exploring Functional Photonic Devices made from a Chiral Metal–Organic Framework Material by a Multiscale Computational Method

Zerulla

Chun

Beutel

et al. 2023

Adv Funct Materials

Self Cite

View full text Add to dashboard Cite

Electronic circular dichroism is an important optical phenomenon offering insights into chiral molecular materials. On the other hand, metal–organic frameworks (MOFs) are a novel group of crystalline porous thin‐film materials that provide tailor‐made chemical and physical properties by carefully selecting their building units. Combining these two aspects of contemporary material research and integrating chiral molecules into MOFs promises devices with unprecedented functionality. However, considering the nearly unlimited degrees of freedom concerning the choice of materials and the geometrical details of the possibly structured films, urgently it needs to complement advanced experimental methods with equally strong modeling techniques. Most notably, these modeling techniques must cope with the challenge that the material and devices thereof cover size scales from Ångströms to mm. In response to that need, a computational workflow is outlined that seamlessly combines quantum chemical methods to capture the properties of individual molecules with optical simulations to capture the properties of functional devices made from these molecular materials. The focus is on chiral properties and applying work to UiO‐67‐BINOL MOFs, for which experimental results are available to benchmark the results of the simulations and explore the optical properties of cavities and metasurfaces made from that chiral material.

show abstract

A Multi‐Scale Approach to Simulate the Nonlinear Optical Response of Molecular Nanomaterials

Zerulla,

Beutel,

Holzer

et al. 2023

Advanced Materials

Self Cite

View full text Add to dashboard Cite

Nonlinear optics is essential for many recent photonic technologies. Here, a novel multi‐scale approach is introduced to simulate the nonlinear optical response of molecular nanomaterials combining ab initio quantum‐chemical and classical Maxwell‐scattering computations. In this approach, the first hyperpolarizability tensor is computed with time‐dependent density‐functional theory and incorporated into a multi‐scattering formalism that considers the optical interaction between neighboring molecules. Such incorporation is achieved by a novel object: the Hyper‐Transition(T)‐matrix. With this object at hand, the nonlinear optical response from single molecules and also from entire photonic devices can be computed, including the full tensorial and dispersive nature of the optical response of the molecules, as well as the optical interaction between different molecules as, for example, in the lattice of a molecular crystal. To demonstrate the applicability of the novel approach, the generation of a second‐harmonic signal from a thin film of an Urea molecular crystal is computed and compared to more traditional simulations. Furthermore, an optical cavity is designed, which enhances the second‐harmonic response of the molecular film up to more than two orders of magnitude. This approach is highly versatile and accurate and can be the working horse for the future exploration of nonlinear photonic molecular materials in structured photonic environments.

show abstract

A T‐Matrix Based Approach to Homogenize Artificial Materials

Cited by 18 publications

References 75 publications

Exploring Functional Photonic Devices made from a Chiral Metal-Organic Framework Material by a Multiscale Computational Method

Exploring Functional Photonic Devices made from a Chiral Metal-Organic Framework Material by a Multiscale Computational Method

Exploring Functional Photonic Devices made from a Chiral Metal–Organic Framework Material by a Multiscale Computational Method

A Multi‐Scale Approach to Simulate the Nonlinear Optical Response of Molecular Nanomaterials

Contact Info

Product

Resources

About