The Experts below are selected from a list of 324 Experts worldwide ranked by ideXlab platform

Larry R. Dalton - One of the best experts on this subject based on the ideXlab platform.

  • Organic Electro-Optic Materials: Understanding Structure/Function Relationships Critical to the Optimization of Electro-Optic Activity
    2020
    Co-Authors: Larry R. Dalton, Benjamin C. Olbricht, Philip A. Sullivan, Joshua A. Davies, Bruce H. Robinson, Denise H. Bale, Stephanie J. Benight, Ilya V. Kosilkin, Bruce E. Eichinger
    Abstract:

    Time-dependent density functional theory quantum mechanical and pseudo-atomistic Monte Carlo statistical mechanical computations are used to guide the systematic improvement of organic electro-optic materials. In particular, the dependence of molecular first hyperpolarizability upon dielectric permittivity and optical frequency is defined as is the dependence of electric field poling-induced acentric order on a variety of intermolecular electrostatic interactions. A number of measurement techniques are used to obtain independent test of theoretical predictions of Chromophore order. The conclusion of these studies is that electro-optic activity of even complex materials (multi-Chromophore-containing dendrimers and composite materials containing several types of Chromophores, i.e., binary Chromophore organic glasses) can be predicted from first principles theory. Laser-assisted electric field poling applied to a binary Chromophore organic glass is used to provided an additional test of theory.

  • Systematic Nanoengineering of Soft Matter Organic Electro-optic Materials†
    Chemistry of Materials, 2011
    Co-Authors: Larry R. Dalton, Bruce E. Eichinger, Bruce H. Robinson, Stephanie J. Benight, Ilya V. Kosilkin, Lewis E. Johnson, Daniel B. Knorr, René M. Overney
    Abstract:

    An overview of the development and utilization of organic electro-optic materials is presented with emphasis on the role played by quantum and statistical mechanical calculations in understanding critical structure/function relationships that have guided the improvement of such materials over the past two decades. This review concentrates largely on three classes of organic electro-optic materials prepared by electric field poling of materials near their glass transition temperature: (1) Chromophore/polymer composite materials, (2) dendrimers and polymers containing covalently incorporated Chromophores, and (3) matrix-assisted-poling (MAP) materials where specific spatially anisotropic interactions enhance poling efficiency. In particular, the role of Chromophore shape, restrictions on Chromophore motion associated with covalent bonds, and lattice dimensionality effects are reviewed. The role of device design and auxiliary properties (optical loss, thermal stability, photochemical stability, processabilit...

  • Theory-inspired development of organic electro-optic materials.
    Accounts of Chemical Research, 2010
    Co-Authors: Philip A. Sullivan, Larry R. Dalton
    Abstract:

    Correlated time-dependent density functional theory (TDDFT) quantum mechanical and pseudo-atomistic Monte Carlo (PAMC) statistical mechanical methods have been used to assist in the understanding of and to guide the improvement of organic electro-optic (OEO) materials, prepared by electric field poling of π-electron Chromophore-containing materials near their glass transition temperature. Theoretical treatment of the effects of dielectric permittivity and optical frequency on molecular (Chromophore) first hyperpolarizabilities has been carried out as well as the analysis of the influence of spatially anisotropic intermolecular electrostatic interactions on the poling-induced noncentrosymmetric order of Chromophores. Three classes of OEO materials have been considered in correlated theoretical and experimental investigations: (1) traditional Chromophore/polymer composite materials, (2) Chromophores covalently incorporated into polymers, dendrimers, and dendronized polymers, and (3) recently discovered mate...

  • Laser-Assisted Poling of Binary Chromophore Materials†
    Journal of Physical Chemistry C, 2008
    Co-Authors: Benjamin C. Olbricht, Philip A. Sullivan, Alok A. Mistry, Joshua A. Davies, Bruce E. Eichinger, Bruce H. Robinson, Philip J. Reid, Larry R. Dalton
    Abstract:

    Binary Chromophore systems represent a new and very promising class of organic second-order nonlinear optical (electro-optic) materials, where favorable intermolecular electrostatic interactions lead to significantly enhanced electro-optic coefficients and to other favorable physical properties such as low optical loss and improved stability. In this report, laser-assisted poling of a binary Chromophore system consisting of a photoaddressable Chromophore host (DR-1-co-PMMA) containing a non-photoaddressable guest Chromophore (YLD_124) is demonstrated. A factor of 2.5 enhancement in poling efficiency of the guest Chromophore (compared to simple conventional electric field poling of the same material) is observed when polarized light is used to selectively enhance the order of the host Chromophores. These results further emphasize the importance of favorable intermolecular interactions thought to exist between guest and host Chromophores in binary Chromophore containing materials. Thin-film samples were pro...

  • Advances in Organic Materials for Optical Modulation
    Journal of Lightwave Technology, 2008
    Co-Authors: Philip A. Sullivan, Benjamin C. Olbricht, Larry R. Dalton
    Abstract:

    Theory-inspired design of organic electro-optic materials is explored for three classes of materials: (1) Chromophore/polymer composites; (2) Chromophores covalently incorporated into polymers, dendrimers, and dendronized polymers; and (3) Chromophores doped into Chromophore-containing host materials. Correlated quantum/statistical mechanical calculations are used to quantitatively simulate electro-optic activity for a variety of materials falling into these three classes, elucidating the dependence of electro-optic activity on Chromophore dipole moment, Chromophore shape, covalent bond potentials, and dielectric permittivity. The practical consequence has been the production of materials exhibiting femtosecond response electro-optic activity approaching 600 pm/V at telecommunication wavelengths. Theory also provides insight into minimizing optical loss and maximizing stability.

Zhen Zhen - One of the best experts on this subject based on the ideXlab platform.

  • structure function relationship exploration for enhanced electro optic activity in isophorone based organic nlo Chromophores
    Dyes and Pigments, 2018
    Co-Authors: Hua Zhang, Hongyan Xiao, Shuhui Bo, Huajun Xu, Shujie Chen, Zhen Zhen, Jiahai Wang
    Abstract:

    Abstract Four isophorone-based Chromophores FLD1-FLD4 has been synthesized and investigated based on julolidinyl donors, with modified isophorone-derived bridges and tricyanovinyldihydrofuran or phenyl-trifluoromethyl-tricyanofuran acceptors. The Chromophore FLD3 was modified with a 2-((tert-butyldimethylsilyl)oxy)ethanethiol group covalently attached to the π-conjugate bridge to ensure its all-trans conformation and prevent close packing of molecules, which benefit the macroscopic electro-optic efficiency. The Chromophore FLD3 possesses better thermal stability than Chromophore FLD1 without the isolation group on the bridge. Moreover, density functional theory calculations suggested that the hyperpolarizability (β) value of Chromophore FLD3 is larger than that of Chromophore FLD1. Polymers doped with Chromophore FLD3 have been poled to afford ultrahigh electro-optic coefficient (r33) of 238 pm/V at 1.31 μm, which is nearly 60% higher than that obtained from Chromophore FLD1 and three times higher than that of analogue Chromophores FLD2 and FLD4.

  • Novel Chromophores with excellent electro-optic activity based on double-donor Chromophores by optimizing thiophene bridges
    Dyes and Pigments, 2015
    Co-Authors: Yuhui Yang, Shuhui Bo, Haoran Wang, Zhen Zhen
    Abstract:

    Abstract Three novel nonlinear optical Chromophores based on the same bis( N,N -diethyl)aniline donor have been synthesized and systematically characterized. These Chromophores showed good thermal stability and Chromophore y1 showed the best thermal stability of 249 °C. Besides, compared with the Chromophore (y1) without the substituted group, Chromophores y2 and y3 show better intramolecular charge-transfer absorption. Most importantly, the high molecular hyperpolarizability of these Chromophores can be effectively translated into large electro-optic coefficients. The electro-optic coefficient of poled films containing 25% wt of Chromophores y1–y3 doped in amorphous polycarbonate afforded values of 149, 138 and 157 pm/V at 1310 nm for Chromophores y1–y3 respectively. These results indicated that the double donors of bis( N,N -diethyl)aniline unit can efficiently improve the electron-donating ability and the special structure can reduce intermolecular electrostatic interactions, thus enhancing the macroscopic electro-optic activity. These properties, together with good solubility, suggest the potential use of these Chromophores as advanced materials.

  • using phenoxazine and phenothiazine as electron donors for second order nonlinear optical Chromophore enhanced electro optic activity
    Dyes and Pigments, 2015
    Co-Authors: Haoran Wang, Yuhui Yang, Shuhui Bo, Huajun Xu, Dan Yang, Zhen Zhen
    Abstract:

    Abstract Two novel Chromophores based on the phenoxazine (Chromophore L1) or phenothiazine (Chromophore L2) donor, and tricyanofuran acceptors linked together via thiophene as the bridges have been synthesized and systematically investigated. Cyclic voltammetry measurements showed that Chromophore L1 had smaller energy gap than Chromophore L2 due to the stronger electron-donating ability. Moreover, Density functional theory calculations suggested that the β value of Chromophore L1 is 17% larger than that of Chromophore L2. The doped film containing the Chromophore L1 showed an r 33 value of 49 pm/V at the concentration of 25 wt% which is two times higher than the EO activity of the Chromophore L2 (23 pm/V) and the traditional aryl Chromophore (10–20 pm/V). High r 33 value, high thermal stability (onset decomposition temperatures higher than 220 °C) suggests the potential use of the new Chromophore in nonlinear optical materials.

  • synthesis of novel polyarylate with elecrooptical Chromophores as side chain as electro optic host polymer
    Colloid and Polymer Science, 2012
    Co-Authors: Liang Wang, Zhen Zhen
    Abstract:

    Two novel soluble polyarylates with different nonlinear optical Chromophores as the side chains were prepared and characterized by UV–visible spectra, nuclear magnetic resonance, and infrared spectroscopy. The titled polymers show us good thermal stability; the thermal decomposition temperature values were 201 and 253 °C, respectively, for polymer sPAR-CTCF and sPAR-CTCP. The glass transition temperatures were 139 and 122 °C for sPAR-CTCF and sPAR-CTCP, respectively. Chromophore FTC-wl was doped in these polymers as a guest Chromophore to form binary Chromophore electro-optic (EO) system. And super large EO coefficients (124 pm/V) were found from FTC-wl-doped sPAR-CTCP binary Chromophore system at high Chromophore loading density.

Leon D Reed - One of the best experts on this subject based on the ideXlab platform.

  • Synthesis of Chromophores with Extremely High Electro-optic Activities. 2. Isophorone- and Combined Isophorone−Thiophene-Based Chromophores
    Chemistry of Materials, 2002
    Co-Authors: Mingqian He, Thomas M Leslie, John A Sinicropi, Sean M. Garner, Leon D Reed
    Abstract:

    Four new isophorone and combined isophorone and thiophene bridged Chromophores have been synthesized. All of these new high μβ Chromophores possess our newly synthesized tricyanovinyldihydrofuran acceptors. Because of our unique acceptor design, all of our Chromophores show high solubility in all organic solvents due to minimized ChromophoreChromophore electrostatic interactions. These Chromophores have also been studied with respect to their solvatochromism and thermal behavior by TGA in air. Preliminary EO characterization of one of these Chromophores in polycarbonate has demonstrated an extremely high r33 of 70 pm/V at 1550 nm. We believe that this is the largest r33 reported at this wavelength.

  • synthesis of Chromophores with extremely high electro optic activities 2 isophorone and combined isophorone thiophene based Chromophores
    Chemistry of Materials, 2002
    Co-Authors: Mingqian He, Thomas M Leslie, John A Sinicropi, Sean M. Garner, Leon D Reed
    Abstract:

    Four new isophorone and combined isophorone and thiophene bridged Chromophores have been synthesized. All of these new high μβ Chromophores possess our newly synthesized tricyanovinyldihydrofuran acceptors. Because of our unique acceptor design, all of our Chromophores show high solubility in all organic solvents due to minimized ChromophoreChromophore electrostatic interactions. These Chromophores have also been studied with respect to their solvatochromism and thermal behavior by TGA in air. Preliminary EO characterization of one of these Chromophores in polycarbonate has demonstrated an extremely high r33 of 70 pm/V at 1550 nm. We believe that this is the largest r33 reported at this wavelength.

Philip A. Sullivan - One of the best experts on this subject based on the ideXlab platform.

  • Organic Electro-Optic Materials: Understanding Structure/Function Relationships Critical to the Optimization of Electro-Optic Activity
    2020
    Co-Authors: Larry R. Dalton, Benjamin C. Olbricht, Philip A. Sullivan, Joshua A. Davies, Bruce H. Robinson, Denise H. Bale, Stephanie J. Benight, Ilya V. Kosilkin, Bruce E. Eichinger
    Abstract:

    Time-dependent density functional theory quantum mechanical and pseudo-atomistic Monte Carlo statistical mechanical computations are used to guide the systematic improvement of organic electro-optic materials. In particular, the dependence of molecular first hyperpolarizability upon dielectric permittivity and optical frequency is defined as is the dependence of electric field poling-induced acentric order on a variety of intermolecular electrostatic interactions. A number of measurement techniques are used to obtain independent test of theoretical predictions of Chromophore order. The conclusion of these studies is that electro-optic activity of even complex materials (multi-Chromophore-containing dendrimers and composite materials containing several types of Chromophores, i.e., binary Chromophore organic glasses) can be predicted from first principles theory. Laser-assisted electric field poling applied to a binary Chromophore organic glass is used to provided an additional test of theory.

  • Theory-inspired development of organic electro-optic materials.
    Accounts of Chemical Research, 2010
    Co-Authors: Philip A. Sullivan, Larry R. Dalton
    Abstract:

    Correlated time-dependent density functional theory (TDDFT) quantum mechanical and pseudo-atomistic Monte Carlo (PAMC) statistical mechanical methods have been used to assist in the understanding of and to guide the improvement of organic electro-optic (OEO) materials, prepared by electric field poling of π-electron Chromophore-containing materials near their glass transition temperature. Theoretical treatment of the effects of dielectric permittivity and optical frequency on molecular (Chromophore) first hyperpolarizabilities has been carried out as well as the analysis of the influence of spatially anisotropic intermolecular electrostatic interactions on the poling-induced noncentrosymmetric order of Chromophores. Three classes of OEO materials have been considered in correlated theoretical and experimental investigations: (1) traditional Chromophore/polymer composite materials, (2) Chromophores covalently incorporated into polymers, dendrimers, and dendronized polymers, and (3) recently discovered mate...

  • Laser-Assisted Poling of Binary Chromophore Materials†
    Journal of Physical Chemistry C, 2008
    Co-Authors: Benjamin C. Olbricht, Philip A. Sullivan, Alok A. Mistry, Joshua A. Davies, Bruce E. Eichinger, Bruce H. Robinson, Philip J. Reid, Larry R. Dalton
    Abstract:

    Binary Chromophore systems represent a new and very promising class of organic second-order nonlinear optical (electro-optic) materials, where favorable intermolecular electrostatic interactions lead to significantly enhanced electro-optic coefficients and to other favorable physical properties such as low optical loss and improved stability. In this report, laser-assisted poling of a binary Chromophore system consisting of a photoaddressable Chromophore host (DR-1-co-PMMA) containing a non-photoaddressable guest Chromophore (YLD_124) is demonstrated. A factor of 2.5 enhancement in poling efficiency of the guest Chromophore (compared to simple conventional electric field poling of the same material) is observed when polarized light is used to selectively enhance the order of the host Chromophores. These results further emphasize the importance of favorable intermolecular interactions thought to exist between guest and host Chromophores in binary Chromophore containing materials. Thin-film samples were pro...

  • Advances in Organic Materials for Optical Modulation
    Journal of Lightwave Technology, 2008
    Co-Authors: Philip A. Sullivan, Benjamin C. Olbricht, Larry R. Dalton
    Abstract:

    Theory-inspired design of organic electro-optic materials is explored for three classes of materials: (1) Chromophore/polymer composites; (2) Chromophores covalently incorporated into polymers, dendrimers, and dendronized polymers; and (3) Chromophores doped into Chromophore-containing host materials. Correlated quantum/statistical mechanical calculations are used to quantitatively simulate electro-optic activity for a variety of materials falling into these three classes, elucidating the dependence of electro-optic activity on Chromophore dipole moment, Chromophore shape, covalent bond potentials, and dielectric permittivity. The practical consequence has been the production of materials exhibiting femtosecond response electro-optic activity approaching 600 pm/V at telecommunication wavelengths. Theory also provides insight into minimizing optical loss and maximizing stability.

  • Acentric lattice electro-optic materials by rational design
    Proceedings of SPIE, 2005
    Co-Authors: Larry R. Dalton, Philip A. Sullivan, Bruce E. Eichinger, Bruce H. Robinson, Denise H. Bale, Philip Ried, Andrew J. P. Akelaitis, Marnie Haller
    Abstract:

    Quantum and statistical mechanical calculations have been used to guide the improvement of the macroscopic electro-optic activity of organic thin film materials to values greater than 300 pm/V at telecommunication wavelengths. Various quantum mechanical methods (Hartree-Fock, INDO, and density functional theory) have been benchmarked and shown to be reliable for estimating trends in molecular first hyperpolarizability, β, for simple variation of donor, bridge, and acceptor structures of charge-transfer (dipolar) Chromophores. β values have been increased significantly over the past five years and quantum mechanical calculations suggest that they can be further significantly improved. Statistical mechanical calculations, including pseudo-atomistic Monte Carlo calculations, have guided the design of the super/supramolecular structures of Chromophores so that they assemble, under the influence of electric field poling, into macroscopic lattices with high degrees of acentric order. Indeed, during the past year, Chromophores doped into single- and multi-Chromophore-containing dendrimer materials to form binary glasses have yielded thin films that exhibit electro-optic activities at telecommunication wavelengths of greater than 300 pm/V. Such materials may be viewed as intermediate between Chromophore/polymer composites and crystalline organic Chromophore materials. Theory suggests that further improvements of electro-optic activity are possible. Auxiliary properties of these materials, including optical loss, thermal and photochemical stability, and processability are discussed. Such organic electro-optic materials have been incorporated into silicon photonic circuitry for active wavelength division multiplexing, reconfigurable optical add/drop multiplexing, and high bandwidth optical rectification. A variety of all-organic devices, including stripline, cascaded prism, Fabry-Perot etalon, and ring microresonator devices, have been fabricated and evaluated.

Mingqian He - One of the best experts on this subject based on the ideXlab platform.

  • Synthesis of New Electrooptic Chromophores and Their Structure−Property Relationship†
    Journal of Physical Chemistry B, 2004
    Co-Authors: Mingqian He, Thomas M Leslie, Sean M. Garner, Michael E. Derosa, Jeffery Cites
    Abstract:

    Several new high μβ Chromophores have been synthesized. These Chromophores were intentionally designed to study structure-property relationships. The synthetic strategy that was followed has been described in our previouspublications. Chromophore photostability was investigated from a structural point of view. Contact and corona poling of the Chromophores have also been accomplished with a 70 pm/V r 3 3 being achieved at λ = 1550 nm. The same Chromophores were also studied in two different polymer host systems to compare their dependence of the electrooptic coefficient and stability on the matrix material.

  • Synthesis of Chromophores with Extremely High Electro-optic Activities. 2. Isophorone- and Combined Isophorone−Thiophene-Based Chromophores
    Chemistry of Materials, 2002
    Co-Authors: Mingqian He, Thomas M Leslie, John A Sinicropi, Sean M. Garner, Leon D Reed
    Abstract:

    Four new isophorone and combined isophorone and thiophene bridged Chromophores have been synthesized. All of these new high μβ Chromophores possess our newly synthesized tricyanovinyldihydrofuran acceptors. Because of our unique acceptor design, all of our Chromophores show high solubility in all organic solvents due to minimized ChromophoreChromophore electrostatic interactions. These Chromophores have also been studied with respect to their solvatochromism and thermal behavior by TGA in air. Preliminary EO characterization of one of these Chromophores in polycarbonate has demonstrated an extremely high r33 of 70 pm/V at 1550 nm. We believe that this is the largest r33 reported at this wavelength.

  • synthesis of Chromophores with extremely high electro optic activities 2 isophorone and combined isophorone thiophene based Chromophores
    Chemistry of Materials, 2002
    Co-Authors: Mingqian He, Thomas M Leslie, John A Sinicropi, Sean M. Garner, Leon D Reed
    Abstract:

    Four new isophorone and combined isophorone and thiophene bridged Chromophores have been synthesized. All of these new high μβ Chromophores possess our newly synthesized tricyanovinyldihydrofuran acceptors. Because of our unique acceptor design, all of our Chromophores show high solubility in all organic solvents due to minimized ChromophoreChromophore electrostatic interactions. These Chromophores have also been studied with respect to their solvatochromism and thermal behavior by TGA in air. Preliminary EO characterization of one of these Chromophores in polycarbonate has demonstrated an extremely high r33 of 70 pm/V at 1550 nm. We believe that this is the largest r33 reported at this wavelength.