Diblock Copolymer Micelles and Supported Films with Noncovalently Incorporated Chromophores: A Modular Platform for Efficient Energy Transfer

Adams, Peter G.; Collins, Aaron M.; Sahin, Tuba; Subramanian, Vijaya; Urban, Volker S.; Vairaprakash, Pothiappan; Tian, Yongming; Evans, Deborah G.; Shreve, Andrew P.; Montaño, Gabriel A.

doi:10.1021/nl504814x

Title: Diblock Copolymer Micelles and Supported Films with Noncovalently Incorporated Chromophores: A Modular Platform for Efficient Energy Transfer

Abstract

Here we report generation of modular, artificial light-harvesting assemblies where an amphiphilic diblock copolymer, poly(ethylene oxide)-block-poly(butadiene), serves as the framework for noncovalent organization of BODIPY-based energy donor and bacteriochlorin-based energy acceptor chromophores. The assemblies are adaptive and form well-defined micelles in aqueous solution and high-quality monolayer and bilayer films on solid supports, with the latter showing greater than 90% energy transfer efficiency. Ultimately, this study lays the groundwork for further development of modular, polymer-based materials for light harvesting and other photonic applications.

Authors:

Adams, Peter G. ^[1]; Collins, Aaron M. ^[1]; Sahin, Tuba ^[2]; Subramanian, Vijaya ^[3]; Urban, Volker S. ^[4]; Vairaprakash, Pothiappan ^[2]; Tian, Yongming ^[5]; Evans, Deborah G. ^[3]; Shreve, Andrew P. ^[3]; Montaño, Gabriel A. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
Univ. of New Mexico, Albuquerque, NM (United States). Center for Biomedical Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biology and Soft Matter Division
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies; New Mexico Inst. of Mining and Technology, Socorro, NM (United States)

Publication Date:: Wed Apr 08 00:00:00 EDT 2015

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1261426

Grant/Contract Number:: AC05-00OR22725; SC0001035; AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: Nano Letters

Additional Journal Information:: Journal Volume: 15; Journal Issue: 4; Journal ID: ISSN 1530-6984

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Amphiphilic diblock copolymers; artificial light harvesting; Forster resonance energy transfer

Citation Formats


                    Adams, Peter G., Collins, Aaron M., Sahin, Tuba, Subramanian, Vijaya, Urban, Volker S., Vairaprakash, Pothiappan, Tian, Yongming, Evans, Deborah G., Shreve, Andrew P., and Montaño, Gabriel A. Diblock Copolymer Micelles and Supported Films with Noncovalently Incorporated Chromophores: A Modular Platform for Efficient Energy Transfer.  United States: N. p., 2015. 
Web.  doi:10.1021/nl504814x.

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                    Adams, Peter G., Collins, Aaron M., Sahin, Tuba, Subramanian, Vijaya, Urban, Volker S., Vairaprakash, Pothiappan, Tian, Yongming, Evans, Deborah G., Shreve, Andrew P., & Montaño, Gabriel A. Diblock Copolymer Micelles and Supported Films with Noncovalently Incorporated Chromophores: A Modular Platform for Efficient Energy Transfer.  United States.  https://doi.org/10.1021/nl504814x

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                    Adams, Peter G., Collins, Aaron M., Sahin, Tuba, Subramanian, Vijaya, Urban, Volker S., Vairaprakash, Pothiappan, Tian, Yongming, Evans, Deborah G., Shreve, Andrew P., and Montaño, Gabriel A. Wed .  
"Diblock Copolymer Micelles and Supported Films with Noncovalently Incorporated Chromophores: A Modular Platform for Efficient Energy Transfer".  United States.  https://doi.org/10.1021/nl504814x.  https://www.osti.gov/servlets/purl/1261426.

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@article{osti_1261426,

  title        = {Diblock Copolymer Micelles and Supported Films with Noncovalently Incorporated Chromophores: A Modular Platform for Efficient Energy Transfer},

  author       = {Adams, Peter G. and Collins, Aaron M. and Sahin, Tuba and Subramanian, Vijaya and Urban, Volker S. and Vairaprakash, Pothiappan and Tian, Yongming and Evans, Deborah G. and Shreve, Andrew P. and Montaño, Gabriel A.},

  abstractNote = {Here we report generation of modular, artificial light-harvesting assemblies where an amphiphilic diblock copolymer, poly(ethylene oxide)-block-poly(butadiene), serves as the framework for noncovalent organization of BODIPY-based energy donor and bacteriochlorin-based energy acceptor chromophores. The assemblies are adaptive and form well-defined micelles in aqueous solution and high-quality monolayer and bilayer films on solid supports, with the latter showing greater than 90% energy transfer efficiency. Ultimately, this study lays the groundwork for further development of modular, polymer-based materials for light harvesting and other photonic applications.},

  doi          = {10.1021/nl504814x},

  journal      = {Nano Letters},

  number       = 4,

  volume       = 15,

  place        = {United States},

  year         = {Wed Apr 08 00:00:00 EDT 2015},

  month        = {Wed Apr 08 00:00:00 EDT 2015}

}

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Title: Diblock Copolymer Micelles and Supported Films with Noncovalently Incorporated Chromophores: A Modular Platform for Efficient Energy Transfer

Abstract

Citation Formats

The architecture and function of the light-harvesting apparatus of purple bacteria: from single molecules to in vivo membranes journal, August 2006

Spectroscopic Properties of Antenna Complexes from Purple Bacteria book, January 2009

Versatile design of biohybrid light-harvesting architectures to tune location, density, and spectral coverage of attached synthetic chromophores for enhanced energy capture journal, March 2014

Integration of multiple chromophores with native photosynthetic antennas to enhance solar energy capture and delivery journal, January 2013

Biohybrid Photosynthetic Antenna Complexes for Enhanced Light-Harvesting journal, February 2012

Constructing a man-made c-type cytochrome maquette in vivo: electron transfer, oxygen transport and conversion to a photoactive light harvesting maquette. journal, January 2014

Design and engineering of photosynthetic light-harvesting and electron transfer using length, time, and energy scales journal, February 2006

Solar Fuels via Artificial Photosynthesis journal, December 2009

Dendritic Light-harvesting Antennas with Excitation Energy Gradients journal, October 2013

Properties of liposomes that contain chloroplast pigments: Photosensitivity and efficiency of energy conversion journal, June 1976

Photochemical energy conversion in chlorophyll-containing lipid bilayer vesicles journal, January 1982

Liposomes for photodynamic therapy journal, January 2004

Electronic excitation transfer in concentrated micelle solutions journal, October 1992

Responsive Polymers for Detection and Sensing Applications: Current Status and Future Developments journal, October 2010

Stimuli-Responsive Polymersomes as Nanocarriers for Drug and Gene Delivery: Stimuli-Responsive Polymersomes as Nanocarriers for … journal, December 2008

Polymer-Based Optical Waveguides: Materials, Processing, and Devices journal, October 2002

Enhanced photoluminescence from poly(phenylene vinylene) ∶ dendrimer polyelectrolyte assemblies in solution journal, January 2004

Engineering FRET processes within synthetic polymers, polymeric assemblies and nanoparticles via modulating spatial distribution of fluorescent donors and acceptors journal, January 2012

Enhanced white-light emission from multiple fluorophores encapsulated in a single layer of diblock copolymer micelles journal, January 2011

Nanostructures of diblock copolymer micelles for controlled fluorescence resonance energy transfer journal, January 2009

Lyotropic Phase Morphologies of Amphiphilic Block Copolymers journal, June 2001

On the Origins of Morphological Complexity in Block Copolymer Surfactants journal, April 2003

Aggregation Behavior of Poly(butadiene- b -ethylene oxide) Block Copolymers in Dilute Aqueous Solutions: Effect of Concentration, Temperature, Ionic Strength, and Type of Surfactant journal, January 2003

Hydrophobic Shell Loading of PB- b -PEO Vesicles journal, January 2009

Biomimetic Monolayer and Bilayer Membranes Made From Amphiphilic Block Copolymer Micelles journal, January 2012

Photosynthetic Antenna-Reaction Center Mimicry by Using Boron Dipyrromethene Sensitizers journal, November 2013

Amphiphilic chlorins and bacteriochlorins in micellar environments. Molecular design, de novo synthesis, and photophysical properties journal, January 2013

Structure of PS−PEO Diblock Copolymers in Solution and the Bulk State Probed Using Dynamic Light-Scattering and Small-Angle Neutron-Scattering and Dynamic Mechanical Measurements journal, July 1997

Energy Transfer book, January 2006

Surface density determination in membranes by fluorescence energy transfer journal, November 1978

Crystal structure of oxygen-evolving photosystem II at a resolution of 1.9 Å journal, April 2011

Photoinduced electron transfer processes in fullerene–organic chromophore systems journal, November 2011

Preparation of Highly Photosensitizing Liposomes with Fullerene-Doped Lipid Bilayer Using Dispersion-Controllable Molecular Exchange Reactions journal, September 2008

High photo-electrochemical activity of thylakoid–carbon nanotube composites for photosynthetic energy conversion journal, January 2013

Adaptation of intracytoplasmic membranes to altered light intensity in Rhodobacter sphaeroides journal, September 2012

Chromatic Adaptation of Photosynthetic Membranes journal, July 2005

Regulation of expression of genes for light-harvesting antenna proteins LH-I and LH-II; reaction center polypeptides RC-L, RC-M, and RC-H; and enzymes of bacteriochlorophyll and carotenoid biosynthesis in Rhodobacter capsulatus by light and oxygen. journal, October 1986

Monomeric RC–LH1 core complexes retard LH2 assembly and intracytoplasmic membrane formation in PufX-minus mutants of Rhodobacter sphaeroides journal, September 2011

Photosynthetic Pigment Localization and Thylakoid Membrane Morphology Are Altered in Synechocystis 6803 Phycobilisome Mutants journal, February 2012

Synthesis of Polymeric Temperature Sensor Based on Photophysical Property of Fullerene and Thermal Sensitivity of Poly( N -isopropylacrylamide) journal, April 2009

Design and Synthesis of a New pH Sensitive Polymeric Sensor Using Fluorescence Resonance Energy Transfer journal, December 2005

Broad-Spectrum Tunable Photoluminescent Nanomaterials Constructed from a Modular Light-Harvesting Platform Based on Macrocyclic Amphiphiles journal, June 2016

Recent progress in macrocyclic amphiphiles and macrocyclic host-based supra-amphiphiles journal, January 2018

Proteoliposomes as energy transferring nanomaterials: enhancing the spectral range of light-harvesting proteins using lipid-linked chromophores journal, January 2019

Aggregation-Induced Emission and White Luminescence from a Combination of π-Conjugated Donor–Acceptor Organic Luminogens journal, October 2018

The architecture and function of the light-harvesting apparatus of purple bacteria: from single molecules to in vivo membranes
journal, August 2006

Spectroscopic Properties of Antenna Complexes from Purple Bacteria
book, January 2009

Versatile design of biohybrid light-harvesting architectures to tune location, density, and spectral coverage of attached synthetic chromophores for enhanced energy capture
journal, March 2014

Integration of multiple chromophores with native photosynthetic antennas to enhance solar energy capture and delivery
journal, January 2013

Biohybrid Photosynthetic Antenna Complexes for Enhanced Light-Harvesting
journal, February 2012

Constructing a man-made c-type cytochrome maquette in vivo: electron transfer, oxygen transport and conversion to a photoactive light harvesting maquette.
journal, January 2014

Design and engineering of photosynthetic light-harvesting and electron transfer using length, time, and energy scales
journal, February 2006

Solar Fuels via Artificial Photosynthesis
journal, December 2009

Dendritic Light-harvesting Antennas with Excitation Energy Gradients
journal, October 2013

Properties of liposomes that contain chloroplast pigments: Photosensitivity and efficiency of energy conversion
journal, June 1976

Photochemical energy conversion in chlorophyll-containing lipid bilayer vesicles
journal, January 1982

Liposomes for photodynamic therapy
journal, January 2004

Electronic excitation transfer in concentrated micelle solutions
journal, October 1992

Responsive Polymers for Detection and Sensing Applications: Current Status and Future Developments
journal, October 2010

Stimuli-Responsive Polymersomes as Nanocarriers for Drug and Gene Delivery: Stimuli-Responsive Polymersomes as Nanocarriers for …
journal, December 2008

Polymer-Based Optical Waveguides: Materials, Processing, and Devices
journal, October 2002

Enhanced photoluminescence from poly(phenylene vinylene) ∶ dendrimer polyelectrolyte assemblies in solution
journal, January 2004

Engineering FRET processes within synthetic polymers, polymeric assemblies and nanoparticles via modulating spatial distribution of fluorescent donors and acceptors
journal, January 2012

Enhanced white-light emission from multiple fluorophores encapsulated in a single layer of diblock copolymer micelles
journal, January 2011

Nanostructures of diblock copolymer micelles for controlled fluorescence resonance energy transfer
journal, January 2009

Lyotropic Phase Morphologies of Amphiphilic Block Copolymers
journal, June 2001

On the Origins of Morphological Complexity in Block Copolymer Surfactants
journal, April 2003

Aggregation Behavior of Poly(butadiene- b -ethylene oxide) Block Copolymers in Dilute Aqueous Solutions: Effect of Concentration, Temperature, Ionic Strength, and Type of Surfactant
journal, January 2003

Hydrophobic Shell Loading of PB- b -PEO Vesicles
journal, January 2009

Biomimetic Monolayer and Bilayer Membranes Made From Amphiphilic Block Copolymer Micelles
journal, January 2012

Photosynthetic Antenna-Reaction Center Mimicry by Using Boron Dipyrromethene Sensitizers
journal, November 2013

Amphiphilic chlorins and bacteriochlorins in micellar environments. Molecular design, de novo synthesis, and photophysical properties
journal, January 2013

Structure of PS−PEO Diblock Copolymers in Solution and the Bulk State Probed Using Dynamic Light-Scattering and Small-Angle Neutron-Scattering and Dynamic Mechanical Measurements
journal, July 1997

Energy Transfer
book, January 2006

Surface density determination in membranes by fluorescence energy transfer
journal, November 1978

Crystal structure of oxygen-evolving photosystem II at a resolution of 1.9 Å
journal, April 2011

Photoinduced electron transfer processes in fullerene–organic chromophore systems
journal, November 2011

Preparation of Highly Photosensitizing Liposomes with Fullerene-Doped Lipid Bilayer Using Dispersion-Controllable Molecular Exchange Reactions
journal, September 2008

High photo-electrochemical activity of thylakoid–carbon nanotube composites for photosynthetic energy conversion
journal, January 2013

Adaptation of intracytoplasmic membranes to altered light intensity in Rhodobacter sphaeroides
journal, September 2012

Chromatic Adaptation of Photosynthetic Membranes
journal, July 2005

Regulation of expression of genes for light-harvesting antenna proteins LH-I and LH-II; reaction center polypeptides RC-L, RC-M, and RC-H; and enzymes of bacteriochlorophyll and carotenoid biosynthesis in Rhodobacter capsulatus by light and oxygen.
journal, October 1986

Monomeric RC–LH1 core complexes retard LH2 assembly and intracytoplasmic membrane formation in PufX-minus mutants of Rhodobacter sphaeroides
journal, September 2011

Photosynthetic Pigment Localization and Thylakoid Membrane Morphology Are Altered in Synechocystis 6803 Phycobilisome Mutants
journal, February 2012

Synthesis of Polymeric Temperature Sensor Based on Photophysical Property of Fullerene and Thermal Sensitivity of Poly( N -isopropylacrylamide)
journal, April 2009

Design and Synthesis of a New pH Sensitive Polymeric Sensor Using Fluorescence Resonance Energy Transfer
journal, December 2005

Broad-Spectrum Tunable Photoluminescent Nanomaterials Constructed from a Modular Light-Harvesting Platform Based on Macrocyclic Amphiphiles
journal, June 2016

Recent progress in macrocyclic amphiphiles and macrocyclic host-based supra-amphiphiles
journal, January 2018

Proteoliposomes as energy transferring nanomaterials: enhancing the spectral range of light-harvesting proteins using lipid-linked chromophores
journal, January 2019

Aggregation-Induced Emission and White Luminescence from a Combination of π-Conjugated Donor–Acceptor Organic Luminogens
journal, October 2018