Photoexcited energy transfer in a weakly coupled dimer

Hernandez, Laura Alfonso; Nelson, Tammie; Tretiak, Sergei; Fernandez-Alberti, Sebastian

doi:10.1021/jp510557f

Title: Photoexcited energy transfer in a weakly coupled dimer

Journal Article · Thu Jan 08 00:00:00 EST 2015 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/jp510557f· OSTI ID:1227902

Hernandez, Laura Alfonso ^[1]; Nelson, Tammie ^[2]; Tretiak, Sergei ^[2]; Fernandez-Alberti, Sebastian ^[1]

Univ. Nacional de Quilmes, Bernal (Argentina)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Nonadiabatic excited-state molecular dynamics (NA-ESMD) simulations have been performed in order to study the time-dependent exciton localization during energy transfer between two chromophore units of the weakly coupled anthracene dimer dithia-anthracenophane (DTA). Simulations are done at both low temperature (10 K) and room temperature (300 K). The initial photoexcitation creates an exciton which is primarily localized on a single monomer unit. Subsequently, the exciton experiences an ultrafast energy transfer becoming localized on either one monomer unit or the other, whereas delocalization between both monomers never occurs. In half of the trajectories, the electronic transition density becomes completely localized on the same monomer as the initial excitation, while in the other half, it becomes completely localized on the opposite monomer. In this article, we present an analysis of the energy transfer dynamics and the effect of thermally induced geometry distortions on the exciton localization. Finally, simulated fluorescence anisotropy decay curves for both DTA and the monomer unit dimethyl anthracene (DMA) are compared. As a result, our analysis reveals that changes in the transition density localization caused by energy transfer between two monomers in DTA is not the only source of depolarization and exciton relaxation within a single DTA monomer unit can also cause reorientation of the transition dipole.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: PICT-2010-2375; AC52-06NA25396

OSTI ID:: 1227902

Report Number(s):: LA-UR-14-28224

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 119, Issue 24; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 22 works

Citation information provided by
Web of Science

References (51)

Stimulated emission due to localized and delocalized carriers in Al _0.35 Ga _0.65 N/Al _0.49 Ga _0.51 N quantum wells Mickevičius, J.; Jurkevičius, J.; Kazlauskas, K. Applied Physics Letters, Vol. 101, Issue 4 https://doi.org/10.1063/1.4738791	journal	July 2012
Localized versus delocalized states: Photoluminescence from electrochemically synthesized ZnO nanowires Voss, T.; Bekeny, C.; Gutowski, J. Journal of Applied Physics, Vol. 106, Issue 5 https://doi.org/10.1063/1.3211294	journal	September 2009
Voltage-dependent conductance of a single graphene nanoribbon Koch, Matthias; Ample, Francisco; Joachim, Christian Nature Nanotechnology, Vol. 7, Issue 11 https://doi.org/10.1038/nnano.2012.169	journal	October 2012
Charge separation in localized and delocalized electronic states in polymeric semiconductors Köhler, A.; dos Santos, D. A.; Beljonne, D. Nature, Vol. 392, Issue 6679 https://doi.org/10.1038/31901	journal	April 1998
Controlling Interchain Interactions in Conjugated Polymers: The Effects of Chain Morphology on Exciton−Exciton Annihilation and Aggregation in MEH−PPV Films Nguyen, Thuc-Quyen; Martini, Ignacio B.; Liu, Jei The Journal of Physical Chemistry B, Vol. 104, Issue 2 https://doi.org/10.1021/jp993190c	journal	January 2000
Understanding the Origin of the 535 nm Emission Band in Oxidized Poly(9,9-dioctylfluorene): The Essential Role of Inter-Chain/Inter-Segment Interactions Sims, M.; Bradley, D. D. C.; Ariu, M. Advanced Functional Materials, Vol. 14, Issue 8 https://doi.org/10.1002/adfm.200305149	journal	August 2004
Fluctuating exciton localization in giant π-conjugated spoked-wheel macrocycles Aggarwal, A. Vikas; Thiessen, Alexander; Idelson, Alissa Nature Chemistry, Vol. 5, Issue 11 https://doi.org/10.1038/nchem.1758	journal	September 2013
Shishiodoshi unidirectional energy transfer mechanism in phenylene ethynylene dendrimers Fernandez-Alberti, S.; Roitberg, Adrian E.; Kleiman, Valeria D. The Journal of Chemical Physics, Vol. 137, Issue 22 https://doi.org/10.1063/1.4745835	journal	December 2012
Energy Transfer in the Nanostar: The Role of Coulombic Coupling and Dynamics Ortiz, Wilfredo; Krueger, Brent P.; Kleiman, Valeria D. The Journal of Physical Chemistry B, Vol. 109, Issue 23 https://doi.org/10.1021/jp050611j	journal	June 2005
Nonadiabatic Molecular Dynamics Simulations of the Energy Transfer between Building Blocks in a Phenylene Ethynylene Dendrimer ^† Fernandez-Alberti, Sebastian; Kleiman, Valeria D.; Tretiak, Sergei The Journal of Physical Chemistry A, Vol. 113, Issue 26 https://doi.org/10.1021/jp900904q	journal	July 2009
Thermally-Limited Exciton Delocalization in Superradiant Molecular Aggregates Arias, Dylan H.; Stone, Katherine W.; Vlaming, Sebastiaan M. The Journal of Physical Chemistry B, Vol. 117, Issue 16 https://doi.org/10.1021/jp3086717	journal	November 2012
Effects of (Multi)branching of Dipolar Chromophores on Photophysical Properties and Two-Photon Absorption Katan, Claudine; Terenziani, Francesca; Mongin, Olivier The Journal of Physical Chemistry A, Vol. 109, Issue 13 https://doi.org/10.1021/jp044193e	journal	April 2005
Enhanced Two‐Photon Absorption of Organic Chromophores: Theoretical and Experimental Assessments Terenziani, Francesca; Katan, Claudine; Badaeva, Ekaterina Advanced Materials, Vol. 20, Issue 24 https://doi.org/10.1002/adma.200800402	journal	December 2008
Excited State Localization and Delocalization of Internal Charge Transfer in Branched Push−Pull Chromophores Studied by Single-Molecule Spectroscopy Aumiler, Damir; Wang, Sufan; Chen, Xudong Journal of the American Chemical Society, Vol. 131, Issue 16 https://doi.org/10.1021/ja901268h	journal	April 2009
Oscillatory Excitation Transfer in Dithiaanthracenophane: Quantum Beat in a Coherent Photochemical Process in Solution ^† Yamazaki, Iwao; Akimoto, Seiji; Yamazaki, Tomoko The Journal of Physical Chemistry A, Vol. 106, Issue 10 https://doi.org/10.1021/jp012455w	journal	March 2002
The real‐time intramolecular electronic excitation transfer dynamics of 9’,9‐bifluorene and 2’,2‐binaphthyl in solution Zhu, F.; Galli, C.; Hochstrasser, R. M. The Journal of Chemical Physics, Vol. 98, Issue 2 https://doi.org/10.1063/1.464329	journal	January 1993
Coherent Control of Oscillatory Excitation Transfer in Dithia-1,5[3,3]anthracenophane by a Phase-Locked Femtosecond Pulse Pair Sato, Shin-ichiro; Nishimura, Yoshinobu; Sakata, Yoshiteru The Journal of Physical Chemistry A, Vol. 107, Issue 47 https://doi.org/10.1021/jp027452d	journal	November 2003
Intermolecular interaction-induced quantum beats in femtosecond time-resolved light scattering from molecules: photon-polarization and inhomogeneous effects Kato, T.; Fujimura, Y. Chemical Physics, Vol. 202, Issue 1 https://doi.org/10.1016/0301-0104(95)00322-3	journal	January 1996
Theoretical Investigation of the Mechanism and Dynamics of Intramolecular Coherent Resonance Energy Transfer in Soft Molecules: A Case Study of Dithia-anthracenophane Yang, Lei; Caprasecca, Stefano; Mennucci, Benedetta Journal of the American Chemical Society, Vol. 132, Issue 47 https://doi.org/10.1021/ja103303u	journal	December 2010
Two-Dimensional Real-Space Analysis of Optical Excitations in Acceptor-Substituted Carotenoids Tretiak, Sergei; Chernyak, Vladimir; Mukamel, Shaul Journal of the American Chemical Society, Vol. 119, Issue 47 https://doi.org/10.1021/ja9720164	journal	November 1997
Collective electronic oscillators for nonlinear optical response of conjugated molecules Tretiak, Sergei; Chernyak, Vladimir; Mukamel, Shaul Chemical Physics Letters, Vol. 259, Issue 1-2 https://doi.org/10.1016/0009-2614(96)00790-7	journal	August 1996
Optimization of parameters for semiempirical methods I. Method Stewart, James J. P. Journal of Computational Chemistry, Vol. 10, Issue 2 https://doi.org/10.1002/jcc.540100208	journal	March 1989
Optimization of parameters for semiempirical methods II. Applications Stewart, James J. P. Journal of Computational Chemistry, Vol. 10, Issue 2 https://doi.org/10.1002/jcc.540100209	journal	March 1989
Configuration interaction singles, time-dependent Hartree–Fock, and time-dependent density functional theory for the electronic excited states of extended systems Hirata, So; Head-Gordon, Martin; Bartlett, Rodney J. The Journal of Chemical Physics, Vol. 111, Issue 24 https://doi.org/10.1063/1.480443	journal	December 1999
Stilbenoid Dimers: Dissection of a Paracyclophane Chromophore Bazan, Guillermo C.; Oldham,, Warren J.; Lachicotte, Rene J. Journal of the American Chemical Society, Vol. 120, Issue 36 https://doi.org/10.1021/ja973816h	journal	September 1998
Excited electronic states of carotenoids: Time-dependent density-matrix-response algorithm Tretiak, Sergei; Chernyak, Vladimir; Mukamel, Shaul International Journal of Quantum Chemistry, Vol. 70, Issue 4-5 https://doi.org/10.1002/(SICI)1097-461X(1998)70:4/5<711::AID-QUA17>3.0.CO;2-4	journal	January 1998
Chemical Bonding and Size Scaling of Nonlinear Polarizabilities of Conjugated Polymers Tretiak, Sergei; Chernyak, Vladimir; Mukamel, Shaul Physical Review Letters, Vol. 77, Issue 22 https://doi.org/10.1103/PhysRevLett.77.4656	journal	November 1996
Localized Electronic Excitations in Phenylacetylene Dendrimers Tretiak, Sergei; Chernyak, Vladimir; Mukamel, Shaul The Journal of Physical Chemistry B, Vol. 102, Issue 18 https://doi.org/10.1021/jp980745f	journal	April 1998
Single-Reference ab Initio Methods for the Calculation of Excited States of Large Molecules Dreuw, Andreas; Head-Gordon, Martin Chemical Reviews, Vol. 105, Issue 11 https://doi.org/10.1021/cr0505627	journal	November 2005
Molecular dynamics with electronic transitions Tully, John C. The Journal of Chemical Physics, Vol. 93, Issue 2 https://doi.org/10.1063/1.459170	journal	July 1990
Proton transfer in solution: Molecular dynamics with quantum transitions Hammes‐Schiffer, Sharon; Tully, John C. The Journal of Chemical Physics, Vol. 101, Issue 6 https://doi.org/10.1063/1.467455	journal	September 1994
Constant temperature simulations using the Langevin equation with velocity Verlet integration Paterlini, M. Germana; Ferguson, David M. Chemical Physics, Vol. 236, Issue 1-3 https://doi.org/10.1016/S0301-0104(98)00214-6	journal	September 1998
Statistical mechanical theory for non-equilibrium systems. IX. Stochastic molecular dynamics Attard, Phil The Journal of Chemical Physics, Vol. 130, Issue 19 https://doi.org/10.1063/1.3138762	journal	May 2009
Representation independent algorithms for molecular response calculations in time-dependent self-consistent field theories Tretiak, Sergei; Isborn, Christine M.; Niklasson, Anders M. N. The Journal of Chemical Physics, Vol. 130, Issue 5 https://doi.org/10.1063/1.3068658	journal	February 2009
Recursive density‐matrix‐spectral‐moment algorithm for molecular nonlinear polarizabilities Tretiak, Sergei; Chernyak, Vladimir; Mukamel, Shaul The Journal of Chemical Physics, Vol. 105, Issue 19 https://doi.org/10.1063/1.472621	journal	November 1996
Adiabatic time-dependent density functional methods for excited state properties Furche, Filipp; Ahlrichs, Reinhart The Journal of Chemical Physics, Vol. 117, Issue 16 https://doi.org/10.1063/1.1508368	journal	October 2002
Nonadiabatic Excited-State Molecular Dynamics Modeling of Photoinduced Dynamics in Conjugated Molecules Nelson, Tammie; Fernandez-Alberti, Sebastian; Chernyak, Vladimir The Journal of Physical Chemistry B, Vol. 115, Issue 18 https://doi.org/10.1021/jp109522g	journal	May 2011
First-order nonadiabatic couplings from time-dependent hybrid density functional response theory: Consistent formalism, implementation, and performance Send, Robert; Furche, Filipp The Journal of Chemical Physics, Vol. 132, Issue 4 https://doi.org/10.1063/1.3292571	journal	January 2010
Nonadiabatic coupling vectors for excited states within time-dependent density functional theory in the Tamm–Dancoff approximation and beyond Tavernelli, Ivano; Curchod, Basile F. E.; Laktionov, Andrey The Journal of Chemical Physics, Vol. 133, Issue 19 https://doi.org/10.1063/1.3503765	journal	November 2010
Nonadiabatic excited-state molecular dynamics: Numerical tests of convergence and parameters Nelson, Tammie; Fernandez-Alberti, Sebastian; Chernyak, Vladimir The Journal of Chemical Physics, Vol. 136, Issue 5 https://doi.org/10.1063/1.3680565	journal	February 2012
Identification of unavoided crossings in nonadiabatic photoexcited dynamics involving multiple electronic states in polyatomic conjugated molecules Fernandez-Alberti, Sebastian; Roitberg, Adrian E.; Nelson, Tammie The Journal of Chemical Physics, Vol. 137, Issue 1 https://doi.org/10.1063/1.4732536	journal	July 2012
Artifacts due to trivial unavoided crossings in the modeling of photoinduced energy transfer dynamics in extended conjugated molecules Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E. Chemical Physics Letters, Vol. 590 https://doi.org/10.1016/j.cplett.2013.10.052	journal	December 2013
Nonadiabatic excited-state molecular dynamics: Treatment of electronic decoherence Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E. The Journal of Chemical Physics, Vol. 138, Issue 22 https://doi.org/10.1063/1.4809568	journal	June 2013
Nonadiabatic Excited-State Molecular Dynamics: Modeling Photophysics in Organic Conjugated Materials Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E. Accounts of Chemical Research, Vol. 47, Issue 4 https://doi.org/10.1021/ar400263p	journal	February 2014
Density Matrix Analysis and Simulation of Electronic Excitations in Conjugated and Aggregated Molecules Tretiak, Sergei; Mukamel, Shaul Chemical Reviews, Vol. 102, Issue 9 https://doi.org/10.1021/cr0101252	journal	September 2002
Multiscale Modeling of Electronic Excitations in Branched Conjugated Molecules Using an Exciton Scattering Approach Wu, Chao; Malinin, Sergey V.; Tretiak, Sergei Physical Review Letters, Vol. 100, Issue 5 https://doi.org/10.1103/PhysRevLett.100.057405	journal	February 2008
Charge-Transfer Excitations Steer the Davydov Splitting and Mediate Singlet Exciton Fission in Pentacene Beljonne, D.; Yamagata, H.; Brédas, J. L. Physical Review Letters, Vol. 110, Issue 22 https://doi.org/10.1103/PhysRevLett.110.226402	journal	May 2013
On the Singlet‐Exciton States of Crystalline Anthracene Silbey, Robert; Jortner, Joshua; Rice, Stuart A. The Journal of Chemical Physics, Vol. 42, Issue 5 https://doi.org/10.1063/1.1696154	journal	March 1965
Temperature Dependence of the Davydov Splitting in Anthracene Kurik, M. V.; Piryatinskii, Yu. P.; Popel, O. M. physica status solidi (b), Vol. 37, Issue 2 https://doi.org/10.1002/pssb.19700370231	journal	January 1970
Theory of fluorescence depolarization in macromolecules and membranes Szabo, Attila The Journal of Chemical Physics, Vol. 81, Issue 1 https://doi.org/10.1063/1.447378	journal	July 1984
Principles of Fluorescence Spectroscopy Lakowicz, Joseph R. Springer New York, NY https://doi.org/10.1007/978-0-387-46312-4	book	January 2006

Cited By (3)

Coherent exciton-vibrational dynamics and energy transfer in conjugated organics Nelson, Tammie R.; Ondarse-Alvarez, Dianelys; Oldani, Nicolas Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04694-8	journal	June 2018
Carbon nanorings with inserted acenes: breaking symmetry in excited state dynamics Franklin-Mergarejo, R.; Alvarez, D. Ondarse; Tretiak, S. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep31253	journal	August 2016
Exciton localization in excited-state dynamics of a tetracene trimer: a surface hopping LC-TDDFTB study Titov, Evgenii; Humeniuk, Alexander; Mitrić, Roland Physical Chemistry Chemical Physics, Vol. 20, Issue 40 https://doi.org/10.1039/c8cp05240a	journal	January 2018

Similar Records

Theoretical Investigation of the Mechanism and Dynamics of Intramolecular Coherent Resonance Energy Transfer in Soft Molecules: A Case Study of Dithia-anthracenophane

Journal Article · Wed Dec 01 00:00:00 EST 2010 · Journal of the American Chemical Society · OSTI ID:1227902

Yang, Lei; Caprasecca, Stefano; Mennucci, Benedetta; +1 more

Photoinduced Intra- and Intermolecular Energy Transfer in Chlorophyll a Dimer

Journal Article · Mon May 08 00:00:00 EDT 2017 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry · OSTI ID:1227902

Zheng, Fulu; Fernandez-Alberti, Sebastian; Tretiak, Sergei; +1 more

Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states

Journal Article · Wed May 18 00:00:00 EDT 2016 · Chemical Physics · OSTI ID:1227902

Nelson, Tammie; Naumov, Artem; Fernandez-Alberti, Sebastian; +1 more

Related Subjects

36 MATERIALS SCIENCE
energy transfer
fluorescence anisotropy
excited states
bichromophore

Title: Photoexcited energy transfer in a weakly coupled dimer

Citation Formats

References (51)

Cited By (3)

Similar Records

Related Subjects