Incoherent nonadiabatic to coherent adiabatic transition of electron transfer in colloidal quantum dot molecules

Hou, Bokang; Thoss, Michael; Banin, Uri; Rabani, Eran

doi:10.1038/s41467-023-38470-0

Incoherent nonadiabatic to coherent adiabatic transition of electron transfer in colloidal quantum dot molecules

Journal Article · Sat May 27 00:00:00 EDT 2023 · Nature Communications

DOI:https://doi.org/10.1038/s41467-023-38470-0· OSTI ID:2229326

^[1]; Thoss, Michael ^[2]; ^[3]; ^[4]

Univ. of California, Berkeley, CA (United States)
Univ. of Freiburg (Germany)
Hebrew Univ. of Jerusalem (Israel)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Tel Aviv Univ., Tel Aviv (Israel). Sackler Center for Computational Molecular and Materials Science

Electron transfer is a fundamental process in chemistry, biology, and physics. One of the most intriguing questions concerns the realization of the transitions between nonadiabatic and adiabatic regimes of electron transfer. Using colloidal quantum dot molecules, we computationally demonstrate how the hybridization energy (electronic coupling) can be tuned by changing the neck dimensions and/or the quantum dot sizes. This provides a handle to tune the electron transfer from the incoherent nonadiabatic regime to the coherent adiabatic regime in a single system. We develop an atomistic model to account for several states and couplings to the lattice vibrations and utilize the mean-field mixed quantum-classical method to describe the charge transfer dynamics. Here, we show that charge transfer rates increase by several orders of magnitude as the system is driven to the coherent, adiabatic limit, even at elevated temperatures, and delineate the inter-dot and torsional acoustic modes that couple most strongly to the charge transfer dynamics.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2229326

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (36)

Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Very Large Electronic Structure Calculations Using an Out-of-Core Filter-Diagonalization Method Toledo, Sivan; Rabani, Eran Journal of Computational Physics, Vol. 180, Issue 1 https://doi.org/10.1006/jcph.2002.7090	journal	July 2002
Concepts and Methods in the Theory of Open Quantum Systems Breuer, Heinz-Peter; Petruccione, Francesco Irreversible Quantum Dynamics https://doi.org/10.1007/3-540-44874-8_4	book	January 2003
Outer-sphere electron transfer in polar solvents Zusman, L. D. Chemical Physics, Vol. 49, Issue 2 https://doi.org/10.1016/0301-0104(80)85267-0	journal	July 1980
The theory of transitions between electronic states. Application to radiationless transitions in polar solvents Zusman, L. D. Chemical Physics, Vol. 80, Issue 1-2 https://doi.org/10.1016/0301-0104(83)85166-0	journal	October 1983
The Theory of Relaxation Processes Redfield, A. G. Advances in Magnetic Resonance https://doi.org/10.1016/B978-1-4832-3114-3.50007-6	book	January 1965
Femtosecond charge transfer dynamics in artificial donor/acceptor systems: switching from adiabatic to nonadiabatic regimes by small structural changes Fiebig, T.; Stock, K.; Lochbrunner, S. Chemical Physics Letters, Vol. 345, Issue 1-2 https://doi.org/10.1016/S0009-2614(01)00869-7	journal	September 2001
Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics Crespo-Otero, Rachel; Barbatti, Mario Chemical Reviews, Vol. 118, Issue 15 https://doi.org/10.1021/acs.chemrev.7b00577	journal	April 2018
Interplay of Surface and Interior Modes in Exciton–Phonon Coupling at the Nanoscale Jasrasaria, Dipti; Rabani, Eran Nano Letters, Vol. 21, Issue 20 https://doi.org/10.1021/acs.nanolett.1c02953	journal	October 2021
Correction to Interplay of Surface and Interior Modes in Exciton–Phonon Coupling at the Nanoscale Jasrasaria, Dipti; Rabani, Eran Nano Letters, Vol. 22, Issue 19 https://doi.org/10.1021/acs.nanolett.2c03590	journal	September 2022
Electron–Hole Correlations Govern Auger Recombination in Nanostructures Philbin, John P.; Rabani, Eran Nano Letters, Vol. 18, Issue 12 https://doi.org/10.1021/acs.nanolett.8b03715	journal	November 2018
The Localized-to-Delocalized Transition in Mixed-Valence Chemistry Demadis, Konstantinos D.; Hartshorn, Chris M.; Meyer, Thomas J. Chemical Reviews, Vol. 101, Issue 9 https://doi.org/10.1021/cr990413m	journal	September 2001
Electronic Structure Pseudopotential Calculations of Large (.apprx.1000 Atoms) Si Quantum Dots Wang, Lin Wang; Zunger, Alex The Journal of Physical Chemistry, Vol. 98, Issue 8 https://doi.org/10.1021/j100059a032	journal	February 1994
Neck Barrier Engineering in Quantum Dot Dimer Molecules via Intraparticle Ripening Cui, Jiabin; Koley, Somnath; Panfil, Yossef E. Journal of the American Chemical Society, Vol. 143, Issue 47 https://doi.org/10.1021/jacs.1c08863	journal	November 2021
Colloidal quantum dot molecules manifesting quantum coupling at room temperature Cui, Jiabin; Panfil, Yossef E.; Koley, Somnath Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-13349-1	journal	December 2019
Crossover between the adiabatic and nonadiabatic electron transfer limits in the Landau-Zener model Zhu, Guang Yuan; Qin, Yi; Meng, Miao Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-020-20557-7	journal	January 2021
Quantum-coherent nanoscience Heinrich, Andreas J.; Oliver, William D.; Vandersypen, Lieven M. K. Nature Nanotechnology, Vol. 16, Issue 12 https://doi.org/10.1038/s41565-021-00994-1	journal	November 2021
Self-consistent hybrid approach for complex systems: Application to the spin-boson model with Debye spectral density Thoss, Michael; Wang, Haobin; Miller, William H. The Journal of Chemical Physics, Vol. 115, Issue 7 https://doi.org/10.1063/1.1385562	journal	August 2001
Localized molecular orbitals for polyatomic molecules. I. A comparison of the Edmiston‐Ruedenberg and Boys localization methods Kleier, Daniel A.; Halgren, Thomas A.; Hall, John H. The Journal of Chemical Physics, Vol. 61, Issue 10 https://doi.org/10.1063/1.1681683	journal	November 1974
On the Theory of Oxidation‐Reduction Reactions Involving Electron Transfer. I Marcus, R. A. The Journal of Chemical Physics, Vol. 24, Issue 5 https://doi.org/10.1063/1.1742723	journal	May 1956
Reduced density matrix hybrid approach: An efficient and accurate method for adiabatic and non-adiabatic quantum dynamics Berkelbach, Timothy C.; Reichman, David R.; Markland, Thomas E. The Journal of Chemical Physics, Vol. 136, Issue 3 https://doi.org/10.1063/1.3671372	journal	January 2012
Temperature dependent activation energy for electron transfer between biological molecules Jortner, Joshua The Journal of Chemical Physics, Vol. 64, Issue 12 https://doi.org/10.1063/1.432142	journal	June 1976
Semiclassical theory of the photon echo: Application to polar fluids Shemetulskis, Norah E.; Loring, Roger F. The Journal of Chemical Physics, Vol. 97, Issue 2 https://doi.org/10.1063/1.463248	journal	July 1992
Extraction, through filter‐diagonalization, of general quantum eigenvalues or classical normal mode frequencies from a small number of residues or a short‐time segment of a signal. I. Theory and application to a quantum‐dynamics model Wall, Michael R.; Neuhauser, Daniel The Journal of Chemical Physics, Vol. 102, Issue 20 https://doi.org/10.1063/1.468999	journal	May 1995
Vibronic spectra in condensed matter: A comparison of exact quantum mechanical and various semiclassical treatments for harmonic baths Egorov, S. A.; Rabani, Eran; Berne, B. J. The Journal of Chemical Physics, Vol. 108, Issue 4 https://doi.org/10.1063/1.475512	journal	January 1998
Nonradiative relaxation processes in condensed phases: Quantum versus classical baths Egorov, S. A.; Rabani, Eran; Berne, B. J. The Journal of Chemical Physics, Vol. 110, Issue 11 https://doi.org/10.1063/1.478420	journal	March 1999
Electronic properties of CdSe nanocrystals in the absence and presence of a dielectric medium Rabani, Eran; Hetényi, Balázs; Berne, B. J. The Journal of Chemical Physics, Vol. 110, Issue 11 https://doi.org/10.1063/1.478431	journal	March 1999
Ehrenfest and classical path dynamics with decoherence and detailed balance Nijjar, Parmeet; Jankowska, Joanna; Prezhdo, Oleg V. The Journal of Chemical Physics, Vol. 150, Issue 20 https://doi.org/10.1063/1.5095810	journal	May 2019
Simulations of nonradiative processes in semiconductor nanocrystals Jasrasaria, Dipti; Weinberg, Daniel; Philbin, John P. The Journal of Chemical Physics, Vol. 157, Issue 2 https://doi.org/10.1063/5.0095897	journal	July 2022
Hybridization and deconfinement in colloidal quantum dot molecules Verbitsky, Lior; Jasrasaria, Dipti; Banin, Uri The Journal of Chemical Physics, Vol. 157, Issue 13 https://doi.org/10.1063/5.0112443	journal	October 2022
A variational solution of the time-dependent Schrodinger equation McLachlan, A. D. Molecular Physics, Vol. 8, Issue 1 https://doi.org/10.1080/00268976400100041	journal	January 1964
Electronic structures of [110]-faceted self-assembled pyramidal InAs/GaAs quantum dots Wang, Lin-Wang; Kim, Jeongnim; Zunger, Alex Physical Review B, Vol. 59, Issue 8 https://doi.org/10.1103/PhysRevB.59.5678	journal	February 1999
Stillinger-Weber potential for the II-VI elements Zn-Cd-Hg-S-Se-Te Zhou, X. W.; Ward, D. K.; Martin, J. E. Physical Review B, Vol. 88, Issue 8 https://doi.org/10.1103/PhysRevB.88.085309	journal	August 2013
Canonical Configurational Interaction Procedure Foster, J. M.; Boys, S. F. Reviews of Modern Physics, Vol. 32, Issue 2 https://doi.org/10.1103/RevModPhys.32.300	journal	April 1960
Electron Transfer Reactions in Condensed Phases Newton, M. D.; Sutin, N. Annual Review of Physical Chemistry, Vol. 35, Issue 1 https://doi.org/10.1146/annurev.pc.35.100184.002253	journal	October 1984
Progress in the Theory of Mixed Quantum-Classical Dynamics Kapral, Raymond Annual Review of Physical Chemistry, Vol. 57, Issue 1 https://doi.org/10.1146/annurev.physchem.57.032905.104702	journal	May 2006

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