Interplay of Surface and Interior Modes in Exciton–Phonon Coupling at the Nanoscale

Jasrasaria, Dipti; Rabani, Eran

doi:10.1021/acs.nanolett.1c02953

Interplay of Surface and Interior Modes in Exciton–Phonon Coupling at the Nanoscale

Journal Article · Tue Oct 05 04:00:00 EDT 2021 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.1c02953· OSTI ID:1963427

; ^[1]

University of California, Berkeley, CA (United States); Tel Aviv University, Tel Aviv (Israel); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division

Exciton-phonon coupling (EXPC) plays a key role in the optoelectronic properties of semiconductor nanocrystals (NCs), but a microscopic picture of EXPC is still lacking, particularly regarding the magnitude and scaling with NC size, the dependence on phonon frequency, and the role of the NC surface. The computational complexity associated with accurately describing excitons and phonons has limited previous theoretical studies of EXPC to small NCs, noninteracting electron-hole models, and/or a small number of phonon modes. We develop an atomistic approach for describing EXPC in NCs of experimentally relevant sizes. We validate our approach by calculating the reorganization energies, a measure of EXPC, for CdSe and CdSe-CdS core-shell NCs, finding good agreement with experimental measurements. We demonstrate that exciton formation distorts the NC lattice primarily along the coordinates of low-frequency acoustic modes. Modes at the NC surface play a significant role in smaller NCs while interior modes dominate for larger systems.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: AC02-05CH11231; SC0019140; SC0019323

OSTI ID:: 1963427

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 20 Vol. 21; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (55)

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
Many-Particle Physics Mahan, Gerald D. Physics of Solids and Liquids (PSLI) https://doi.org/10.1007/978-1-4757-5714-9	book	January 2000
Electron—phonon interactions in semiconductor nanocrystals Takagahara, T. Journal of Luminescence, Vol. 70, Issue 1-6 https://doi.org/10.1016/0022-2313(96)00050-6	journal	October 1996
Phonon dispersion measured directly from molecular dynamics simulations Kong, Ling Ti Computer Physics Communications, Vol. 182, Issue 10 https://doi.org/10.1016/j.cpc.2011.04.019	journal	October 2011
Size-Dependent Exciton–Phonon Coupling in CdSe Nanocrystals through Resonance Raman Excitation Profile Analysis Lin, Chen; Gong, Ke; Kelley, David F. The Journal of Physical Chemistry C, Vol. 119, Issue 13 https://doi.org/10.1021/acs.jpcc.5b00774	journal	March 2015
Extending Semiconductor Nanocrystals from the Quantum Dot Regime to the Molecular Cluster Regime Jethi, Lakshay; Mack, Timothy G.; Kambhampati, Patanjali The Journal of Physical Chemistry C, Vol. 121, Issue 46 https://doi.org/10.1021/acs.jpcc.7b08439	journal	November 2017
Temperature Dependence of Emission Line Widths from Semiconductor Nanocrystals Reveals Vibronic Contributions to Line Broadening Processes Mack, Timothy G.; Jethi, Lakshay; Kambhampati, Patanjali The Journal of Physical Chemistry C, Vol. 121, Issue 51 https://doi.org/10.1021/acs.jpcc.7b09903	journal	December 2017
Direct Observation of Vibronic Coupling between Excitonic States of CdSe Nanocrystals and Their Passivating Ligands Mack, Timothy G.; Jethi, Lakshay; Andrews, Mark The Journal of Physical Chemistry C, Vol. 123, Issue 8 https://doi.org/10.1021/acs.jpcc.8b11098	journal	February 2019
Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths Cui, Jian; Beyler, Andrew P.; Coropceanu, Igor Nano Letters, Vol. 16, Issue 1 https://doi.org/10.1021/acs.nanolett.5b03790	journal	December 2015
Semiconductor Seeded Nanorods with Graded Composition Exhibiting High Quantum-Yield, High Polarization, and Minimal Blinking Hadar, Ido; Philbin, John P.; Panfil, Yossef E. Nano Letters, Vol. 17, Issue 4 https://doi.org/10.1021/acs.nanolett.7b00254	journal	February 2017
Tuning Electron–Phonon Interactions in Nanocrystals through Surface Termination Yazdani, Nuri; Bozyigit, Deniz; Vuttivorakulchai, Kantawong Nano Letters, Vol. 18, Issue 4 https://doi.org/10.1021/acs.nanolett.7b04729	journal	March 2018
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
Electron–Phonon Coupling in CdSe/CdS Core/Shell Quantum Dots Lin, Chen; Gong, Ke; Kelley, David F. ACS Nano, Vol. 9, Issue 8 https://doi.org/10.1021/acsnano.5b02230	journal	July 2015
Size, Ligand, and Defect-Dependent Electron–Phonon Coupling in Chalcogenide and Perovskite Nanocrystals and Its Impact on Luminescence Line Widths Yazdani, Nuri; Volk, Sebastian; Yarema, Olesya ACS Photonics, Vol. 7, Issue 5 https://doi.org/10.1021/acsphotonics.0c00034	journal	April 2020
Quantum Dot Luminescent Concentrator Cavity Exhibiting 30-fold Concentration Bronstein, Noah D.; Yao, Yuan; Xu, Lu ACS Photonics, Vol. 2, Issue 11 https://doi.org/10.1021/acsphotonics.5b00334	journal	August 2015
Unraveling the Structure and Dynamics of Excitons in Semiconductor Quantum Dots Kambhampati, Patanjali Accounts of Chemical Research, Vol. 44, Issue 1 https://doi.org/10.1021/ar1000428	journal	January 2011
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
Temperature and Size Dependence of Nonradiative Relaxation and Exciton−Phonon Coupling in Colloidal CdTe Quantum Dots Morello, G.; De Giorgi, M.; Kudera, S. The Journal of Physical Chemistry C, Vol. 111, Issue 16 https://doi.org/10.1021/jp068307t	journal	April 2007
Hot Exciton Relaxation Dynamics in Semiconductor Quantum Dots: Radiationless Transitions on the Nanoscale Kambhampati, Patanjali The Journal of Physical Chemistry C, Vol. 115, Issue 45 https://doi.org/10.1021/jp2058673	journal	October 2011
Charge Transport in a Quantum Dot Supercrystal Chu, Iek-Heng; Radulaski, Marina; Vukmirovic, Nenad The Journal of Physical Chemistry C, Vol. 115, Issue 43 https://doi.org/10.1021/jp206526s	journal	October 2011
State-Resolved Exciton−Phonon Couplings in CdSe Semiconductor Quantum Dots Sagar, D. M.; Cooney, Ryan R.; Sewall, Samuel L. The Journal of Physical Chemistry C, Vol. 112, Issue 25 https://doi.org/10.1021/jp803386g	journal	May 2008
Highly Emissive Colloidal CdSe/CdS Heterostructures of Mixed Dimensionality Talapin, Dmitri V.; Koeppe, Robert; Götzinger, Stephan Nano Letters, Vol. 3, Issue 12 https://doi.org/10.1021/nl034815s	journal	December 2003
Electron–Phonon Coupling in CdSe Nanocrystals from an Atomistic Phonon Model Kelley, Anne Myers ACS Nano, Vol. 5, Issue 6 https://doi.org/10.1021/nn201475d	journal	May 2011
Breaking the Phonon Bottleneck in PbSe and CdSe Quantum Dots: Time-Domain Density Functional Theory of Charge Carrier Relaxation Kilina, Svetlana V.; Kilin, Dmitri S.; Prezhdo, Oleg V. ACS Nano, Vol. 3, Issue 1 https://doi.org/10.1021/nn800674n	journal	December 2008
Soft surfaces of nanomaterials enable strong phonon interactions Bozyigit, Deniz; Yazdani, Nuri; Yarema, Maksym Nature, Vol. 531, Issue 7596 https://doi.org/10.1038/nature16977	journal	March 2016
Charge transport in semiconductors assembled from nanocrystal quantum dots Yazdani, Nuri; Andermatt, Samuel; Yarema, Maksym Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16560-7	journal	June 2020
Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals Guzelturk, Burak; Cotts, Benjamin L.; Jasrasaria, Dipti Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22116-0	journal	March 2021
2D matrix engineering for homogeneous quantum dot coupling in photovoltaic solids Xu, Jixian; Voznyy, Oleksandr; Liu, Mengxia Nature Nanotechnology, Vol. 13, Issue 6 https://doi.org/10.1038/s41565-018-0117-z	journal	April 2018
Exciton-phonon coupling and disorder in the excited states of CdSe colloidal quantum dots Salvador, Mayrose R.; Graham, Matthew W.; Scholes, Gregory D. The Journal of Chemical Physics, Vol. 125, Issue 18 https://doi.org/10.1063/1.2363190	journal	November 2006
Transferable pair potentials for CdS and ZnS crystals Grünwald, Michael; Zayak, Alexey; Neaton, Jeffrey B. The Journal of Chemical Physics, Vol. 136, Issue 23 https://doi.org/10.1063/1.4729468	journal	June 2012
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
A microscopic picture of surface charge trapping in semiconductor nanocrystals Mooney, Jonathan; Krause, Michael M.; Saari, Jonathan I. The Journal of Chemical Physics, Vol. 138, Issue 20 https://doi.org/10.1063/1.4807054	journal	May 2013
Photoinduced electron transfer from semiconductor quantum dots to metal oxide nanoparticles Tvrdy, Kevin; Frantsuzov, Pavel A.; Kamat, Prashant V. Proceedings of the National Academy of Sciences, Vol. 108, Issue 1 https://doi.org/10.1073/pnas.1011972107	journal	December 2010
Atomic fluctuations in electronic materials revealed by dephasing Palato, Samuel; Seiler, Hélène; Nijjar, Parmeet Proceedings of the National Academy of Sciences, Vol. 117, Issue 22 https://doi.org/10.1073/pnas.1916792117	journal	May 2020
Quantum dot laser Ledentsov, N. N. Semiconductor Science and Technology, Vol. 26, Issue 1 https://doi.org/10.1088/0268-1242/26/1/014001	journal	November 2010
Calculation of the Huang–Rhys parameter in spherical quantum dots: the optical deformation potential effect Hamma, M.; Miranda, R. P.; Vasilevskiy, M. I. Journal of Physics: Condensed Matter, Vol. 19, Issue 34 https://doi.org/10.1088/0953-8984/19/34/346215	journal	July 2007
ProDy: Protein Dynamics Inferred from Theory and Experiments Bakan, A.; Meireles, L. M.; Bahar, I. Bioinformatics, Vol. 27, Issue 11, p. 1575-1577 https://doi.org/10.1093/bioinformatics/btr168	journal	April 2011
Evol and ProDy for bridging protein sequence evolution and structural dynamics Bakan, A.; Dutta, A.; Mao, W. Bioinformatics, Vol. 30, Issue 18 https://doi.org/10.1093/bioinformatics/btu336	journal	May 2014
Ab initio modeling of phonon-assisted relaxation of electrons and excitons in semiconductor nanocrystals for multiexciton generation Zeng, Taofang; He, Yi Physical Review B, Vol. 103, Issue 3 https://doi.org/10.1103/PhysRevB.103.035428	journal	January 2021
Size dependence of electron-phonon coupling in semiconductor nanospheres: The case of CdSe Klein, M. C.; Hache, F.; Ricard, D. Physical Review B, Vol. 42, Issue 17 https://doi.org/10.1103/PhysRevB.42.11123	journal	December 1990
Exciton–LO-phonon couplings in spherical semiconductor microcrystallites Nomura, Shintaro; Kobayashi, Takayoshi Physical Review B, Vol. 45, Issue 3 https://doi.org/10.1103/PhysRevB.45.1305	journal	January 1992
Exciton-phonon interaction in CdSe and CuCl polar semiconductor nanospheres Marini, J. C.; Stebe, B.; Kartheuser, E. Physical Review B, Vol. 50, Issue 19 https://doi.org/10.1103/PhysRevB.50.14302	journal	November 1994
Pseudopotential calculations of nanoscale CdSe quantum dots Wang, Lin-Wang; Zunger, Alex Physical Review B, Vol. 53, Issue 15 https://doi.org/10.1103/PhysRevB.53.9579	journal	April 1996
Size dependence of electron—LO-phonon coupling in semiconductor nanocrystals Scamarcio, G.; Spagnolo, V.; Ventruti, G. Physical Review B, Vol. 53, Issue 16 https://doi.org/10.1103/PhysRevB.53.R10489	journal	April 1996
Anomalous Stokes shift in CdSe nanocrystals Liptay, T. J.; Marshall, L. F.; Rao, P. S. Physical Review B, Vol. 76, Issue 15 https://doi.org/10.1103/PhysRevB.76.155314	journal	October 2007
Size dependent, state-resolved studies of exciton-phonon couplings in strongly confined semiconductor quantum dots Sagar, D. M.; Cooney, Ryan R.; Sewall, Samuel L. Physical Review B, Vol. 77, Issue 23 https://doi.org/10.1103/PhysRevB.77.235321	journal	June 2008
First-principles calculation of the electron-phonon interaction in semiconductor nanoclusters Han, Peng; Bester, Gabriel Physical Review B, Vol. 85, Issue 23 https://doi.org/10.1103/PhysRevB.85.235422	journal	June 2012
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
Fundamental difference between measured and calculated exciton-phonon coupling in nanostructures Han, Peng; Bester, Gabriel Physical Review B, Vol. 99, Issue 10 https://doi.org/10.1103/PhysRevB.99.100302	journal	March 2019
Enhanced Polar Exciton-LO-Phonon Interaction in Quantum Dots Heitz, R.; Mukhametzhanov, I.; Stier, O. Physical Review Letters, Vol. 83, Issue 22 https://doi.org/10.1103/PhysRevLett.83.4654	journal	November 1999
Electron-phonon interactions from first principles Giustino, Feliciano Reviews of Modern Physics, Vol. 89, Issue 1 https://doi.org/10.1103/RevModPhys.89.015003	journal	February 2017
Semiconductor Quantum Dots for Bioimaging and Biodiagnostic Applications Kairdolf, Brad A.; Smith, Andrew M.; Stokes, Todd H. Annual Review of Analytical Chemistry, Vol. 6, Issue 1 https://doi.org/10.1146/annurev-anchem-060908-155136	journal	June 2013
S PECTROSCOPY AND H OT E LECTRON R ELAXATION D YNAMICS IN S EMICONDUCTOR Q UANTUM W ELLS AND Q UANTUM D OTS Nozik, Arthur J. Annual Review of Physical Chemistry, Vol. 52, Issue 1 https://doi.org/10.1146/annurev.physchem.52.1.193	journal	October 2001
Spectral and Dynamical Properties of Multiexcitons in Semiconductor Nanocrystals Klimov, Victor I. Annual Review of Physical Chemistry, Vol. 58, Issue 1 https://doi.org/10.1146/annurev.physchem.58.032806.104537	journal	May 2007
Absorption and intensity-dependent photoluminescence measurements on CdSe quantum dots: assignment of the first electronic transitions Ekimov, A. I.; Kudryavtsev, I. A.; Efros, Al. L. Journal of the Optical Society of America B, Vol. 10, Issue 1 https://doi.org/10.1364/JOSAB.10.000100	journal	January 1993

Similar Records

Circumventing the phonon bottleneck by multiphonon-mediated hot exciton cooling at the nanoscale

Journal Article · Wed Aug 16 00:00:00 EDT 2023 · npj Computational Materials · OSTI ID:2217263

Theory of Photoluminescence Spectral Line Shapes of Semiconductor Nanocrystals

Journal Article · Tue Aug 08 00:00:00 EDT 2023 · Journal of Physical Chemistry Letters · OSTI ID:2323300

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
exciton−phonon coupling
nanocrystal surfaces
quantum dots
reorganization energy
semiconductor nanocrystals

Interplay of Surface and Interior Modes in Exciton–Phonon Coupling at the Nanoscale

Citation Formats

References (55)

Similar Records

Related Subjects