Investigation of plasmon relaxation mechanisms using nonadiabatic molecular dynamics

Wu, Xiaoyan; Liu, Baopi; Frauenheim, Thomas; Tretiak, Sergei; Yam, ChiYung; Zhang, Yu

doi:10.1063/5.0127435

Investigation of plasmon relaxation mechanisms using nonadiabatic molecular dynamics

Journal Article · Wed Nov 30 23:00:00 EST 2022 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0127435· OSTI ID:1922787

^[1]; Liu, Baopi ^[1]; Frauenheim, Thomas ^[2]; ^[3]; ^[4]; ^[3]

Shenzhen JL Computational Science and Applied Research Institute (China)
Shenzhen JL Computational Science and Applied Research Institute (China); Beijing Computational Science Research Center (China); Univ. of Bremen (Germany)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Electronic Science and Technology of China (China); Hong Kong Quantum AI Lab Limited (China)

Hot carriers generated from the decay of plasmon excitation can be harvested to drive a wide range of physical or chemical processes. However, their generation efficiency is limited by the concomitant phonon-induced relaxation processes by which the energy in excited carriers is transformed into heat. However, simulations of dynamics of nanoscale clusters are challenging due to the computational complexity involved. Here, in this paper, we adopt our newly developed Trajectory Surface Hopping (TSH) nonadiabatic molecular dynamics algorithm to simulate plasmon relaxation in Au₂₀ clusters, taking the atomistic details into account. The electronic properties are treated within the Linear Response Time-Dependent Tight-binding Density Functional Theory (LR-TDDFTB) framework. The relaxation of plasmon due to coupling to phonon modes in Au₂₀ beyond the Born–Oppenheimer approximation is described by the TSH algorithm. The numerically efficient LR-TDDFTB method allows us to address a dense manifold of excited states to ensure the inclusion of plasmon excitation. Starting from the photoexcited plasmon states in Au₂₀ cluster, we find that the time constant for relaxation from plasmon excited states to the lowest excited states is about 2.7 ps, mainly resulting from a stepwise decay process caused by low-frequency phonons of the Au₂₀ cluster. Furthermore, our simulations show that the lifetime of the phonon-induced plasmon dephasing process is ~10.4 fs and that such a swift process can be attributed to the strong nonadiabatic effect in small clusters. Our simulations demonstrate a detailed description of the dynamic processes in nanoclusters, including plasmon excitation, hot carrier generation from plasmon excitation dephasing, and the subsequent phonon-induced relaxation process.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1922787

Report Number(s):: LA-UR-22-25284

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 157; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (70)

Hydrogen Detected by the Naked Eye: Optical Hydrogen Gas Sensors Based on Core/Shell Plasmonic Nanorod Metamaterials Nasir, Mazhar E.; Dickson, Wayne; Wurtz, Gregory A. Advanced Materials, Vol. 26, Issue 21 https://doi.org/10.1002/adma.201305958	journal	March 2014
SCC-DFTB parameters for simulating hybrid gold-thiolates compounds Fihey, Arnaud; Hettich, Christian; Touzeau, Jérémy Journal of Computational Chemistry, Vol. 36, Issue 27 https://doi.org/10.1002/jcc.24046	journal	August 2015
Implementation of surface hopping molecular dynamics using semiempirical methods Fabiano, E.; Keal, T. W.; Thiel, W. Chemical Physics, Vol. 349, Issue 1-3 https://doi.org/10.1016/j.chemphys.2008.01.044	journal	June 2008
Plasmon-Mediated Electron Injection from Au Nanorods into MoS2: Traditional versus Photoexcitation Mechanism Zhang, Zhaosheng; Liu, Lihong; Fang, Wei-Hai Chem, Vol. 4, Issue 5 https://doi.org/10.1016/j.chempr.2018.02.025	journal	May 2018
Approximate time-dependent density functional theory Niehaus, T. A. Journal of Molecular Structure: THEOCHEM, Vol. 914, Issue 1-3 https://doi.org/10.1016/j.theochem.2009.04.034	journal	November 2009
Direct probe of size-dependent electronic relaxation in single-sized Au and nearly monodisperse Pt colloidal nano-particles Smith, Brian A.; Zhang, Jin Z.; Giebel, Ursula Chemical Physics Letters, Vol. 270, Issue 1-2 https://doi.org/10.1016/s0009-2614(97)00339-4	journal	May 1997
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
Chemical Interface Damping of Surface Plasmon Resonances Lee, Stephen A.; Link, Stephan Accounts of Chemical Research, Vol. 54, Issue 8 https://doi.org/10.1021/acs.accounts.0c00872	journal	March 2021
NEXMD Software Package for Nonadiabatic Excited State Molecular Dynamics Simulations Malone, Walter; Nebgen, Benjamin; White, Alexander Journal of Chemical Theory and Computation, Vol. 16, Issue 9 https://doi.org/10.1021/acs.jctc.0c00248	journal	July 2020
First Principles Nonadiabatic Excited-State Molecular Dynamics in NWChem Song, Huajing; Fischer, Sean A.; Zhang, Yu Journal of Chemical Theory and Computation, Vol. 16, Issue 10 https://doi.org/10.1021/acs.jctc.0c00295	journal	August 2020
Time-Dependent Extension of the Long-Range Corrected Density Functional Based Tight-Binding Method Kranz, Julian J.; Elstner, Marcus; Aradi, Bálint Journal of Chemical Theory and Computation, Vol. 13, Issue 4 https://doi.org/10.1021/acs.jctc.6b01243	journal	March 2017
Theory of Plasmonic Hot-Carrier Generation and Relaxation Zhang, Yu The Journal of Physical Chemistry A, Vol. 125, Issue 41 https://doi.org/10.1021/acs.jpca.1c05837	journal	October 2021
Atomistic Insights into Chemical Interface Damping of Surface Plasmon Excitations in Silver Nanoclusters Douglas-Gallardo, Oscar A.; Berdakin, Matías; Sánchez, Cristián G. The Journal of Physical Chemistry C, Vol. 120, Issue 42 https://doi.org/10.1021/acs.jpcc.6b08519	journal	October 2016
Interplay between Intra- and Interband Transitions Associated with the Plasmon-Induced Hot Carrier Generation Process in Silver and Gold Nanoclusters Berdakin, Matias; Douglas-Gallardo, Oscar A.; Sánchez, Cristián G. The Journal of Physical Chemistry C, Vol. 124, Issue 2 https://doi.org/10.1021/acs.jpcc.9b10871	journal	December 2019
Fast Numerical Evaluation of Time-Derivative Nonadiabatic Couplings for Mixed Quantum–Classical Methods Ryabinkin, Ilya G.; Nagesh, Jayashree; Izmaylov, Artur F. The Journal of Physical Chemistry Letters, Vol. 6, Issue 21 https://doi.org/10.1021/acs.jpclett.5b02062	journal	October 2015
Slow Relaxation of Surface Plasmon Excitations in Au₅₅: The Key to Efficient Plasmonic Heating in Au/TiO₂ Ranasingha, Oshadha; Wang, Hong; Zobač, Vladimír The Journal of Physical Chemistry Letters, Vol. 7, Issue 8 https://doi.org/10.1021/acs.jpclett.6b00283	journal	April 2016
Fundamental Limitations to Plasmonic Hot-Carrier Solar Cells Zhang, Yu; Yam, ChiYung; Schatz, George C. The Journal of Physical Chemistry Letters, Vol. 7, Issue 10 https://doi.org/10.1021/acs.jpclett.6b00879	journal	May 2016
Interfacial States Cause Equal Decay of Plasmons and Hot Electrons at Gold–Metal Oxide Interfaces Foerster, Benjamin; Hartelt, Michael; Collins, Sean S. E. Nano Letters, Vol. 20, Issue 5 https://doi.org/10.1021/acs.nanolett.0c00223	journal	March 2020
Modeling Auger Processes with Nonadiabatic Molecular Dynamics Zhou, Guoqing; Lu, Gang; Prezhdo, Oleg V. Nano Letters, Vol. 21, Issue 1 https://doi.org/10.1021/acs.nanolett.0c04442	journal	December 2020
Determining Plasmonic Hot Electrons and Photothermal Effects during H ₂ Evolution with TiN–Pt Nanohybrids Rej, Sourav; Mascaretti, Luca; Santiago, Eva Yazmin ACS Catalysis, Vol. 10, Issue 9 https://doi.org/10.1021/acscatal.0c00343	journal	March 2020
Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure Rossi, Tuomas P.; Erhart, Paul; Kuisma, Mikael ACS Nano, Vol. 14, Issue 8 https://doi.org/10.1021/acsnano.0c03004	journal	July 2020
Ligands Slow Down Pure-Dephasing in Semiconductor Quantum Dots Liu, Jin; Kilina, Svetlana V.; Tretiak, Sergei ACS Nano, Vol. 9, Issue 9 https://doi.org/10.1021/acsnano.5b03255	journal	August 2015
Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry Brown, Ana M.; Sundararaman, Ravishankar; Narang, Prineha ACS Nano, Vol. 10, Issue 1 https://doi.org/10.1021/acsnano.5b06199	journal	December 2015
Plasmonic Hot-Carrier-Mediated Tunable Photochemical Reactions Zhang, Yu; Nelson, Tammie; Tretiak, Sergei ACS Nano, Vol. 12, Issue 8 https://doi.org/10.1021/acsnano.8b03830	journal	July 2018
Hot-Electron Dynamics and Thermalization in Small Metallic Nanoparticles Saavedra, J. R. M.; Asenjo-Garcia, Ana; García de Abajo, F. Javier ACS Photonics, Vol. 3, Issue 9 https://doi.org/10.1021/acsphotonics.6b00217	journal	July 2016
Understanding Hot-Electron Generation and Plasmon Relaxation in Metal Nanocrystals: Quantum and Classical Mechanisms Besteiro, Lucas V.; Kong, Xiang-Tian; Wang, Zhiming ACS Photonics, Vol. 4, Issue 11 https://doi.org/10.1021/acsphotonics.7b00751	journal	October 2017
Relaxation of Plasmon-Induced Hot Carriers Liu, Jun G.; Zhang, Hui; Link, Stephan ACS Photonics, Vol. 5, Issue 7 https://doi.org/10.1021/acsphotonics.7b00881	journal	December 2017
Noble Metals on the Nanoscale: Optical and Photothermal Properties and Some Applications in Imaging, Sensing, Biology, and Medicine Jain, Prashant K.; Huang, Xiaohua; El-Sayed, Ivan H. Accounts of Chemical Research, Vol. 41, Issue 12, p. 1578-1586 https://doi.org/10.1021/ar7002804	journal	December 2008
Some Interesting Properties of Metals Confined in Time and Nanometer Space of Different Shapes El-Sayed, Mostafa A. Accounts of Chemical Research, Vol. 34, Issue 4 https://doi.org/10.1021/ar960016n	journal	April 2001
Femtochemistry at Metal Surfaces: Nonadiabatic Reaction Dynamics Frischkorn, Christian; Wolf, Martin Chemical Reviews, Vol. 106, Issue 10 https://doi.org/10.1021/cr050161r	journal	October 2006
Plasmons in Strongly Coupled Metallic Nanostructures Halas, Naomi J.; Lal, Surbhi; Chang, Wei-Shun Chemical Reviews, Vol. 111, Issue 6 https://doi.org/10.1021/cr200061k	journal	June 2011
Direct Photocatalysis by Plasmonic Nanostructures Kale, Matthew J.; Avanesian, Talin; Christopher, Phillip ACS Catalysis, Vol. 4, Issue 1 https://doi.org/10.1021/cs400993w	journal	December 2013
The PYXAID Program for Non-Adiabatic Molecular Dynamics in Condensed Matter Systems Akimov, Alexey V.; Prezhdo, Oleg V. Journal of Chemical Theory and Computation, Vol. 9, Issue 11 https://doi.org/10.1021/ct400641n	journal	October 2013
Global Flux Surface Hopping Approach for Mixed Quantum-Classical Dynamics Wang, Linjun; Trivedi, Dhara; Prezhdo, Oleg V. Journal of Chemical Theory and Computation, Vol. 10, Issue 9 https://doi.org/10.1021/ct5003835	journal	June 2014
Instantaneous Generation of Charge-Separated State on TiO ₂ Surface Sensitized with Plasmonic Nanoparticles Long, Run; Prezhdo, Oleg V. Journal of the American Chemical Society, Vol. 136, Issue 11 https://doi.org/10.1021/ja5001592	journal	March 2014
Mechanistic Insights into Photocatalyzed H ₂ Dissociation on Au Clusters Wu, Qisheng; Zhou, Linsen; Schatz, George C. Journal of the American Chemical Society, Vol. 142, Issue 30 https://doi.org/10.1021/jacs.0c04491	journal	July 2020
Hot Electrons Generated from Doped Quantum Dots via Upconversion of Excitons to Hot Charge Carriers for Enhanced Photocatalysis Dong, Yitong; Choi, Julius; Jeong, Hae-Kwon Journal of the American Chemical Society, Vol. 137, Issue 16 https://doi.org/10.1021/jacs.5b02026	journal	April 2015
Three-Stage Evolution from Nonscalable to Scalable Optical Properties of Thiolate-Protected Gold Nanoclusters Zhou, Meng; Higaki, Tatsuya; Li, Yingwei Journal of the American Chemical Society, Vol. 141, Issue 50 https://doi.org/10.1021/jacs.9b09066	journal	December 2019
Analysis of State-Specific Vibrations Coupled to the Unidirectional Energy Transfer in Conjugated Dendrimers Soler, Miguel A.; Roitberg, Adrian E.; Nelson, Tammie The Journal of Physical Chemistry A, Vol. 116, Issue 40 https://doi.org/10.1021/jp301293e	journal	October 2012
Time-Domain Ab Initio Study of Phonon-Induced Relaxation of Plasmon Excitations in a Silver Quantum Dot Neukirch, Amanda J.; Guo, Zhenyu; Prezhdo, Oleg V. The Journal of Physical Chemistry C, Vol. 116, Issue 28 https://doi.org/10.1021/jp303361y	journal	July 2012
Spectral Properties and Relaxation Dynamics of Surface Plasmon Electronic Oscillations in Gold and Silver Nanodots and Nanorods Link, Stephan; El-Sayed, Mostafa A. The Journal of Physical Chemistry B, Vol. 103, Issue 40 https://doi.org/10.1021/jp9917648	journal	October 1999
Hot Electrons Do the Impossible: Plasmon-Induced Dissociation of H ₂ on Au Mukherjee, Shaunak; Libisch, Florian; Large, Nicolas Nano Letters, Vol. 13, Issue 1 https://doi.org/10.1021/nl303940z	journal	December 2012
Hot-Electron Photodetection with a Plasmonic Nanostripe Antenna Chalabi, Hamidreza; Schoen, David; Brongersma, Mark L. Nano Letters, Vol. 14, Issue 3 https://doi.org/10.1021/nl4044373	journal	February 2014
Auger-Mediated Electron Relaxation Is Robust to Deep Hole Traps: Time-Domain Ab Initio Study of CdSe Quantum Dots Trivedi, Dhara J.; Wang, Linjun; Prezhdo, Oleg V. Nano Letters, Vol. 15, Issue 3 https://doi.org/10.1021/nl504982k	journal	February 2015
Surface Ligands Increase Photoexcitation Relaxation Rates in CdSe Quantum Dots Kilina, Svetlana; Velizhanin, Kirill A.; Ivanov, Sergei ACS Nano, Vol. 6, Issue 7 https://doi.org/10.1021/nn302371q	journal	June 2012
Plasmonic-metal nanostructures for efficient conversion of solar to chemical energy Linic, Suljo; Christopher, Phillip; Ingram, David B. Nature Materials, Vol. 10, Issue 12 https://doi.org/10.1038/nmat3151	journal	November 2011
Photochemical transformations on plasmonic metal nanoparticles Linic, Suljo; Aslam, Umar; Boerigter, Calvin Nature Materials, Vol. 14, Issue 6 https://doi.org/10.1038/nmat4281	journal	May 2015
An autonomous photosynthetic device in which all charge carriers derive from surface plasmons Mubeen, Syed; Lee, Joun; Singh, Nirala Nature Nanotechnology, Vol. 8, Issue 4 https://doi.org/10.1038/nnano.2013.18	journal	February 2013
Plasmon-induced hot carrier science and technology Brongersma, Mark L.; Halas, Naomi J.; Nordlander, Peter Nature Nanotechnology, Vol. 10, Issue 1 https://doi.org/10.1038/nnano.2014.311	journal	January 2015
Single plasmon hot carrier generation in metallic nanoparticles Román Castellanos, Lara; Hess, Ortwin; Lischner, Johannes Communications Physics, Vol. 2, Issue 1 https://doi.org/10.1038/s42005-019-0148-2	journal	May 2019
Optical characterization of single plasmonic nanoparticles Olson, Jana; Dominguez-Medina, Sergio; Hoggard, Anneli Chemical Society Reviews, Vol. 44, Issue 1 https://doi.org/10.1039/c4cs00131a	journal	January 2015
Plasmon-induced hot-carrier generation differences in gold and silver nanoclusters Douglas-Gallardo, Oscar A.; Berdakin, Matías; Frauenheim, Thomas Nanoscale, Vol. 11, Issue 17 https://doi.org/10.1039/c9nr01352k	journal	January 2019
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
Electromagnetic fields around silver nanoparticles and dimers Hao, Encai; Schatz, George C. The Journal of Chemical Physics, Vol. 120, Issue 1, p. 357-366 https://doi.org/10.1063/1.1629280	journal	January 2004
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
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
Perspective: Nonadiabatic dynamics theory Tully, John C. The Journal of Chemical Physics, Vol. 137, Issue 22 https://doi.org/10.1063/1.4757762	journal	December 2012
On the chemical mechanism of surface enhanced Raman scattering: Experiment and theory Kambhampati, Patanjali; Child, C. M.; Foster, Michelle C. The Journal of Chemical Physics, Vol. 108, Issue 12 https://doi.org/10.1063/1.475909	journal	March 1998
DFTB+, a software package for efficient approximate density functional theory based atomistic simulations Hourahine, B.; Aradi, B.; Blum, V. The Journal of Chemical Physics, Vol. 152, Issue 12 https://doi.org/10.1063/1.5143190	journal	March 2020
Nonadiabatic molecular dynamics simulations based on time-dependent density functional tight-binding method Wu, Xiaoyan; Wen, Shizheng; Song, Huajing The Journal of Chemical Physics, Vol. 157, Issue 8 https://doi.org/10.1063/5.0100339	journal	August 2022
Heterometallic antenna−reactor complexes for photocatalysis Swearer, Dayne F.; Zhao, Hangqi; Zhou, Linan Proceedings of the National Academy of Sciences, Vol. 113, Issue 32 https://doi.org/10.1073/pnas.1609769113	journal	July 2016
Shape and size dependence of radiative, non-radiative and photothermal properties of gold nanocrystals Link, Stephan; El-Sayed, Mostafa A. International Reviews in Physical Chemistry, Vol. 19, Issue 3 https://doi.org/10.1080/01442350050034180	journal	July 2000
Tight-binding approach to time-dependent density-functional response theory Niehaus, T. A.; Suhai, S.; Della Sala, F. Physical Review B, Vol. 63, Issue 8 https://doi.org/10.1103/physrevb.63.085108	journal	February 2001
Static polarizabilities and optical absorption spectra of gold clusters ( Au n , n = 2 – 14 and 20) from first principles Idrobo, Juan C.; Walkosz, Weronika; Yip, Shing Fan Physical Review B, Vol. 76, Issue 20 https://doi.org/10.1103/physrevb.76.205422	journal	November 2007
Ab initio study of phonon-induced dephasing of plasmon excitations in silver quantum dots Guo, Zhenyu; Habenicht, Bradley F.; Liang, Wan-Zhen Physical Review B, Vol. 81, Issue 12 https://doi.org/10.1103/physrevb.81.125415	journal	March 2010
Ab initio nanoplasmonics: The impact of atomic structure Zhang, Pu; Feist, Johannes; Rubio, Angel Physical Review B, Vol. 90, Issue 16 https://doi.org/10.1103/physrevb.90.161407	journal	October 2014
Photodetection with Active Optical Antennas Knight, M. W.; Sobhani, H.; Nordlander, P. Science, Vol. 332, Issue 6030, p. 702-704 https://doi.org/10.1126/science.1203056	journal	May 2011
Observing the Multiexciton State in Singlet Fission and Ensuing Ultrafast Multielectron Transfer Chan, W. -L.; Ligges, M.; Jailaubekov, A. Science, Vol. 334, Issue 6062 https://doi.org/10.1126/science.1213986	journal	December 2011
Plasmonics for improved photovoltaic devices Atwater, Harry A.; Polman, Albert Materials for Sustainable Energy https://doi.org/10.1142/9789814317665_0001	book	October 2010
O PTICAL P ROPERTIES AND U LTRAFAST D YNAMICS OF M ETALLIC N ANOCRYSTALS Link, Stephan; El-Sayed, Mostafa A. Annual Review of Physical Chemistry, Vol. 54, Issue 1 https://doi.org/10.1146/annurev.physchem.54.011002.103759	journal	October 2003

Similar Records

Nonadiabatic Molecular Dynamics Simulations Based on Time-Dependent Density Functional Tight-Binding Method

Journal Article · Tue Jul 19 00:00:00 EDT 2022 · Journal of Chemical Physics · OSTI ID:1879390

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Born-Oppenheimer approximation
chemical processes
inorganic and physical chemistry
linear response
materials science
nanoclusters
non-adiabatic molecular dynamics
phonons
plasmons
surface hopping

Investigation of plasmon relaxation mechanisms using nonadiabatic molecular dynamics

Citation Formats

References (70)

Similar Records

Related Subjects