Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure

ACS Nano
Tuomas P RossiMikael Kuisma

Abstract

Metal nanoparticles are attractive for plasmon-enhanced generation of hot carriers, which may be harnessed in photochemical reactions. In this work, we analyze the coherent femtosecond dynamics of photon absorption, plasmon formation, and subsequent hot-carrier generation through plasmon dephasing using first-principles simulations. We predict the energetic and spatial hot-carrier distributions in small metal nanoparticles and show that the distribution of hot electrons is very sensitive to the local structure. Our results show that surface sites exhibit enhanced hot-electron generation in comparison to the bulk of the nanoparticle. Although the details of the distribution depend on particle size and shape, as a general trend, lower-coordinated surface sites such as corners, edges, and {100} facets exhibit a higher proportion of hot electrons than higher-coordinated surface sites such as {111} facets or the core sites. The present results thereby demonstrate how hot carriers could be tailored by careful design of atomic-scale structures in nanoscale systems.

References

Feb 1, 1996·Journal of Molecular Graphics·W HumphreyK Schulten
Nov 1, 1991·Physical Review. a·C Yannouleas, R A Broglia
Mar 1, 1995·Physical Review. a·O GritsenkoE J Baerends
Dec 15, 1994·Physical Review. B, Condensed Matter·P E Blöchl
Aug 15, 1996·Physical Review. B, Condensed Matter·K Yabana, G F Bertsch
Jul 17, 1989·Physical Review Letters·C YannouleasP F Bortignon
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Feb 20, 2010·Nature Materials·Harry A Atwater, Albert Polman
Mar 12, 2011·Journal of Physics. Condensed Matter : an Institute of Physics Journal·J EnkovaaraK W Jacobsen
May 10, 2011·Science·Mark W KnightNaomi J Halas
Dec 1, 2012·Nano Letters·Shaunak MukherjeeNaomi J Halas
Feb 26, 2013·Nature Nanotechnology·Syed MubeenMartin Moskovits
Feb 8, 2014·Nano Letters·Hamidreza ChalabiMark L Brongersma
Jun 25, 2014·ACS Nano·Alejandro ManjavacasPeter Nordlander
Dec 17, 2014·Nature Communications·Ravishankar SundararamanHarry A Atwater
Jan 7, 2015·Nature Nanotechnology·Mark L BrongersmaPeter Nordlander
Mar 10, 2015·The Journal of Chemical Physics·Tuomas P RossiRisto M Nieminen
May 21, 2015·Nature Materials·Suljo LinicMatthew Morabito
Jun 3, 2015·Nature Communications·Marco BernardiSteven G Louie
Aug 8, 2015·Science·Matthew J Kale, Phillip Christopher
Dec 18, 2015·Nature Communications·Jie MaLin-Wang Wang
Dec 20, 2015·Physical Review Letters·Tuomas P RossiRisto M Nieminen
Jul 23, 2016·Proceedings of the National Academy of Sciences of the United States of America·Dayne F SwearerNaomi J Halas
Mar 11, 2017·Physical Review Letters·Ana M BrownHarry A Atwater
Mar 17, 2017·ACS Nano·Benjamin FoersterCarsten Sönnichsen
Mar 17, 2017·Annual Review of Physical Chemistry·Phillip Christopher, Martin Moskovits
Mar 23, 2017·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Ask Hjorth LarsenKarsten W Jacobsen
Apr 13, 2017·Journal of the American Chemical Society·Shijing TanHrvoje Petek
Jun 27, 2017·ACS Nano·Runmin ZhangPeter Nordlander
Jul 1, 2017·Nano Letters·Gururaj V NaikJennifer A Dionne
Dec 20, 2017·The Journal of Physical Chemistry Letters·Xinyuan YouTamar Seideman
Apr 26, 2018·Physical Review Letters·Shijing TanHrvoje Petek
Feb 16, 2019·ACS Nano·Priyank V KumarDavid J Norris
Mar 12, 2019·Faraday Discussions·Priyank V KumarDavid J Norris
Apr 18, 2019·Nanoscale·Oscar A Douglas-GallardoCristián G Sánchez
May 17, 2019·Faraday Discussions·Javier AizpuruaAnatoly Zayats
Oct 28, 2019·Light, Science & Applications·Yonatan Dubi, Yonatan Sivan
Mar 17, 2020·The Journal of Chemical Physics·Lara Román CastellanosJohannes Lischner

❮ Previous
Next ❯

Citations

Apr 29, 2021·Accounts of Chemical Research·Zhandong Li, Dmitry Kurouski

❮ Previous
Next ❯

Methods Mentioned

BETA
surface plasmon resonance

Software Mentioned

VMD
ASE
Matplotlib
NumPy
GPAW
TDDFT

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.