Tuning Electron-Phonon Interactions in Nanocrystals through Surface Termination

Nuri Yazdani; Deniz Bozyigit; Kantawong Vuttivorakulchai; Mathieu Luisier; Ivan Infante; Vanessa Wood

doi:10.1021/acs.nanolett.7b04729

Tuning Electron-Phonon Interactions in Nanocrystals through Surface Termination

Nuri Yazdani, Deniz Bozyigit, Kantawong Vuttivorakulchai, Mathieu Luisier, Ivan Infante, Vanessa Wood^*

^*Corresponding author for this work

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

We perform ab initio molecular dynamics on experimentally relevant-sized lead sulfide (PbS) nanocrystals (NCs) constructed with thiol or Cl, Br, and I anion surfaces to determine their vibrational and dynamic electronic structure. We show that electron-phonon interactions can explain the large thermal broadening and fast carrier cooling rates experimentally observed in Pb-chalcogenide NCs. Furthermore, our simulations reveal that electron-phonon interactions are suppressed in halide-terminated NCs due to reduction of both the thermal displacement of surface atoms and the spatial overlap of the charge carriers with these large atomic vibrations. This work shows how surface engineering, guided by simulations, can be used to systematically control carrier dynamics.

Original language	English
Pages (from-to)	2233-2242
Number of pages	10
Journal	Nano Letters
Volume	18
Issue number	4
Early online date	2 Mar 2018
DOIs	https://doi.org/10.1021/acs.nanolett.7b04729
Publication status	Published - 11 Apr 2018

Funding

The authors acknowledge an ETH Research Grant (N.Y), the Swiss National Science Foundation Quantum Sciences and Technology NCCR (D.B. and N.Y.), the Swiss National Science Foundation project 149454/TORNAD (K.V.), and The Netherlands Organization of Scientific Research (NWO) Innovational Research Incentive (Vidi) Scheme (Grant 723.013.002) (I.I.). This work was done in collaboration with the Dutch eScience center. Computations were supported by a grant from the Swiss National Supercomputing Centre (CSCS; project ID s674).

Funders	Funder number
Swiss National Science Foundation Quantum Sciences and Technology NCCR
Swiss National Supercomputing Centre
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	149454/TORNAD
Eidgenössische Technische Hochschule Zürich
Nederlandse Organisatie voor Wetenschappelijk Onderzoek	723.013.002

Keywords

carrier cooling
electron-phonon coupling
Nanocrystals
phonons
quantum dots
thermal broadening

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1021/acs.nanolett.7b04729

Persistent URL (handle)

Copy link address

Cite this

@article{e58581c587a54e36b2cecdcee6027570,

title = "Tuning Electron-Phonon Interactions in Nanocrystals through Surface Termination",

abstract = "We perform ab initio molecular dynamics on experimentally relevant-sized lead sulfide (PbS) nanocrystals (NCs) constructed with thiol or Cl, Br, and I anion surfaces to determine their vibrational and dynamic electronic structure. We show that electron-phonon interactions can explain the large thermal broadening and fast carrier cooling rates experimentally observed in Pb-chalcogenide NCs. Furthermore, our simulations reveal that electron-phonon interactions are suppressed in halide-terminated NCs due to reduction of both the thermal displacement of surface atoms and the spatial overlap of the charge carriers with these large atomic vibrations. This work shows how surface engineering, guided by simulations, can be used to systematically control carrier dynamics.",

keywords = "carrier cooling, electron-phonon coupling, Nanocrystals, phonons, quantum dots, thermal broadening",

author = "Nuri Yazdani and Deniz Bozyigit and Kantawong Vuttivorakulchai and Mathieu Luisier and Ivan Infante and Vanessa Wood",

year = "2018",

month = apr,

day = "11",

doi = "10.1021/acs.nanolett.7b04729",

language = "English",

volume = "18",

pages = "2233--2242",

journal = "Nano Letters",

issn = "1530-6984",

publisher = "American Chemical Society",

number = "4",

}

TY - JOUR

T1 - Tuning Electron-Phonon Interactions in Nanocrystals through Surface Termination

AU - Yazdani, Nuri

AU - Bozyigit, Deniz

AU - Vuttivorakulchai, Kantawong

AU - Luisier, Mathieu

AU - Infante, Ivan

AU - Wood, Vanessa

PY - 2018/4/11

Y1 - 2018/4/11

N2 - We perform ab initio molecular dynamics on experimentally relevant-sized lead sulfide (PbS) nanocrystals (NCs) constructed with thiol or Cl, Br, and I anion surfaces to determine their vibrational and dynamic electronic structure. We show that electron-phonon interactions can explain the large thermal broadening and fast carrier cooling rates experimentally observed in Pb-chalcogenide NCs. Furthermore, our simulations reveal that electron-phonon interactions are suppressed in halide-terminated NCs due to reduction of both the thermal displacement of surface atoms and the spatial overlap of the charge carriers with these large atomic vibrations. This work shows how surface engineering, guided by simulations, can be used to systematically control carrier dynamics.

AB - We perform ab initio molecular dynamics on experimentally relevant-sized lead sulfide (PbS) nanocrystals (NCs) constructed with thiol or Cl, Br, and I anion surfaces to determine their vibrational and dynamic electronic structure. We show that electron-phonon interactions can explain the large thermal broadening and fast carrier cooling rates experimentally observed in Pb-chalcogenide NCs. Furthermore, our simulations reveal that electron-phonon interactions are suppressed in halide-terminated NCs due to reduction of both the thermal displacement of surface atoms and the spatial overlap of the charge carriers with these large atomic vibrations. This work shows how surface engineering, guided by simulations, can be used to systematically control carrier dynamics.

KW - carrier cooling

KW - electron-phonon coupling

KW - Nanocrystals

KW - phonons

KW - quantum dots

KW - thermal broadening

UR - http://www.scopus.com/inward/record.url?scp=85045016023&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85045016023&partnerID=8YFLogxK

U2 - 10.1021/acs.nanolett.7b04729

DO - 10.1021/acs.nanolett.7b04729

M3 - Article

AN - SCOPUS:85045016023

SN - 1530-6984

VL - 18

SP - 2233

EP - 2242

JO - Nano Letters

JF - Nano Letters

IS - 4

ER -

Tuning Electron-Phonon Interactions in Nanocrystals through Surface Termination

Abstract

Funding

Keywords

UN SDGs

Access to Document

Persistent URL (handle)

Other files and links

Fingerprint

Cite this