Regulating the femtosecond excited-state lifetime of a single molecule

Research output: Contribution to journalArticle

5 Citations (Scopus)
43 Downloads (Pure)

Abstract

The key to controlling reactions of molecules induced with the current of a scanning tunneling microscope (STM) tip is the ultrashort intermediate excited ionic state. The initial condition of the excited state is set by the energy and position of the injected current; thereafter, its dynamics determines the reaction outcome. We show that a STM can directly and controllably influence the excited-state dynamics. For the STM-induced desorption of toluene molecules from the Si(111)-7x7 surface, as the tip approaches the molecule, the probability of manipulation drops by two orders of magnitude. A two-channel quenching of the excited state is proposed, consisting of an invariant surface channel and a tip height–dependent channel. We conclude that picometer tip proximity regulates the lifetime of the excited state from 10 femtoseconds to less than 0.1 femtoseconds.

Original languageEnglish
Pages (from-to)1012-1016
Number of pages5
JournalScience
Volume361
Issue number6406
Early online date7 Sep 2018
DOIs
Publication statusPublished - 7 Sep 2018

Fingerprint

life (durability)
microscopes
excitation
scanning
molecules
toluene
proximity
manipulators
desorption
quenching
energy

ASJC Scopus subject areas

  • General

Cite this

Regulating the femtosecond excited-state lifetime of a single molecule. / Rusimova, Kristina; Purkiss, Rebecca; Howes, R; Lee, Frank; Crampin, Simon; Sloan, Peter.

In: Science, Vol. 361, No. 6406, 07.09.2018, p. 1012-1016.

Research output: Contribution to journalArticle

@article{57236463b29942be87ff6c3d71f62632,
title = "Regulating the femtosecond excited-state lifetime of a single molecule",
abstract = "The key to controlling reactions of molecules induced with the current of a scanning tunneling microscope (STM) tip is the ultrashort intermediate excited ionic state. The initial condition of the excited state is set by the energy and position of the injected current; thereafter, its dynamics determines the reaction outcome. We show that a STM can directly and controllably influence the excited-state dynamics. For the STM-induced desorption of toluene molecules from the Si(111)-7x7 surface, as the tip approaches the molecule, the probability of manipulation drops by two orders of magnitude. A two-channel quenching of the excited state is proposed, consisting of an invariant surface channel and a tip height–dependent channel. We conclude that picometer tip proximity regulates the lifetime of the excited state from 10 femtoseconds to less than 0.1 femtoseconds.",
author = "Kristina Rusimova and Rebecca Purkiss and R Howes and Frank Lee and Simon Crampin and Peter Sloan",
year = "2018",
month = "9",
day = "7",
doi = "10.1126/science.aat9688",
language = "English",
volume = "361",
pages = "1012--1016",
journal = "Science",
issn = "0036-8075",
publisher = "American Association for the Advancement of Science",
number = "6406",

}

TY - JOUR

T1 - Regulating the femtosecond excited-state lifetime of a single molecule

AU - Rusimova, Kristina

AU - Purkiss, Rebecca

AU - Howes, R

AU - Lee, Frank

AU - Crampin, Simon

AU - Sloan, Peter

PY - 2018/9/7

Y1 - 2018/9/7

N2 - The key to controlling reactions of molecules induced with the current of a scanning tunneling microscope (STM) tip is the ultrashort intermediate excited ionic state. The initial condition of the excited state is set by the energy and position of the injected current; thereafter, its dynamics determines the reaction outcome. We show that a STM can directly and controllably influence the excited-state dynamics. For the STM-induced desorption of toluene molecules from the Si(111)-7x7 surface, as the tip approaches the molecule, the probability of manipulation drops by two orders of magnitude. A two-channel quenching of the excited state is proposed, consisting of an invariant surface channel and a tip height–dependent channel. We conclude that picometer tip proximity regulates the lifetime of the excited state from 10 femtoseconds to less than 0.1 femtoseconds.

AB - The key to controlling reactions of molecules induced with the current of a scanning tunneling microscope (STM) tip is the ultrashort intermediate excited ionic state. The initial condition of the excited state is set by the energy and position of the injected current; thereafter, its dynamics determines the reaction outcome. We show that a STM can directly and controllably influence the excited-state dynamics. For the STM-induced desorption of toluene molecules from the Si(111)-7x7 surface, as the tip approaches the molecule, the probability of manipulation drops by two orders of magnitude. A two-channel quenching of the excited state is proposed, consisting of an invariant surface channel and a tip height–dependent channel. We conclude that picometer tip proximity regulates the lifetime of the excited state from 10 femtoseconds to less than 0.1 femtoseconds.

UR - http://www.scopus.com/inward/record.url?scp=85052892788&partnerID=8YFLogxK

U2 - 10.1126/science.aat9688

DO - 10.1126/science.aat9688

M3 - Article

VL - 361

SP - 1012

EP - 1016

JO - Science

JF - Science

SN - 0036-8075

IS - 6406

ER -