Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Atomic-scale quantum sensing based on the ultrafast coherence of an H 2 molecule in an STM cavity

Journal Article · · Science
 [1];  [1];  [2]
  1. Department of Physics and Astronomy, University of California, Irvine, CA 92697, USA.
  2. Department of Physics and Astronomy, University of California, Irvine, CA 92697, USA.; Department of Chemistry, University of California, Irvine, CA 92697, USA.

A scanning tunneling microscope (STM) combined with a pump-probe femtosecond terahertz (THz) laser can enable coherence measurements of single molecules. We report THz pump-probe measurements that demonstrate quantum sensing based on a hydrogen (H2) molecule in the cavity created with an STM tip near a surface. Atomic-scale spatial and femtosecond temporal resolutions were obtained from this quantum coherence. The H2acts as a two-level system, with its coherent superposition exhibiting extreme sensitivity to the applied electric field and the underlying atomic composition of the copper nitride (Cu2N) monolayer islands grown on a Cu(100) surface. We acquired time-resolved images of THz rectification of H2over Cu2N islands for variable pump-probe delay times to visualize the heterogeneity of the chemical environment at sub-angstrom scale.

Research Organization:
Univ. of California, Irvine, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
DOE Contract Number:
SC0019448
OSTI ID:
1980746
Journal Information:
Science, Vol. 376, Issue 6591; ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English

References (36)

Quantum sensing journal July 2017
Towards quantum sensing with molecular spins journal December 2019
Quantum control of proximal spins using nanoscale magnetic resonance imaging journal May 2011
Nanoscale nuclear magnetic resonance with chemical resolution journal June 2017
A robust scanning diamond sensor for nanoscale imaging with single nitrogen-vacancy centres journal April 2012
Nanoscale electric-field imaging based on a quantum sensor and its charge-state control under ambient condition journal April 2021
Ultrasensitive detection of force and displacement using trapped ions journal August 2010
Scanning Single-Electron Transistor Microscopy: Imaging Individual Charges journal April 1997
Observation of electron–hole puddles in graphene using a scanning single-electron transistor journal November 2007
Probing and imaging spin interactions with a magnetic single-molecule sensor journal May 2019
Quantitative imaging of electric surface potentials with single-atom sensitivity journal June 2019
Electron spin resonance of single iron phthalocyanine molecules and role of their non-localized spins in magnetic interactions journal November 2021
Probing quantum coherence in single-atom electron spin resonance journal February 2018
Atomic-scale sensing of the magnetic dipolar field from single atoms journal March 2017
Coherent spin manipulation of individual atoms on a surface journal October 2019
Electron paramagnetic resonance of individual atoms on a surface journal October 2015
Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging journal November 2016
Sub-cycle atomic-scale forces coherently control a single-molecule switch journal September 2020
High-Power Terahertz Generation Using Large-Area Plasmonic Photoconductive Emitters journal March 2015
Strongly coverage-dependent excitations of adsorbed molecular hydrogen journal March 2005
Enhanced resolution imaging of ultrathin ZnO layers on Ag(111) by multiple hydrogen molecules in a scanning tunneling microscope junction journal May 2018
Interaction of hydrogen with metal nitrides and imides journal November 2002
Resonant-Enhanced Spectroscopy of Molecular Rotations with a Scanning Tunneling Microscope journal June 2014
Distinction of Nuclear Spin States with the Scanning Tunneling Microscope journal October 2013
Rotational and Vibrational Excitations of a Hydrogen Molecule Trapped within a Nanocavity of Tunable Dimension journal October 2013
Rotational Spectromicroscopy: Imaging the Orbital Interaction between Molecular Hydrogen and an Adsorbed Molecule journal May 2015
Atomic-scale intermolecular interaction of hydrogen with a single VOPc molecule on the Au(111) surface journal January 2021
Huge negative differential conductance inAu−H2molecular nanojunctions journal February 2008
Vibrationally Induced Two-Level Systems in Single-Molecule Junctions journal December 2006
Trapping and Characterization of a Single Hydrogen Molecule in a Continuously Tunable Nanocavity journal August 2015
Incommensurability and atomic structure of c ( 2 × 2 ) N / Cu ( 100 ) : A scanning tunneling microscopy study journal July 2008
Large Magnetic Anisotropy of a Single Atomic Spin Embedded in a Surface Molecular Network journal August 2007
Spectroscopy and Microscopy of Spin-Sensitive Rectification Current Induced by Microwave Radiation journal November 2005
Atomic-scale rectification at microwave frequency journal January 2006
CO Tip Functionalization Inverts Atomic Force Microscopy Contrast via Short-Range Electrostatic Forces journal April 2014
Ion-Selective, Atom-Resolved Imaging of a 2D Cu 2 N Insulator: Field and Current Driven Tip-Enhanced Raman Spectromicroscopy Using a Molecule-Terminated Tip journal May 2019