Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

The Journal of Chemical Physics

Pump–probe spectroscopy and photophysical properties of single di-benzanthanthrene molecules in a naphthalene crystal

Fedor Jelezko, Brahim Lounis, Michel Orrit

Published Aug 8, 1997• 64 citations
Publisher

Abstract

We report on a new crystalline host–guest system for single molecule spectroscopy; dibenzanthanthrene (DBATT) in a naphthalene crystal. As compared to DBATT in an n-hexadecane Shpol’skii matrix (a combination studied earlier), this system is shifted to the red (618.7 nm), has a lower triplet yield and shorter triplet lifetimes. Thanks to the narrow lines of this system (20 MHz), to its high photostability and to the absence of spectral diffusion, even in strained crystals, we could measure line shapes and widths with great accuracy. As an illustration of the potential of this new system for quantum optical experiments, we present pump–probe experiments with strong laser fields. The experiments are in very good agreement with calculations based on Bloch’s equations, demonstrating the validity of these equations for single molecules in solids under intense resonant fields.

DOI
10.1063/1.474525

Related papers

Single Molecules Driven by Strong Resonant Fields: Hyper-Raman and Subharmonic Resonances

Brahim Lounis, Fedor Jelezko, Michel Orrit

We present pump-probe experiments on single molecules in a solid matrix, with strong laser fields and a new host-guest system, dibenzanthanthrene in a naphthalene crystal. Besides strong light-shifts of the lines, we observe the hyper-Raman resonance, for the first time in condensed matter. For strong pump and probe, we also observe subharmonic resonances due to a''kicked pendulum'' motion of the Bloch vector. Since our results agree with Bloch's equations without any adjustable parameter, they provide a stringent test of the optical two-level model as applied to single molecules in solids.

Physical Review Letters•May 12, 1997•51 citations

Optical Spectroscopy of Single Impurity Molecules in Solids

W. E. Moerner, Thomas Basché

Abstract Optical spectroscopy of a single impurity molecule provides the first truly local probe of host–guest interactions in doped solids. In conventional optical high‐resolution experiments with many molecules only ensemble averages of the microscopic parameters can be obtained. In the single‐molecule regime, the exquisite sensitivity of an individual dopant molecule to both the local environment and to external perturbations has been exploited in recent experiments to reveal a wealth of fascinating novel phenomena such as spectral diffusion in crystals and polymers, optical modification of a single impurity molecule (spectral hole‐burning), local field measurements at the site of a single impurity molecule, and quantum optics in a solid.

Angewandte Chemie International Edition in English•Apr 1, 1993•192 citations

Sub-nanosecond coherent optical manipulation of a single aromatic molecule at cryogenic temperature

Quentin Deplano, Philippe Tamarat, Brahim Lounis +1 more

Single molecules trapped in the solid state at liquid helium temperatures are promising quantum emitters for the development of quantum technologies owing to their remarkable photostability and their lifetime-limited optical coherence time of the order of 10 ns. The coherent preparation of their electronic state requires resonant excitation with a Rabi period much shorter than their optical coherence time. Sculpting the optical excitation with sharp edges and a high on–off intensity ratio (∼3 × 105) from a single-frequency laser beam, we demonstrate sub-nanosecond drive of a single dibenzanthanthrene molecule embedded in a naphthalene matrix at 3.2 K, over more than 17 Rabi periods. With pulses tailored for a half-Rabi period, the electronic excited state is prepared with fidelity as high as 0.97. Using single-molecule Ramsey spectroscopy, we prove up to 5 K that the optical coherence lifetime remains at its fundamental upper limit set by twice the excited-state lifetime, making single molecules suitable for quantum bit manipulations under standard cryogen-free cooling technologies.

arXiv:2312.03359•AVS Quantum Science•Dec 1, 2023•2 citations

Optical Spectroscopy on Single Molecules in Solids

Daniel Walser

Experiments with single quantum systems are at the frontier of modern physics. Probing single molecules allows for very precise control of light-matter interaction and for quantum optical studies. Moreover, a single guest molecule in a solid host matrix is a very sensitive probe of local dynamics in its nano-environment. Fluorescence excitation spectroscopy on single molecules is a powerful tool for spectroscopic characterizations at highest resolution, as information can be revealed that is not accessible in experiments on ensembles of molecules. The detection of the fluorescence signal of a single absorber is achieved by exploiting the high spectral selectivity given by the ratio (10 10) of homogeneous to inhomogeneous linewidths of optical transitions at cryogenic temperatures (zero-phonon transitions). Two-photon fluorescence excitation, a fundamental nonlinear optical process, was observed on a single quantum system [1]. Single diphenyl-octatetraene molecules trapped in an n-tetradecane matrix were excited from the 1Ag ground to the lowest excited singlet state by simultaneous absorption of two photons using a single-mode cw laser. Excited molecules were observed through weak one-photon emission resulting from a symmetry breaking induced by the crystal field. The fundamental principles and the experimental technique of single molecule spectroscopy will be introduced briefly and some particular single molecule experiments presented. This work was done in collaboration with T. Plakhotnik, A. Renn and U.P. Wild

Kluwer Academic Publishers eBooks•Mar 5, 2006•1 citation

Pump-Probe Experiments with a Single Molecule: ac-Stark Effect and Nonlinear Optical Response

Philippe Tamarat, Brahim Lounis, J. Bernard +5 more

We have measured the ac-Stark effect on single terrylene molecules in $p$-terphenyl crystals at superfluid helium temperatures. With the pump beam far enough from resonance, the molecular transition shifts as expected, i.e., proportional to the pump intensity and to the inverse pump detuning. Experiments closer to resonance with stronger beams show Autler-Townes-like structures that can be well reproduced by means of Bloch equations with two intense laser fields. These experiments are a demonstration of nonlinear optical effects with the localized electronic states of a single molecule trapped in a solid.

Physical Review Letters•Aug 21, 1995•97 citations

Single organic molecules for applications in quantum technology

Alex S. Clark

Single organic molecules hold great promise for generating, manipulating, and storing single photons. Such processes form the basis for new quantum-enhanced technologies such as sensing, communications, and computation. In this talk I will focus on a particularly promising molecule – dibenzoterrylene (DBT). When DBT is introduced into a solid crystal of anthracene it is photostable and emits light between 780 and 795 nm. When cooled to cryogenic temperature, DBT is isolated from phonon-induced dephasing meaning that the photons have a lifetime-limited. I will present recent results in growing DBT-doped anthracene crystals, introducing these to nanophotonic interfaces for enhancing the collection of photons, tuning the DBT emission wavelength to coincide with rubidium atomic absorption, and finally pump-probe spectroscopy experiments to find long-lived triplet states in DBT which will be useful for building a single-molecule quantum memory.

Physical Chemistry of Semiconductor Materials and Interfaces•Aug 20, 2020•0 citations
We report on a new crystalline host–guest system for single molecule spectroscopy; dibenzanthanthrene (DBATT) in a naphthalene crystal. As compared to DBATT in an n-hexadecane Shpol’skii matrix (a combination studied earlier), this system is shifted to the red (618.7 nm), has a lower triplet yield and shorter triplet lifetimes. Thanks to the narrow lines of this system (20 MHz), to its high photostability and to the absence of spectral diffusion, even in strained crystals, we could measure line shapes and widths with great accuracy. As an illustration of the potential of this new system for quantum optical experiments, we present pump–probe experiments with strong laser fields. The experiments are in very good agreement with calculations based on Bloch’s equations, demonstrating the validity of these equations for single molecules in solids under intense resonant fields.
We present pump-probe experiments on single molecules in a solid matrix, with strong laser fields and a new host-guest system, dibenzanthanthrene in a naphthalene crystal. Besides strong light-shifts of the lines, we observe the hyper-Raman resonance, for the first time in condensed matter. For strong pump and probe, we also observe subharmonic resonances due to a''kicked pendulum'' motion of the Bloch vector. Since our results agree with Bloch's equations without any adjustable parameter, they provide a stringent test of the optical two-level model as applied to single molecules in solids.
Abstract Optical spectroscopy of a single impurity molecule provides the first truly local probe of host–guest interactions in doped solids. In conventional optical high‐resolution experiments with many molecules only ensemble averages of the microscopic parameters can be obtained. In the single‐molecule regime, the exquisite sensitivity of an individual dopant molecule to both the local environment and to external perturbations has been exploited in recent experiments to reveal a wealth of fascinating novel phenomena such as spectral diffusion in crystals and polymers, optical modification of a single impurity molecule (spectral hole‐burning), local field measurements at the site of a single impurity molecule, and quantum optics in a solid.
Single molecules trapped in the solid state at liquid helium temperatures are promising quantum emitters for the development of quantum technologies owing to their remarkable photostability and their lifetime-limited optical coherence time of the order of 10 ns. The coherent preparation of their electronic state requires resonant excitation with a Rabi period much shorter than their optical coherence time. Sculpting the optical excitation with sharp edges and a high on–off intensity ratio (∼3 × 105) from a single-frequency laser beam, we demonstrate sub-nanosecond drive of a single dibenzanthanthrene molecule embedded in a naphthalene matrix at 3.2 K, over more than 17 Rabi periods. With pulses tailored for a half-Rabi period, the electronic excited state is prepared with fidelity as high as 0.97. Using single-molecule Ramsey spectroscopy, we prove up to 5 K that the optical coherence lifetime remains at its fundamental upper limit set by twice the excited-state lifetime, making single molecules suitable for quantum bit manipulations under standard cryogen-free cooling technologies.
Experiments with single quantum systems are at the frontier of modern physics. Probing single molecules allows for very precise control of light-matter interaction and for quantum optical studies. Moreover, a single guest molecule in a solid host matrix is a very sensitive probe of local dynamics in its nano-environment. Fluorescence excitation spectroscopy on single molecules is a powerful tool for spectroscopic characterizations at highest resolution, as information can be revealed that is not accessible in experiments on ensembles of molecules. The detection of the fluorescence signal of a single absorber is achieved by exploiting the high spectral selectivity given by the ratio (10 10) of homogeneous to inhomogeneous linewidths of optical transitions at cryogenic temperatures (zero-phonon transitions). Two-photon fluorescence excitation, a fundamental nonlinear optical process, was observed on a single quantum system [1]. Single diphenyl-octatetraene molecules trapped in an n-tetradecane matrix were excited from the 1Ag ground to the lowest excited singlet state by simultaneous absorption of two photons using a single-mode cw laser. Excited molecules were observed through weak one-photon emission resulting from a symmetry breaking induced by the crystal field. The fundamental principles and the experimental technique of single molecule spectroscopy will be introduced briefly and some particular single molecule experiments presented. This work was done in collaboration with T. Plakhotnik, A. Renn and U.P. Wild
We have measured the ac-Stark effect on single terrylene molecules in ppp-terphenyl crystals at superfluid helium temperatures. With the pump beam far enough from resonance, the molecular transition shifts as expected, i.e., proportional to the pump intensity and to the inverse pump detuning. Experiments closer to resonance with stronger beams show Autler-Townes-like structures that can be well reproduced by means of Bloch equations with two intense laser fields. These experiments are a demonstration of nonlinear optical effects with the localized electronic states of a single molecule trapped in a solid.
Single organic molecules hold great promise for generating, manipulating, and storing single photons. Such processes form the basis for new quantum-enhanced technologies such as sensing, communications, and computation. In this talk I will focus on a particularly promising molecule – dibenzoterrylene (DBT). When DBT is introduced into a solid crystal of anthracene it is photostable and emits light between 780 and 795 nm. When cooled to cryogenic temperature, DBT is isolated from phonon-induced dephasing meaning that the photons have a lifetime-limited. I will present recent results in growing DBT-doped anthracene crystals, introducing these to nanophotonic interfaces for enhancing the collection of photons, tuning the DBT emission wavelength to coincide with rubidium atomic absorption, and finally pump-probe spectroscopy experiments to find long-lived triplet states in DBT which will be useful for building a single-molecule quantum memory.