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

Physical Review A

Photon emission from a single molecule in a solid matrix: Phase-delay control

Yonggang Peng, Yujun Zheng

Published Jul 30, 2013• 10 citations
Publisher

Abstract

In this paper, we study the influence of time-dependent phase delay on the emission of few photons from a single molecule in a solid matrix. The results demonstrate that a time-dependent phase of the pulses can be used to control the photon emission and strongly affects the spectrum of single molecules. The spectrum of the photon emission probabilities reflects the fast dynamics of the states of the system when the duration of the driven laser pulses is short. Also, it is shown that the coupling between the system and the rf field strongly affects the spectrum of the photon emission probabilities in space.

DOI
10.1103/physreva.88.013425

Related papers

Control of the photon emission of single molecules in a solid matrix

Baiping Han, Yujun Zheng

We consider the photon spontaneous emission of single molecules in a solid matrix with spectral diffusion. A general theoretical strategy for calculating the photon emission statistics in a solid matrix of single molecules is derived. In particular, the control photon emission from single molecules in a solid matrix driven simultaneously by a laser and an electric radiofrequency (rf) field is investigated. The photon emission of single molecules can be modulated by an rf field. The formulation also allows for the study of the average waiting time for the emission event of a single molecule.

Physical Review A•Jul 16, 2008•23 citations

Photon emission from a driven single-molecule source: A renormalization group approach

Igor Rozhkov, Eli Barkai

The photon emission from a single molecule driven simultaneously by a laser and a slow electric radio frequency (rf) field is studied. We use a non-Hermitian Hamiltonian approach which accounts for the radiative decay of a two-level system modeling the single-molecule source. We apply the renormalization group method for differential equations to obtain long time solution of the corresponding Schrodinger equation, which allows us to calculate the average waiting time for the first photon emission. Then, we analyze the conditions for suppression and enhancement of photon emission in this dissipative two-level system. In particular we derive a transcendental equation, which yields the nontrivial rf field control parameters, for which enhancement and suppression of photon emission occurs. For finite values of radiative decay rate an abrupt transition to the state when both situations are indistinguishable is found for certain values of the rf field parameters. Our results are shown to be in agreement with the available experiments [Ch. Brunel et al., Phys. Rev. Lett. 81, 2679 (1998)].

The Journal of Chemical Physics•Aug 15, 2005•8 citations

Temporal shaping of single-photon pulses

Gaston Hornecker, Emanuel Peinke, Julien Claudon +2 more

The ability to control the temporal shape of single-photon pulses is highly desirable in quantum information processing. For instance, it has been shown that Gaussian pulses are best suited for linear optics quantum computing1. By mimicking the time-reversal of a spontaneous emission event, it also allows to optimize the absorption of the prepared photons by a quantum emitter. In this work we investigate the potential of using fast modifications of the detuning between an atomic system and a cavity mode during photon emission to reach this goal. We compare two approaches consisting of varying the emitter or cavity frequency. The latter, achievable by a fast modification of the refractive index of a solid state cavity, will be shown to have negligible influence on the photon spectrum. It allows to create Gaussian pulses interacting with a fidelity to the target photons of 99%, as well as time-reversed photons absorbed by an atom in a cavity with a probability of 93%.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•May 7, 2015•4 citations

Coherent Destruction of Photon Emission from a Single Molecule Source: A Renormalization Group Approach

Igor Rozhkov, Eli Barkai

The photon emission from a single molecule driven simultaneously by a laser and a slow electric radio frequency (rf) field is studied. We use a non-Hermitian Hamiltonian approach which accounts for the radiative decay of a two level system modeling a single molecule source. We apply the renormalization group method for differential equations to obtain long time solution of the corresponding Schrdinger equation, which allows us to calculate the average waiting time for the first photon emission. Then, we analyze the conditions for suppression and enhancement of photon emission in this dissipative two-level system. In particular we derive a transcendental equation, which yields the non-trivial rf field control parameters, for which enhancement and suppression of photon emission occurs. For finite values of radiative decay rate an abrupt transition from the molecule's localization in its ground state to delocalization is found for certain critical values of the rf field parameters. Our results are shown to be in agreement with the available experiments [Ch. Brunel et al, Phys. Rev. Lett. 81, 2679 (1998)].

arXiv:cond-mat/0407301•Jul 12, 2004•0 citations

Shaped and Feedback-Controlled Excitation of Single Molecules in the Weak-Field Limit

Alexander Weigel, Aleksandar Sebesta, Philipp Kukura

Coherent control uses tailored femtosecond pulse shapes to influence quantum pathways and drive a light-induced process toward a specific outcome. There has been a long-standing debate whether the absorption properties or the probability for population to remain in an excited state of a molecule can be influenced by the pulse shape, even if only a single photon is absorbed. Most such experiments are performed on many molecules simultaneously, so that ensemble averaging reduces the access to quantum effects. Here, we demonstrate systematic coherent control experiments on the fluorescence intensity of a single molecule in the weak-field limit. We demonstrate that a delay scan of interfering pulses reproduces the excitation spectrum of the molecule upon Fourier transformation, but that the spectral phase of a pulse sequence does not affect the transition probability. We generalize this result to arbitrary pulse shapes by performing the first closed-loop coherent control experiments on a single molecule.

The Journal of Physical Chemistry Letters•Sep 17, 2015•35 citations

On the effects of absolute laser phase on the interaction of a pulsed laser with polar versus nonpolar molecules

Alex Brown, William J. Meath

The absolute laser phase dependence of the time-dependent populations of the molecular states, including the steady-state (long time) populations of the states, associated with the interaction of a molecule with a pulsed laser is investigated using illustrative two-level examples. One-photon transitions, including the effects of permanent dipoles, are discussed as a function of the pulse duration, intensity, and (absolute) laser phase, for selected laser frequencies. The effects of laser phase can be large, depending on the values of the pulse duration for a given frequency and intensity. The effects of permanent dipoles, relative to no permanent dipoles, are significant for large laser field strengths ε0. When the laser-molecule coupling parameter b=μ12ε0/E21⩾0.2, where μ12 and E21 are the transition dipole and energy difference between the ground and excited states, respectively, the dynamics of the pulse-molecule interaction are (strongly) phase dependent, independent of pulse duration, whereas the corresponding steady-state populations of the molecular states may or may not be phase-dependent depending on the pulse duration. Analytical rotating wave approximations for pulsed laser-molecule interactions are useful for interpreting the dynamics and the steady-state results as a function of field strength and pulse duration, including the effects of permanent dipole moments. The results reported in this paper are based on molecular parameters associated with an S0→S1 electronic transition in a dipolar molecule. However, they are presented in reduced form and therefore can be scaled to other regions of the electromagnetic spectrum. Short, intense pulses at or beyond the limits of current laser technology will often be required for the types of absolute laser phase effects of this paper to be appreciable for electronic excitations. The discussion, in the UV-VIS, also suffers from the use of a two-level model and from the requirement of field intensities that can be beyond the Keldysh limit. For other spectral regions, these absolute laser phase effects will be much more readily applicable.

The Journal of Chemical Physics•Dec 1, 1998•37 citations
In this paper, we study the influence of time-dependent phase delay on the emission of few photons from a single molecule in a solid matrix. The results demonstrate that a time-dependent phase of the pulses can be used to control the photon emission and strongly affects the spectrum of single molecules. The spectrum of the photon emission probabilities reflects the fast dynamics of the states of the system when the duration of the driven laser pulses is short. Also, it is shown that the coupling between the system and the rf field strongly affects the spectrum of the photon emission probabilities in space.
We consider the photon spontaneous emission of single molecules in a solid matrix with spectral diffusion. A general theoretical strategy for calculating the photon emission statistics in a solid matrix of single molecules is derived. In particular, the control photon emission from single molecules in a solid matrix driven simultaneously by a laser and an electric radiofrequency (rf) field is investigated. The photon emission of single molecules can be modulated by an rf field. The formulation also allows for the study of the average waiting time for the emission event of a single molecule.
The photon emission from a single molecule driven simultaneously by a laser and a slow electric radio frequency (rf) field is studied. We use a non-Hermitian Hamiltonian approach which accounts for the radiative decay of a two-level system modeling the single-molecule source. We apply the renormalization group method for differential equations to obtain long time solution of the corresponding Schrodinger equation, which allows us to calculate the average waiting time for the first photon emission. Then, we analyze the conditions for suppression and enhancement of photon emission in this dissipative two-level system. In particular we derive a transcendental equation, which yields the nontrivial rf field control parameters, for which enhancement and suppression of photon emission occurs. For finite values of radiative decay rate an abrupt transition to the state when both situations are indistinguishable is found for certain values of the rf field parameters. Our results are shown to be in agreement with the available experiments [Ch. Brunel et al., Phys. Rev. Lett. 81, 2679 (1998)].
The ability to control the temporal shape of single-photon pulses is highly desirable in quantum information processing. For instance, it has been shown that Gaussian pulses are best suited for linear optics quantum computing1. By mimicking the time-reversal of a spontaneous emission event, it also allows to optimize the absorption of the prepared photons by a quantum emitter. In this work we investigate the potential of using fast modifications of the detuning between an atomic system and a cavity mode during photon emission to reach this goal. We compare two approaches consisting of varying the emitter or cavity frequency. The latter, achievable by a fast modification of the refractive index of a solid state cavity, will be shown to have negligible influence on the photon spectrum. It allows to create Gaussian pulses interacting with a fidelity to the target photons of 99%, as well as time-reversed photons absorbed by an atom in a cavity with a probability of 93%.
The photon emission from a single molecule driven simultaneously by a laser and a slow electric radio frequency (rf) field is studied. We use a non-Hermitian Hamiltonian approach which accounts for the radiative decay of a two level system modeling a single molecule source. We apply the renormalization group method for differential equations to obtain long time solution of the corresponding Schrdinger equation, which allows us to calculate the average waiting time for the first photon emission. Then, we analyze the conditions for suppression and enhancement of photon emission in this dissipative two-level system. In particular we derive a transcendental equation, which yields the non-trivial rf field control parameters, for which enhancement and suppression of photon emission occurs. For finite values of radiative decay rate an abrupt transition from the molecule's localization in its ground state to delocalization is found for certain critical values of the rf field parameters. Our results are shown to be in agreement with the available experiments [Ch. Brunel et al, Phys. Rev. Lett. 81, 2679 (1998)].
Coherent control uses tailored femtosecond pulse shapes to influence quantum pathways and drive a light-induced process toward a specific outcome. There has been a long-standing debate whether the absorption properties or the probability for population to remain in an excited state of a molecule can be influenced by the pulse shape, even if only a single photon is absorbed. Most such experiments are performed on many molecules simultaneously, so that ensemble averaging reduces the access to quantum effects. Here, we demonstrate systematic coherent control experiments on the fluorescence intensity of a single molecule in the weak-field limit. We demonstrate that a delay scan of interfering pulses reproduces the excitation spectrum of the molecule upon Fourier transformation, but that the spectral phase of a pulse sequence does not affect the transition probability. We generalize this result to arbitrary pulse shapes by performing the first closed-loop coherent control experiments on a single molecule.
The absolute laser phase dependence of the time-dependent populations of the molecular states, including the steady-state (long time) populations of the states, associated with the interaction of a molecule with a pulsed laser is investigated using illustrative two-level examples. One-photon transitions, including the effects of permanent dipoles, are discussed as a function of the pulse duration, intensity, and (absolute) laser phase, for selected laser frequencies. The effects of laser phase can be large, depending on the values of the pulse duration for a given frequency and intensity. The effects of permanent dipoles, relative to no permanent dipoles, are significant for large laser field strengths ε0. When the laser-molecule coupling parameter b=μ12ε0/E21⩾0.2, where μ12 and E21 are the transition dipole and energy difference between the ground and excited states, respectively, the dynamics of the pulse-molecule interaction are (strongly) phase dependent, independent of pulse duration, whereas the corresponding steady-state populations of the molecular states may or may not be phase-dependent depending on the pulse duration. Analytical rotating wave approximations for pulsed laser-molecule interactions are useful for interpreting the dynamics and the steady-state results as a function of field strength and pulse duration, including the effects of permanent dipole moments. The results reported in this paper are based on molecular parameters associated with an S0→S1 electronic transition in a dipolar molecule. However, they are presented in reduced form and therefore can be scaled to other regions of the electromagnetic spectrum. Short, intense pulses at or beyond the limits of current laser technology will often be required for the types of absolute laser phase effects of this paper to be appreciable for electronic excitations. The discussion, in the UV-VIS, also suffers from the use of a two-level model and from the requirement of field intensities that can be beyond the Keldysh limit. For other spectral regions, these absolute laser phase effects will be much more readily applicable.