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

Single-molecule photon emission statistics for systems with explicit time dependence: Generating function approach

Yonggang Peng, Shijie Xie, Yujun Zheng, Frank L. H. Brown

Published Dec 3, 2009• 20 citations
Publisher

Abstract

Generating function calculations are extended to allow for laser pulse envelopes of arbitrary shape in numerical applications. We investigate photon emission statistics for two-level and V- and Lambda-type three-level systems under time-dependent excitation. Applications relevant to electromagnetically induced transparency and photon emission from single quantum dots are presented.

DOI
10.1063/1.3265855

Related papers

Single molecule photon emission statistics of driven three-level systems

Yonggang Peng, Yujun Zheng, Frank L. H. Brown

We study the statistics of photon emission from three-level single molecule systems. The generating function method [Y. Zheng and F. L. H. Brown, Phys. Rev. Lett. 90, 238305 (2003)] is used to calculate steady state absorption line shapes and Mandel's Q parameter as a function of excitation frequency, as well as the time dependence associated with approach to the steady state. The line shape calculations confirm known results derived via other methods, while the Q parameter results display complex frequency dependences not amenable to simple interpretation. This study confirms the applicability of the generating function formalism to multilevel quantum systems, including the proper modeling of quantum coherence effects.

The Journal of Chemical Physics•Mar 13, 2007•39 citations

Photon statistics of V-type three-level system in single quantum dots

Yonggang Peng, Yujun Zheng

Based on the generating function approach developed recently, the theoretical study of the photon emission statistics in single InGaAs∕GaAs quantum dots is presented. We show the X- and Y-polarized photon emission statistics, the joint probabilities and marginal probabilities of V-type three-level system in single quantum dots driven by single pulse and a pair of pulses, respectively. The first moment confirm known experimental results while the Mandel’s Q parameters results display complex behaviors.

Applied Physics Letters•Mar 3, 2008•20 citations

Theory for Wavelength-Resolved Photon Emission Statistics in Single-Molecule Fluorescence Spectroscopy

Golan Bel, Frank L. H. Brown

We derive the moment generating function for photon emissions from a single molecule driven by laser excitation. The frequencies of the fluoresced photons are explicitly considered. Calculations are performed for the case of a two-level dye molecule, showing that measured photon statistics will display a strong and nonintuitive dependence on detector bandwidth. Moreover, it is demonstrated that the antibunching phenomenon, associated with negative values of Mandel's Q parameter, results from correlations between photons with well separated frequencies.

arXiv:0908.1924•Physical Review Letters•Jan 9, 2009•47 citations

The effect of environment on fluorescence photon statistics of single molecule system

Han Bai

The fluorescence photon emission of single molecule two-level system (TLS) simultaneously driven by the laser and electric radio frequency (RF) fields is investigated, using the generating function method developed recently. The fluorescence photon statistical properties of single molecule TLS are studied theoretically, under the single laser pulse field and the single RF pulse. Further, we can control the photon emission of two-level system.

Zhongguo kexue. Wulixue Lixue Tianwenxue•Jan 1, 2011•0 citations

Photon statistics of time dependent electronic excitation of spin injected quantum dots

Chiran Wijesundara, Jeffrey Carvalho, Yuan Lü +1 more

The time dynamics of spin-injected, electrically contacted quantum dots were investigated with a focus on the time evolution of photon statistics. Photon statistics can provide insights into whether the device functions as an effective single-photon emitter or exhibits higher-order emissions. Through these investigations, we found that the shape of the electrical excitation pulse has a direct impact on photon statistics. Specifically, the rising edge of the pulse corresponds to a significantly higher number of higher-order photon states, which decay much faster than single photons associated with the falling edge of the electrical pulse. This relationship implies that the pulse shape can be tailored to optimize the device as either a better single-photon source or a generator of higher-order photon states, with potential applications in creating deterministic higher-order photon Fock states. The ability to easily modify the pulse shape is a unique feature of electrically excited quantum dots.

arXiv:2501.16747•Jan 28, 2025•0 citations

Quantum Emitters

Lukáš Novotný, Bert Hecht

The chapter discusses quantum emitters, exploring their fundamental mechanisms, properties, and applications. Beginning with two-level systems, we introduce the concept of extinction cross-section. To capture phenomena, such as fluorescence, the discussion extends to four-level systems and spontaneous as well as stimulated emission processes, crucial for understanding laser operation. We then examine the dependence of the quantum yield on the local environment. Single-photon emission is scrutinized in terms of the second-order autocorrelation function through both steady-state and time-dependent analyses, providing a comprehensive understanding of this essential feature of quantum emitters. The chapter further addresses the generation of indistinguishable single photons, a key requirement for quantum computing and secure communication. Various types of quantum emitters are then introduced, including fluorescent molecules, semiconductor quantum dots, and color centers in diamond, each with unique properties and applications. Finally, single molecules are presented as probes for localized fields, with an in-depth look at field distributions in a laser focus and sources of strongly localized fields.

Cambridge University Press eBooks•Oct 31, 2025•0 citations
Generating function calculations are extended to allow for laser pulse envelopes of arbitrary shape in numerical applications. We investigate photon emission statistics for two-level and V- and Lambda-type three-level systems under time-dependent excitation. Applications relevant to electromagnetically induced transparency and photon emission from single quantum dots are presented.
We study the statistics of photon emission from three-level single molecule systems. The generating function method [Y. Zheng and F. L. H. Brown, Phys. Rev. Lett. 90, 238305 (2003)] is used to calculate steady state absorption line shapes and Mandel's Q parameter as a function of excitation frequency, as well as the time dependence associated with approach to the steady state. The line shape calculations confirm known results derived via other methods, while the Q parameter results display complex frequency dependences not amenable to simple interpretation. This study confirms the applicability of the generating function formalism to multilevel quantum systems, including the proper modeling of quantum coherence effects.
Based on the generating function approach developed recently, the theoretical study of the photon emission statistics in single InGaAs∕GaAs quantum dots is presented. We show the X- and Y-polarized photon emission statistics, the joint probabilities and marginal probabilities of V-type three-level system in single quantum dots driven by single pulse and a pair of pulses, respectively. The first moment confirm known experimental results while the Mandel’s Q parameters results display complex behaviors.
We derive the moment generating function for photon emissions from a single molecule driven by laser excitation. The frequencies of the fluoresced photons are explicitly considered. Calculations are performed for the case of a two-level dye molecule, showing that measured photon statistics will display a strong and nonintuitive dependence on detector bandwidth. Moreover, it is demonstrated that the antibunching phenomenon, associated with negative values of Mandel's Q parameter, results from correlations between photons with well separated frequencies.
The time dynamics of spin-injected, electrically contacted quantum dots were investigated with a focus on the time evolution of photon statistics. Photon statistics can provide insights into whether the device functions as an effective single-photon emitter or exhibits higher-order emissions. Through these investigations, we found that the shape of the electrical excitation pulse has a direct impact on photon statistics. Specifically, the rising edge of the pulse corresponds to a significantly higher number of higher-order photon states, which decay much faster than single photons associated with the falling edge of the electrical pulse. This relationship implies that the pulse shape can be tailored to optimize the device as either a better single-photon source or a generator of higher-order photon states, with potential applications in creating deterministic higher-order photon Fock states. The ability to easily modify the pulse shape is a unique feature of electrically excited quantum dots.
The chapter discusses quantum emitters, exploring their fundamental mechanisms, properties, and applications. Beginning with two-level systems, we introduce the concept of extinction cross-section. To capture phenomena, such as fluorescence, the discussion extends to four-level systems and spontaneous as well as stimulated emission processes, crucial for understanding laser operation. We then examine the dependence of the quantum yield on the local environment. Single-photon emission is scrutinized in terms of the second-order autocorrelation function through both steady-state and time-dependent analyses, providing a comprehensive understanding of this essential feature of quantum emitters. The chapter further addresses the generation of indistinguishable single photons, a key requirement for quantum computing and secure communication. Various types of quantum emitters are then introduced, including fluorescent molecules, semiconductor quantum dots, and color centers in diamond, each with unique properties and applications. Finally, single molecules are presented as probes for localized fields, with an in-depth look at field distributions in a laser focus and sources of strongly localized fields.