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We consider the theory of the non-linear spectroscopy for a single molecule undergoing stochastic dynamics and interacting with a sequence of two laser pulses. General expressions for photon counting statistics are obtained, and an exact…

Optics · Physics 2008-01-13 F. Shikerman , E. Barkai

A theory is formulated for time dependent fluctuations of the spectrum of a single molecule in a dynamic environment. In particular, we investigate the photon counting statistics of a single molecule undergoing a spectral diffusion process.…

Statistical Mechanics · Physics 2007-05-23 YounJoon Jung , Eli Barkai , Robert J. Silbey

Pump-probe microscopy is an emerging nonlinear imaging technique based on high repetition rate lasers and fast intensity modulation. Here we present new methods for pump-probe microscopy that keep the beam intensity constant and instead…

Optics · Physics 2021-04-07 Jun Jiang , David Grass , Yue Zhou , Warren S. Warren , Martin C. Fischer

Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with…

Optics · Physics 2025-05-14 Sanchayeeta Jana , Simon Durst , Lucas Ludwig , Markus Lippitz

There are many ways of calculating photon statistics in quantum optics in general and single molecule spectroscopy in particular such as the generating function method, the quantum jump approach or time ordering methods. In this paper…

Optics · Physics 2007-10-30 Faina Shikerman , Yong He , Eli Barkai

We investigate the distribution of the number of photons emitted by a single molecule undergoing a spectral diffusion process and interacting with a continuous wave laser field. The spectral diffusion is modeled based on a stochastic…

Statistical Mechanics · Physics 2009-11-10 Yong He , Eli Barkai

Optical solitary waves (solitons) that interact in a nonlinear system can bind and form a structure similar to a molecule. The rich dynamics of this process have created a demand for rapid spectral characterization to deepen the…

Optics · Physics 2023-06-21 Lukasz A. Sterczewski , Jaroslaw Sotor

The pioneering experiments of linear spectroscopy were performed using flames in the 1800s, but nonlinear optical measurements had to wait until lasers became available in the twentieth century. Because the nonlinear cross section of…

Quantum Physics · Physics 2016-07-13 Andreas Maser , Benjamin Gmeiner , Tobias Utikal , Stephan Götzinger , Vahid Sandoghdar

We introduce and experimentally demonstrate a method, where the two intrinsic time scales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photo-electron photo-ion coincidence…

Photon statistics is a powerful tool for characterizing the emission dynamics of nanoscopic systems and their photophysics. Recent advances that combine correlation spectroscopy with scanning tunneling microscopy-induced luminescence (STML)…

Mesoscale and Nanoscale Physics · Physics 2018-12-20 Pablo Merino , Anna Rosławska , Christopher C. Leon , Abhishek Grewal , Christoph Große , Cesar González , Klaus Kuhnke , Klaus Kern

Spectral diffusion is a result of random spectral jumps of a narrow line as a result of a fluctuating environment. It is an important issue in spectroscopy, because the observed spectral broadening prevents access to the intrinsic line…

Ultrafast optical pump-probe spectroscopy is a powerful tool to study dynamics in solid materials on femto- and picosecond timescales. In such experiments, a pump pulse induces dynamics inside a sample by impulsive light-matter interaction,…

We extend the generating function technique for calculation of single molecule photon emission statistics [Y. Zheng and F. L. H. Brown, Phys. Rev. Lett., 90,238305 (2003)] to systems governed by multi-level quantum dynamics. This opens up…

Materials Science · Physics 2009-09-18 Golan Bel , Yujun Zheng , Frank L. H. Brown

We investigate the distribution of number of photons emitted by a single molecule undergoing a spectral diffusion process and interacting with a continuous wave field. Using a generating function formalism an exact analytical formula for…

Statistical Mechanics · Physics 2009-11-10 Yong He , Eli Barkai

Two atoms in an ultracold gas are correlated at short inter-atomic distances due to threshold effects where the potential energy of their interaction dominates the kinetic energy. The correlations manifest themselves in a distinct nodal…

Atomic Physics · Physics 2011-04-15 Christiane P. Koch , Ronnie Kosloff

We calculated third order non-linear polarization to estimate the two-photon absorption of non-interacting two-level molecules in the transmission-type degenerate pump-probe geometry. The spectral intensity and the phase changes of the…

Optics · Physics 2019-05-01 Tsogvoo Khos-Ochir , Kim Myung-Whun , Purevdorj Munkhbaatar

We apply input-output theory with quantum pulses [AH Kiilerich, K M\o lmer, Phys. Rev. Lett. {\bf 123}, 123604 (2019)] to a model of a new type of two-photon detector consisting of one molecule that can detect two photons arriving…

Quantum Physics · Physics 2021-10-20 Saumya Biswas , S. J. van Enk

We theoretically investigate the statistical properties of photon emission of a driven two-level single-molecule system undergoing spectral diffusion induced by nonequilibrium environmental fluctuations. Within the framework of the…

Quantum Physics · Physics 2026-05-06 Xiangji Cai , Yonggang Peng , Yujun Zheng

We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a…

Optics · Physics 2018-12-11 Daria Popova-Gorelova , Jochen Küpper , Robin Santra

Linear and non-linear spectroscopies are powerful tools used to investigate the energetics and dynamics of electronic excited states of both molecules and crystals. While highly accurate \emph{ab initio} calculations of molecular spectra…

Materials Science · Physics 2019-09-26 Alan M. Lewis , Timothy C. Berkelbach
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