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

Measurement of optical dephasing by double phase switching

Azriel Z. Genack, K. Leung, Axel Schenzle

Published Jul 1, 1983• 5 citations
Publisher

Abstract

We show that the optical dephasing time ${T}_{2}$ can be obtained from a measurement of the time delay ${T}_{0}$ between two shifts of $\ifmmode\pm\else\textpm\fi{}\frac{\ensuremath{\pi}}{2}$ in the phase of the exciting laser for which a null occurs in the jump in the nonlinear transmission through a sample. The phase shift is imposed upon a single-mode cw laser by applying a rectangular voltage pulse to an electro-optic phase modulator placed in the laser beam. The time delay at which the null occurs is proportional to ${T}_{2}$, which is given by the expression ${T}_{2}=(\frac{2}{\mathrm{ln}2}){T}_{0}$. The method is demonstrated in atomic sodium and iodine vapor and the separation of third-order optical transients from linear transients induced by the phase shift is discussed. An analytic expression for the jump in the nonlinear transmission, induced by the second phase shift, as well as for the transient in transmission following a single phase shift of a laser which weakly saturates an optically thin sample is derived. It is also shown that optical dephasing rates may be inferred from the variation of the integral of the transmitted light in a double-phase-switching experiment.

DOI
10.1103/physreva.28.308

Related papers

Coherent Transients by Optical Phase Switching: Dephasing in La Cl3 : Pr3+

Azriel Z. Genack, David A. Weitz, R. M. Macfarlane +2 more

A novel coherent transient effect is observed following a rapid shift in the relative phase of an exciting laser and sample polarization. An analytical expression is derived for the signal which is a sum of exponentially decaying terms with characteristic times involving both ${T}_{1}$ and ${T}_{2}$. Phase switching is a powerful approach to the study of optical relaxation and is applied here to measure dephasing in La${\mathrm{Cl}}_{3}$: ${\mathrm{Pr}}^{3+}$.

Physical Review Letters•Aug 11, 1980•31 citations

Optical coherent transients by laser frequency switching

Azriel Z. Genack, Richard G. Brewer

A simple method for observing coherent optical-transient phenomena is described. Effects such as photon echoes and free induction decay (FID) should allow studies of the dynamic properties of atoms, molecules, and solids on a time scale ranging from milliseconds to \ensuremath{\sim} 50 ps. The frequency of a cw dye laser is switched with an intracavity electro-optic modulator, producing in an external sample coherent transients which are detected in the forward beam. Measurements of long dephasing times are possible, as in FID, because the laser can oscillate indefinitely at the new frequency following a step-function switching pulse. Measurements of short decay times are also practical because the switching time is not restricted by the laser gain or cavity ringing time. In addition, the dye's dephasing time of a few picoseconds or less is too rapid to interfere with these observations. Since the pulse sequence can be preselected, the entire class of coherent optical transients is accessible. The method thus incorporates all of the advantages inherent in Stark switching, including heterodyne detection and high sensitivity, without being restricted to Stark-tunable systems. Laser frequency switching is discussed also in terms of a theoretical model which exposes the time-dependent properties of a phase-modulated cavity mode. Dephasing studies have been carried out thus far in atomic and molecular gases and low-temperature solids containing inorganic impurity ions or large organic molecules. The utility of the FID effect is emphasized where precise dephasing times are obtained from time-frequency Fourier transformation of FID signals using a digital computer. The first quantitative and detailed test of FID theory is provided by these experimental techniques.

Physical Review A•Apr 1, 1978•65 citations

Electro-Optic Generation Of Coherent Optical Transients

D. Anafi, Azriel Z. Genack

Optical Transient Experiments allow one to probe the coherent interaction of light with matter, as well as measure the time for energy transfer, T1, and loss of phase coherence, T2, in atoms, molecules and solids. Coherent optical transients are induced when the interaction of light with the sample is changed in a time which is short compared to T2. The interaction can be modified by changing the amplitude, frequency or phase of the existing laser light. This can be accomplished with an electro-optic modulator which makes it possible to electronically control a wide variety of laser experiments. The method of electro-optic laser phase and frequency switching with an extra-cavity modulator is discussed below.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jan 30, 1980•0 citations

Coherent Transients by Laser-Acoustical Diffraction Spectroscopy

A. H. Zewail

Recently we have reported[1] on the measurements of electronic dephasing (T_2) and radiationless decay (T_1) in molecules using emission spectroscopy as a probe for the detection of the photon echo. This right-angle photon echo utilizes a single mode of a narrow-band (~MHz) cw dye laser and an intracavity electro-optical (EO) element that modulates the frequency of the laser.[2] Applying voltage pulses into the EO crystal switches the laser frequency from ω_0 (the peak frequency of the transition resonance) into another frequency ω. This switching procedure introduced by Brewer et al. for the observation of transients in the forward direction of the laser allows one to observe coherent transients in gases,[1,2] solids[3-5] and molecular beams.[6] Typically, the dispersion of the nonlinear EO crystal (e.g., AD*P) gives a 60 MHz frequency shift within the inhomogeneous resonance of the optical transition (width ~GHz or larger). Therefore, to switch the laser frequency further, one must use high-voltage signals that are usually hard to obtain especially for multiple-pulse experiments. Secondly, there is a limit on the frequency shift which is conditioned by the mode spacing of the cavity. Thirdly, because the laser is switched into a new group of molecules some complications may arise in interpreting the transient spectra especially in large molecules. This is because in large molecules the density of excited states is high and thus the buildup of transients of w molecules (which could be complex) will be superimposed on the decay of ω_0 molecules. Finally, off-resonance effects (e.g., beats) between the molecules at frequency ω and ω_0 cannot be avoided.

Journal of the Optical Society of America A•May 1, 1978•1 citation

Two-photon optical transients by intensity switching

Maryna D'Souza, Arvind Kumar

A new method of observing two-photon optical transients is proposed, namely, by intensity switching of incident cw laser beams. This method, which is an alternative to the standard dc Stark or frequency-switching techniques, employs the second-order optical (ac) Stark effect to throw the two-photon active levels in or out of resonance by appropriately switching the intensities of the two laser beams. Theoretical treatment for the three basic transients optical nutation, free induction decay, and two-pulse echo in thin samples using intensity switching, is given for both the cases: co- and counter-propagating beams. The feasibility of the method for the $5{S}_{\frac{1}{2}}\ensuremath{-}3{S}_{\frac{1}{2}}$ transition in Na vapor is demonstrated. An important feature is the apearance of an intensity-dependent beat frequency in the optical FID signal.

Physical Review A•Sep 1, 1980•4 citations

Phase modulation technique for eliminating phase noise in picosecond T2 measurements based on stimulated Raman gain

Martine M. De Maziere, D. Schoemaker

The pump and probe variant of the stimulated Raman gain technique permits the measurement of picosecond dephasing times with low-power, continuous-wave mode-locked lasers, but it suffers by its susceptibility to inevitable randomly induced fluctuations in the relative phases of the interacting laser fields. The resulting severe requirements on optical stability can be circumvented through application of a double-modulation–detection scheme that we have developed. It is based on rms detection of the T2 signal as generated through application of a low-frequency phase modulation of precise amplitude, additional to the commonly applied rf modulation with corresponding lock-in detection. A detailed description of the method and its experimental realization is presented. T2 measurements on the 656 cm−1 vibration of liquid CS2 illustrate its performance. In comparison with previous techniques, precision is improved by about a factor of 4. But more important is the fact that the technique permits to make a continuous recording of the T2 signal, while achieving at the same time a reduction in measurement time by an order of magnitude. Furthermore, optimization of the optical setup is possible, through direct monitoring of the dephasing signal at any delay. Automating the data taking and processing should be straightforward.

Journal of Applied Physics•Aug 15, 1985•12 citations
We show that the optical dephasing time T2{T}_{2}T2​ can be obtained from a measurement of the time delay T0{T}_{0}T0​ between two shifts of \ifmmode±\else\textpm\fi\ensuremathπ2\ifmmode\pm\else\textpm\fi{}\frac{\ensuremath{\pi}}{2}\ifmmode±\else\textpm\fi2\ensuremathπ​ in the phase of the exciting laser for which a null occurs in the jump in the nonlinear transmission through a sample. The phase shift is imposed upon a single-mode cw laser by applying a rectangular voltage pulse to an electro-optic phase modulator placed in the laser beam. The time delay at which the null occurs is proportional to T2{T}_{2}T2​, which is given by the expression T2=(2ln2)T0{T}_{2}=(\frac{2}{\mathrm{ln}2}){T}_{0}T2​=(ln22​)T0​. The method is demonstrated in atomic sodium and iodine vapor and the separation of third-order optical transients from linear transients induced by the phase shift is discussed. An analytic expression for the jump in the nonlinear transmission, induced by the second phase shift, as well as for the transient in transmission following a single phase shift of a laser which weakly saturates an optically thin sample is derived. It is also shown that optical dephasing rates may be inferred from the variation of the integral of the transmitted light in a double-phase-switching experiment.
A novel coherent transient effect is observed following a rapid shift in the relative phase of an exciting laser and sample polarization. An analytical expression is derived for the signal which is a sum of exponentially decaying terms with characteristic times involving both T1{T}_{1}T1​ and T2{T}_{2}T2​. Phase switching is a powerful approach to the study of optical relaxation and is applied here to measure dephasing in LaCl3{\mathrm{Cl}}_{3}Cl3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+.
A simple method for observing coherent optical-transient phenomena is described. Effects such as photon echoes and free induction decay (FID) should allow studies of the dynamic properties of atoms, molecules, and solids on a time scale ranging from milliseconds to \ensuremath{\sim} 50 ps. The frequency of a cw dye laser is switched with an intracavity electro-optic modulator, producing in an external sample coherent transients which are detected in the forward beam. Measurements of long dephasing times are possible, as in FID, because the laser can oscillate indefinitely at the new frequency following a step-function switching pulse. Measurements of short decay times are also practical because the switching time is not restricted by the laser gain or cavity ringing time. In addition, the dye's dephasing time of a few picoseconds or less is too rapid to interfere with these observations. Since the pulse sequence can be preselected, the entire class of coherent optical transients is accessible. The method thus incorporates all of the advantages inherent in Stark switching, including heterodyne detection and high sensitivity, without being restricted to Stark-tunable systems. Laser frequency switching is discussed also in terms of a theoretical model which exposes the time-dependent properties of a phase-modulated cavity mode. Dephasing studies have been carried out thus far in atomic and molecular gases and low-temperature solids containing inorganic impurity ions or large organic molecules. The utility of the FID effect is emphasized where precise dephasing times are obtained from time-frequency Fourier transformation of FID signals using a digital computer. The first quantitative and detailed test of FID theory is provided by these experimental techniques.
Optical Transient Experiments allow one to probe the coherent interaction of light with matter, as well as measure the time for energy transfer, T1, and loss of phase coherence, T2, in atoms, molecules and solids. Coherent optical transients are induced when the interaction of light with the sample is changed in a time which is short compared to T2. The interaction can be modified by changing the amplitude, frequency or phase of the existing laser light. This can be accomplished with an electro-optic modulator which makes it possible to electronically control a wide variety of laser experiments. The method of electro-optic laser phase and frequency switching with an extra-cavity modulator is discussed below.
Recently we have reported[1] on the measurements of electronic dephasing (T_2) and radiationless decay (T_1) in molecules using emission spectroscopy as a probe for the detection of the photon echo. This right-angle photon echo utilizes a single mode of a narrow-band (~MHz) cw dye laser and an intracavity electro-optical (EO) element that modulates the frequency of the laser.[2] Applying voltage pulses into the EO crystal switches the laser frequency from ω_0 (the peak frequency of the transition resonance) into another frequency ω. This switching procedure introduced by Brewer et al. for the observation of transients in the forward direction of the laser allows one to observe coherent transients in gases,[1,2] solids[3-5] and molecular beams.[6] Typically, the dispersion of the nonlinear EO crystal (e.g., AD*P) gives a 60 MHz frequency shift within the inhomogeneous resonance of the optical transition (width ~GHz or larger). Therefore, to switch the laser frequency further, one must use high-voltage signals that are usually hard to obtain especially for multiple-pulse experiments. Secondly, there is a limit on the frequency shift which is conditioned by the mode spacing of the cavity. Thirdly, because the laser is switched into a new group of molecules some complications may arise in interpreting the transient spectra especially in large molecules. This is because in large molecules the density of excited states is high and thus the buildup of transients of w molecules (which could be complex) will be superimposed on the decay of ω_0 molecules. Finally, off-resonance effects (e.g., beats) between the molecules at frequency ω and ω_0 cannot be avoided.
A new method of observing two-photon optical transients is proposed, namely, by intensity switching of incident cw laser beams. This method, which is an alternative to the standard dc Stark or frequency-switching techniques, employs the second-order optical (ac) Stark effect to throw the two-photon active levels in or out of resonance by appropriately switching the intensities of the two laser beams. Theoretical treatment for the three basic transients optical nutation, free induction decay, and two-pulse echo in thin samples using intensity switching, is given for both the cases: co- and counter-propagating beams. The feasibility of the method for the $5{S}_{\frac{1}{2}}\ensuremath{-}3{S}_{\frac{1}{2}}$ transition in Na vapor is demonstrated. An important feature is the apearance of an intensity-dependent beat frequency in the optical FID signal.
The pump and probe variant of the stimulated Raman gain technique permits the measurement of picosecond dephasing times with low-power, continuous-wave mode-locked lasers, but it suffers by its susceptibility to inevitable randomly induced fluctuations in the relative phases of the interacting laser fields. The resulting severe requirements on optical stability can be circumvented through application of a double-modulation–detection scheme that we have developed. It is based on rms detection of the T2 signal as generated through application of a low-frequency phase modulation of precise amplitude, additional to the commonly applied rf modulation with corresponding lock-in detection. A detailed description of the method and its experimental realization is presented. T2 measurements on the 656 cm−1 vibration of liquid CS2 illustrate its performance. In comparison with previous techniques, precision is improved by about a factor of 4. But more important is the fact that the technique permits to make a continuous recording of the T2 signal, while achieving at the same time a reduction in measurement time by an order of magnitude. Furthermore, optimization of the optical setup is possible, through direct monitoring of the dephasing signal at any delay. Automating the data taking and processing should be straightforward.