Intensity Of Excitation Pulse Research Articles

Signatures of Dynamically Dressed States.

The interaction of a resonant light field with a quantum two-level system is of key interest both for fundamental quantum optics and quantum technological applications employing resonant excitation. While emission under resonant continuous-wave excitation has been well studied, the more complex emission spectrum of dynamically dressed states-a quantum two-level system driven by resonant pulsed excitation-has so far been investigated in detail only theoretically. Here, we present the first experimental observation of the complete resonance fluorescence emission spectrum of a single quantum two-level system, in the form of an excitonic transition in a semiconductor quantum dot, driven by finite Gaussian pulses. We observe multiple emerging sidebands as predicted by theory, with an increase of their number and spectral detuning with excitation pulse intensity and a dependence of their spectral shape and intensity on the pulse length. Detuning-dependent measurements provide additional insights into the emission features. The experimental results are in excellent agreement with theoretical calculations of the emission spectra, corroborating our findings.

Ultrafast vibrational excitation transfer on resonant antenna lattices revealed by two-dimensional infrared spectroscopy.

High-quality lattice resonances in arrays of infrared antennas operating in an open-cavity regime form polariton states by means of strong coupling to molecular vibrations. We studied polaritons formed by carbonyl stretching modes of (poly)methyl methacrylate on resonant antenna arrays using femtosecond 2DIR spectroscopy. At a normal incidence of excitation light, doubly degenerate antenna-lattice resonances (ALRs) form two polariton states: a lower polariton and an upper polariton. At an off-normal incidence geometry of 2DIR experiments, the ALR degeneracy is lifted and, consequently, the polariton energies are split. We spectrally resolved and tracked the time-dependent evolution of a cross-peak signal associated with the excitation of reservoir states and the unidirectional transfer of the excess energy to lower polaritons. Bi-exponential decay of the cross-peak suggests that a reversible energy exchange between the bright and dark lower polaritons occurs with a characteristic transfer time of ∼200fs. The cross-peak signal further decays within ∼800fs, which is consistent with the relaxation time of the carbonyl stretching vibration and with the dephasing time of the ALR. An increase in the excitation pulse intensity leads to saturation of the cross-peak amplitude and a modification of the relaxation dynamics. Using quantum-mechanical modeling, we found that the kinetic scheme that captures all the experimental observations implies that only the bright lower polariton accepts the energy from the reservoir, suggesting that transfer occurs via a mechanism involving dipole-dipole interaction. An efficient reservoir-to-polariton transfer can play an important role in developing novel room-temperature quantum optical devices in the mid-infrared wavelength region.

Intersubband Relaxation in CdSe Colloidal Quantum Wells.

The dynamics of intersubband relaxation are critical to quantum well technologies such as quantum cascade lasers and quantum well infrared photodetectors. Here, intersubband relaxation in CdSe colloidal quantum wells, or nanoplatelets, is studied via pump-push-probe transient spectroscopy. An initial interband pump pulse is followed by a secondary infrared push excitation, resonant with intersubband absorption, which promotes electrons from the first conduction band of the quantum well to the second conduction band. A probe pulse monitors subsequent electron cooling to the band edge of the quantum well. Using this technique, intersubband relaxation is studied as a function of critical variables such as colloidal quantum well size and thickness, surface ligand chemistry, temperature, and excitation pulse intensity. Larger quantum well sizes, judicious selection of surface ligand chemistry (e.g., thiolates), low temperatures, and elevated push pulse fluences slow intersubband relaxation. However, compared to resonant intraband relaxation in colloidal quantum dots (up to hundreds of picoseconds), intersubband relaxation in colloidal quantum wells is rapid (<1 ps) under all examined conditions. These experiments indicate that rapid relaxation is driven by both LO phonon and surface scattering. The short time scale of relaxation observed in these materials may hinder intersubband technologies such as mid-infrared detectors, although such rapid relaxation may prove valuable in optical switching.

Excitation-Dependent Emission Color Tuning from an Individual Mn-Doped Perovskite Microcrystal.

Divalent manganese cation (Mn2+) doped perovskite materials are of great interest for their unique optical, magnetic, and electric properties. Herein, we report an excitation-dependent emission color tuning from an individual Mn-doped CsPbCl3 microcrystal (MC) with a wide color tuning range, reversible and continuous color change, and high photostability. We demonstrate that the Mn-doped CsPbCl3 MCs exhibit dual-color emission from both host excitons (blue) and Mn-dopants (orange) through an internal energy transfer (IET) process. By simple change of the laser excitation repetition rate or pulse intensity, the relative emission intensity between exciton (Iexciton) and Mn-dopant (IMn) can be continuously and reversibly tuned from IMn/Itotal (Itotal = IMn + Iexciton) = 0.9-0.8 to 0.1-0.2, corresponding to a color change from orange to blue. Such emission color tuning is enabled by the saturation of Mn-dopant emission at high excitation intensity and a linear dependence of exciton emission with excitation intensity. Transient spectroscopy and temperature-dependent photoluminescence (PL) measurements confirm that the exciton-to-dopant IET in Mn-doped CsPbCl3 MCs is mediated by some shallow trap states, rather than through a direct transfer pathway. Therefore, the saturation of Mn-dopant emission is caused by a bottlenecked energy transfer effect by saturating the mediating trap states at high excitation intensities. The Mn-doped MCs also exhibit a high photostability on the reversible switch of emission color between orange and blue for more than 300 cycles within a continuous operation time of 14 h. In view of the stable and color-switchable emission properties, Mn-doped perovskite MCs may find application in nanophotonic devices using a single MC.

Photon Echo from Localized Excitons in Semiconductor Nanostructures

An overview on photon echo spectroscopy under resonant excitation of the exciton complexes in semiconductor nanostructures is presented. The use of four-wave-mixing technique with the pulsed excitation and heterodyne detection allowed us to measure the coherent response of the system with the picosecond time resolution. It is shown that, for resonant selective pulsed excitation of the localized exciton complexes, the coherent signal is represented by the photon echoes due to the inhomogeneous broadening of the optical transitions. In case of resonant excitation of the trions or donor-bound excitons, the Zeeman splitting of the resident electron ground state levels under the applied transverse magnetic field results in quantum beats of photon echo amplitude at the Larmor precession frequency. Application of magnetic field makes it possible to transfer coherently the optical excitation into the spin ensemble of the resident electrons and to observe a long-lived photon echo signal. The described technique can be used as a high-resolution spectroscopy of the energy splittings in the ground state of the system. Next, we consider the Rabi oscillations and their damping under excitation with intensive optical pulses for the excitons complexes with a different degree of localization. It is shown that damping of the echo signal with increase of the excitation pulse intensity is strongly manifested for excitons, while on trions and donor-bound excitons this effect is substantially weaker.

Ultrafast Transmission Modulation and Recovery via Vibrational Strong Coupling

Strong coupling between vibrational modes and cavity optical modes leads to the formation of vibration-cavity polaritons, separated by the vacuum Rabi splitting. The splitting depends on the square root of the concentration of absorbers confined in the cavity, which has important implications on the response of the coupled system after ultrafast infrared excitation. In this work, we report on solutions of W(CO)6 in hexane with a concentration chosen to access a regime that borders on weak coupling. Under these conditions, large fractions of the W(CO)6 oscillators can be excited, and the anharmonicity of the molecules leads to a commensurate reduction in the Rabi splitting. We report excitation fractions > 0.4, depending on excitation pulse intensity, and show drastic increases in transmission that can be modulated on the picosecond time scale. In comparison to previous experiments, the transient spectra that we observe are much simpler because excited-state transitions lie outside of the transmission spectrum of the cavity, thereby contributing only weakly to the spectra. We find that the Rabi splitting recovers with the characteristic vibrational relaxation lifetime and anisotropy decay of uncoupled W(CO)6, implying that polaritons are not directly involved in the relaxation we observe after the first few ps. The results help corroborate the model that we proposed to describe the results at higher concentrations and show that the ground-state bleach of cavity-coupled molecules has a broad, multisigned spectral response.

Фотонное эхо на локализованных экситонах в полупроводниковых наноструктурах

AbstractAn overview on photon echo spectroscopy under resonant excitation of the exciton complexes in semiconductor nanostructures is presented. The use of four-wave-mixing technique with the pulsed excitation and heterodyne detection allowed us to measure the coherent response of the system with the picosecond time resolution. It is shown that, for resonant selective pulsed excitation of the localized exciton complexes, the coherent signal is represented by the photon echoes due to the inhomogeneous broadening of the optical transitions. In case of resonant excitation of the trions or donor-bound excitons, the Zeeman splitting of the resident electron ground state levels under the applied transverse magnetic field results in quantum beats of photon echo amplitude at the Larmor precession frequency. Application of magnetic field makes it possible to transfer coherently the optical excitation into the spin ensemble of the resident electrons and to observe a long-lived photon echo signal. The described technique can be used as a high-resolution spectroscopy of the energy splittings in the ground state of the system. Next, we consider the Rabi oscillations and their damping under excitation with intensive optical pulses for the excitons complexes with a different degree of localization. It is shown that damping of the echo signal with increase of the excitation pulse intensity is strongly manifested for excitons, while on trions and donor-bound excitons this effect is substantially weaker.

Two-photon absorption of high-power picosecond pulses in PbWO4, ZnWO4, PbMoO4, and CaMoO4 crystals

The nonlinear process of two-photon interband absorption is studied in tungstate and molybdate oxide crystals excited by a sequence of high-power picosecond pulses with a wavelength of 523.5 nm. The transmission of the crystals is measured for the excitation pulse intensity up to 100 GW/cm2. The pulse intensity in the crystals initially transparent at a wavelength of 523.5 nm is strongly limited due to two-photon absorption (TPA), and the reciprocal transmission in PbWO4 and ZnWO4 crystals reaches 50–60. In all crystals, TPA induces long-lived one-photon absorption, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the laser excitation intensity. Absorption dichroism manifests itself in a significant difference in the transmission intensities when the principal orthogonal optical axes of the crystals are excited. The TPA coefficients are determined during the excitation of two optical axes of the crystals. TPA coefficients β for the crystals vary over a wide range, namely, from β = 2.4 cm/GW for PbMoO4 to β = 0.14 cm/GW for CaMoO4, and the values of β can differ almost threefold when different optical axes of a crystal are excited. Good agreement is achieved between the measured intensities limited by TPA and the estimates calculated from the measured nonlinear coefficients. Stimulated Raman scattering (SRS) upon excitation at a wavelength of 523.5 nm is only detected in two of the four crystals under study. The experimental results make it possible to explain the suppression of SRS by its competition with TPA, and the measured nonlinear coefficients are used to estimate this suppression.

Photoluminescence developed from polystyrene and CdS/polystyrene nanocomposite films in picosecond time range by repetitional irradiation of excitation femtosecond pulses in PL up conversion measurements

A CdS/SPS nanocomposite film in which CdS nanoparticles were embedded into partially sulfonated polystyrene (SPS) was synthesized and its subpicosecond time resolved photoluminescence (photoluminescence up conversion: PL Up-C) measurements were carried out. A similar measurement was also done for pure SPS and polystyrene (PS) films that were used as the matrix. For a CdS/SPS, PL Up-C signals (sum frequency signal; SFS) were observed at the first measurement. They were also observed for pure SPS and PS films by repetitional measurements though they were not observed at the first measurement. It seems that the development of SFS for SPS and PS films is due to relatively stable luminescent substances formed from themselves by exposing them to intense femtosecond laser pulse (for excitation) during the measurements. The SFS development process was also readily observed for a CdS/SPS film by reducing excitation pulse intensity in the measurements. Therefore, PL that was observed for a CdS/SPS film is also mainly due to luminescent substances formed from the SPS matrix but CdS nanoparticles. CdS nanoparticles embedded into a SPS film may act as an accelerator for PL development from the SPS matrix. The origin of PL may be several luminescent substances formed by photo- or thermal-degradation of SPS via multiphoton (probably two photons) absorption of SPS itself and/or photo-excitation of CdS nanoparticles. Although the luminescent substances could not be assigned, they might be oxidative decomposition products of SPS that have long conjugated π bonds with a PS main polymer chain that absorbs the excitation femtosecond pulse ( λ max = 396 nm).

Detailed Investigation of the Femtosecond Pump−Probe Spectroscopy of the Hydrated Electron

We recently reported the first pump−probe measurements on the hydrated electron with sufficient time resolution (∼35 fs) to directly observe the initial processes in the solvation dynamics of this key prototype for condensed-phase dynamics [Silva, C.; Walhout, P. K.; Yokoyama, K.; Barbara, P. F. Phys. Rev. Lett. 1998, 80, 1086]. An unprecedented relaxation process for the hydrated electron was observed that occurs on the 35−80 fs time scale and exhibits a solvent isotope effect (τ(D2O)/τ(H2O) ∼ 1.4). The new process was assigned to inertial/librational motion of the water surrounding the excess electron. The present paper reports a more extensive study of the ∼35 fs resolved dynamics of the hydrated electron in H2O and D2O at more probe wavelengths and as a function of pump-pulse intensity. The results are in agreement with the preliminary report and support the importance of librational water motion in the relaxation dynamics of the hydrated electron. New high excitation pulse intensity measurements reve...

Phonon oscillations in the spectrum of the reversible bleaching of gallium arsenide under interband absorption of a high-power picosecond light pulse

Under the irradiation of GaAs with a high-power picosecond light pulse of the photon energy h ̵ ω ex > E g in the spectrum of the reversible bleaching of the sample were found local minimums. These distinctions of the spectrum have been studied and interpreted as a result of a stepwise electron, accompanied by emitting an optical phonon, traveling in the conduction band towards its bottom, from where electrons escape in the process of the recombination superluminescence.

Temporal representation in the control of movement

Theories of the representation of specific kinetic and spatiotem-poral features of movement range from the explicit assertion that temporal aspects of movement are not represented (Kugler et al. 1980) to the idea that they are represented and that they have neurophysiological correlates (Ivry &amp; Corcos 1993; Ivry &amp; Keele 1989). Jeannerod's thesis is that mental and visual images have common mechanisms and that there is a link between the image to move and the mechanisms involved with movement. The target article takes the position that certain parameters are coded in motor representations (sect. 4) but that the duration of an action is not one of them. This position is based on the work of Gottlieb et al. (1989b) and of Decety et al. (1989). Both these studies are worth considering in detail. In Note 1, Jeannerod suggests that: “in time-constrained tasks subjects control the amplitude parameter of force impulses, whereas in spatially constrained tasks the duration of the force impulse is affected by accuracy demands.” This is not exactly correct. Excitation pulse intensity (amplitude) is modulated both in tasks that require spatial and those that require temporal accuracy. Excitation pulse duration is modulated for changes in movement distance and inertial load. If subjects are required to be very accurate spatially, they will move at less than maximum speed for a given distance and this is achieved by lower levels of excitation intensity (Gottlieb et al. 1990).

Organizing principles for single joint movements. III. Speed-insensitive strategy as a default

1. Human subjects made discrete elbow flexions in a horizontal plane over different distances, from a stationary initial position to a visually defined stationary target 9 degrees wide. We measured joint angle, acceleration, and electromyograms (EMGs) from two agonist and two antagonist muscles. 2. Subjects made movements over four different distances following one of four different instructions. The first instructed the subject simply to choose a comfortable speed. The other three explicitly emphasized either speed, accuracy, or maintenance of the "same" speed over different distances. These instructions produced a wide range of movement velocities. 3. The initial rises of the acceleration (and therefore of the inertial torque), as well as the initial slope of the agonist EMG, were all invariant over changes in the target distance for any single instruction but were all sensitive to the given instruction. 4. Our results demonstrate that the speed-insensitive strategy is a standard or default pattern for performing movements that may be carried out for different instructions over a wide range of speeds. A uniform intensity of excitation pulse is not a byproduct of moving at maximal speed. Submaximal intensities are associated with submaximal speeds and are a selected feature of the pattern of movement control.

The cooperativity phenomena in a pigment-protein complex of light-harvesting antenna revealed by picosecond absorbance difference spectroscopy

A model of the cooperative changes in optical properties of light-harvesting bacteriochlorophyll molecules of complex B890 in response to the absorption of light quanta is proposed. According to the model, each antenna chromophore may persist in either of two optically non-excited states, R and T. The occurrence of at least one excitation per complex causes all optically non-excited chromophores of the complex to be converted from state R to state T. The theory is shown to be in good agreement with experimental ‘light curves’ ( ΔAvs intensity of picosecond excitation pulse) for the ‘minor’ and ‘major’ signals of light-harvesting bacteriochlorophylls of complex B890 from Chromatium minutissimum.

Annihilation of singlet excitons in J aggregates of pseudoisocyanine (PIC) studied by pico- and subpicosecond spectroscopy

The excited-state dynamics of J aggregates of PIC have been studied by means of picosecond and subpicosecond absorption spectroscopy as well as integrated fluorescence yield measurements. The results of these measurements show that both the lifetime and the fluorescence yield are strongly dependent on excitation pulse intensity. At relatively high light intensity (1014 photons cm−2 pulse−1) the S1 lifetime is essentially pulse limited (&amp;lt;1 ps) and the fluorescence yield is very low. Upon decreasing the light intensity a gradual increase of the excited-state lifetime and fluorescence yield is observed. At very low excitation intensity (1010 photons cm−2 pulse−1) a single exponential lifetime of 400 ps is observed. At intermediate intensities the excited-state decay is strongly nonexponential. The observed intensity dependence of the excited-state dynamics is attributed to efficient exciton–exciton annihilation between the highly mobile singlet excitons. By applying an expression for bimolecular exciton annihilation, derived and used for photosynthetic antenna systems [Paillotin et al., Biophys. J. 25, 513 (1979)], and treating the energy migration as a hopping motion, information about aggregate size and exciton hopping rate was obtained.

Low-Intensity picosecond fluorescence kinetics and excitation dynamics in barley chloroplasts

The fluorescence decays of barley chloroplasts have been measured by single-photon counting with tunable picosecond dye laser excitation. The fluorescence decays of dark-adapted chloroplasts are best fitted to a sum of three exponential lifetime components with 1 e lifetimes of 112, 380 and 2214 ps. The relative magnitude of each component is shown to be dependent on the excitation wavelength and collected emission wavelength. The excitation wavelength dependence is correlated with the Photosystem (PS) I and PS II action study of Ried [36] and with the measured pigment distributions in the photosynthetic unit [37,41]. Experiments varying the single excitation pulse intensity from 10 8 to 10 12 photons/cm 2 pulse show that our results are not distorted by singlet-singlet annihilation. Unflowed samples where the cloroplasts are under constant illumination show 2-fold increases in quantum yield of fluorescence primarily in the two longer 1 e lifetime components. Theoretical calculations of Shipman [31] on an isolated reaction center with a homogeneous antenna are discussed and the principles extended to discussion of the measured barley chloroplast fluorescence decay components in terms of photosynthetic unit light-harvesting array models and earlier experimental work. Our data support a photosynthetic unit model in which 70–90% of the photons absorbed are quenched by either PS I or efficiently quenching PS II in a process where the fluorescence lifetime is 100 ps. The origin of the intermediate 380 ps. component is probably due to excitation transfer to a PS II reaction center in a redox state which quenches less efficiently.

Kinetics of distant-pair recombination

Abstract The kinetics of the recombination of separately trapped electrons and holes are treated theoretically, and the results are compared with the low-temperature 1·4 eV luminescence of a-Si: H. The carriers are assumed to be distributed at random spatially, and the recombination transition rate is assumed to depend exponentially on the electron-hole separation. We obtain an exact solution, in the form of a non-linear integral equation, for the case of luminescence decay following a single excitation pulse; and we give approximate solutions for repetitively pulsed excitation (as in time-resolved spectroscopy) and for continuous excitation. Good agreement is found between the experimentally observed behaviour of a-Si: H and the predictions of the distant-pair model, without any adjustable parameters. In particular, the model predicts that the decay curve will be independent of the excitation pulse intensity when the pulse creates fewer than ∼ 1018 cm−3 carriers. We show, therefore, that frequency-respon...

Radiationless intermolecular energy transfer with participation of acceptor excited triplet states

Radiationless energy transfer between like and unlike molecules has been experimentally studied under conditions where acceptor molecules have been excited to the triplet state Homogeneous singlet-triplet-triplet migration has been discovered in highlyconcentrated chlorophyll “a” and pheophytin “a” solutions in castor oil at 183 K by measuring the variation of pigment relative quantum yields of fluorescence and triplet state formation as a function of exciting pulse intensity. Heterogeneous single-triplet-triplet energy transfer has been observed in solid solutions of different complex organic molecules (perylene + phenanthrene, Na-fluorescein+chlorophyll “a”, pyrene+Mg-phthalocyanine) as the fluorescent donor state quenching in the presence of acceptor triplet-excited molecules. Primary emphasis is placed on a direct observation of the effect of energy transfer on the excited-state lifetime of the donor. The benzophenone phosphorescence quenching (shortening of phosphorescence lifetime) in the presence of Mg-mesoporphyrin triplet molecules has been found to be caused by the heterogeneous triplet-triplet-triplet energy transfer. Good agreement of the theoretical and experimental results permits us to conclude that all types of observed transfer processes are described by the Förster-Galanin theory for dipole-dipole radiationless energy transfer with no additional assumptions.