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PubMed2006

Optical control of excited-state vibrational coherences of a molecule in solution: The influence of the excitation pulse spectrum and phase in LD690.

Spectral and phase shaping of femtosecond laser pulses is used to selectively excite vibrational wave packets on the ground (S0) and excited (S1) electronic states in the laser dye LD690. The transient absorption signals observed following excitation near the peak of the ground-state absorption spectrum are characterized by a dominant 586 cm(-1) vibrational mode. This vibration is assigned to a wave packet on the S0 potential energy surface. When the excitation pulse is tuned to the blue wing of the absorption spectrum, a lower frequency 568 cm(-1) vibration dominates the response. This lower frequency mode is assigned to a vibrational wave packet on the S1 electronic state. The spectrum and phase of the excitation pulse also influence both the dephasing of the vibrational wave packet and the amplitude profiles of the oscillations as a function of probe wavelength. Excitation by blue-tuned, positively chirped pulses slows the apparent dephasing of the vibrational coherences compared with a transform-limited pulse having the same spectrum. Blue-tuned negatively chirped excitation pulses suppress the observation of coherent oscillations in the ground state.

Journal Article↗
PubMed2004

Intramolecular vibrational energy redistribution in bridged azulene-anthracene compounds: ballistic energy transport through molecular chains.

Intramolecular vibrational energy flow in excited bridged azulene-anthracene compounds is investigated by time-resolved pump-probe laser spectroscopy. The bridges consist of molecular chains and are of the type (CH(2))(m) with m up to 6 as well as (CH(2)OCH(2))(n) (n=1,2) and CH(2)SCH(2). After light absorption into the azulene S(1) band and subsequent fast internal conversion, excited molecules are formed where the vibrational energy is localized at the azulene side. The vibrational energy transfer through the molecular bridge to the anthracene side and, finally, to the surrounding medium is followed by probing the red edge of the azulene S(3) absorption band at 300 nm and/or the anthracene S(1) absorption band at 400 nm. In order to separate the time scales for intramolecular and intermolecular energy transfer, most of the experiments were performed in supercritical xenon where vibrational energy transfer to the bath is comparably slow. The intramolecular equilibration proceeds in two steps. About 15%-20% of the excitation energy leaves the azulene side within a short period of 300 fs. This component accompanies the intramolecular vibrational energy redistribution (IVR) within the azulene chromophore and it is caused by dephasing of normal modes contributing to the initial local excitation of the azulene side and extending over large parts of the molecule. Later, IVR in the whole molecule takes place transferring vibrational energy from the azulene through the bridge to the anthracene side and thereby leading to microcanonical equilibrium. The corresponding time constants tau(IVR) for short bridges increase with the chain length. For longer bridges consisting of more than three elements, however, tau(IVR) is constant at around 4-5 ps. Comparison with molecular dynamics simulations suggests that the coupling of these chains to the two chromophores limits the rate of intramolecular vibrational energy transfer. Inside the bridges the energy transport is essentially ballistic and, therefore, tau(IVR) is independent on the length.

Journal Article↗
PubMed2005

Electronically forbidden (5sigmau-->ksigmau) photoionization of CS2: mode-specific electronic-vibrational coupling.

Vibrationally resolved photoelectron spectroscopy of the CS(2) (+)(B (2)Sigma(u) (+)) state is used to show how nontotally symmetric vibrations "activate" a forbidden electronic transition in the photoionization continuum, specifically, a 5sigma(u)-->ksigma(u) shape resonance, that would be inaccessible in the absence of a symmetry breaking vibration. This electronic channel is forbidden owing to inversion symmetry selection rules, but it can be accessed when a nonsymmetric vibration is excited, such as bending or antisymmetric stretching. Photoelectron spectra are acquired for photon energies 17</=hnu</=72 eV, and it is observed that the forbidden vibrational transitions are selectively enhanced in the region of a symmetry-forbidden continuum shape resonance centered at hnu approximately 42 eV. Schwinger variational calculations are performed to analyze the data, and the theoretical analysis demonstrates that the observed forbidden transitions are due to photoelectron-mediated vibronic coupling, rather than interchannel Herzberg-Teller mixing. We observe and explain the counterintuitive result that some vibrational branching ratios vary strongly with energy in the region of the resonance, even though the resonance position and width are not appreciably influenced by geometry changes that correspond to the affected vibrations. In addition, we find that another resonant channel, 5sigma(u)-->kpi(g), influences the symmetric stretch branching ratio. All of the observed effects can be understood within the framework of the Chase adiabatic approximation, i.e., the Born-Oppenheimer approximation applied to photoionization.

Journal Article↗
PubMed2005

Vibrational energy relaxation of azulene studied by the transient grating method. II. Liquid solvents.

The vibrational energy dissipation process of the ground-state azulene in various liquids has been studied by the transient grating spectroscopy. The acoustic signal produced by the temperature rise of the solvent due to the vibrational energy relaxation of azulene was monitored. The temperature rise-time constant of the solvent has been determined both by the fitting of the acoustic signal to a theoretical model equation and by the analysis of the acoustic peak shift. We found that the temperature rise-time constants determined by the transient grating method in various solvents are larger than the vibrational energy relaxation time constants determined by the transient absorption measurement [D. Schwarzer, J. Troe, M. Votsmeier, and M. Zerezke, J. Chem. Phys. 105, 3121 (1996)]. The difference is explained by different energy dissipation pathways from azulene to solvent; vibrational-vibrational (V-V) energy transfer and vibrational-translational (V-T) energy transfer. The contribution of the V-V energy transfer is estimated in various liquid solvents from the difference between the temperature rise time and vibrational energy relaxation time, and the solvent V-T relaxation time.

Journal Article↗
PubMed2005

Exit-channel dynamics in barrierless unimolecular reactions: criteria of vibrational adiabaticity.

Conversion of translational into vibrational energy during the last step of a unimolecular reaction is brought about by the curvature of the reaction path. The corresponding coupling is analyzed by an angle-action reaction path Hamiltonian (RPH). The accuracy of the vibrational adiabatic approximation is found to be completely independent of the shape of the potential energy Vs. Vibrations are adiabatic when two independent dimensionless parameters are small. The first one, denoted as sigma, controls the dynamic coupling. The physical significance of the condition sigma<<1 is that the amplitude of the vibrations normal to the reaction path should be much smaller than the radius of curvature of the reaction path. The second parameter, denoted as mu, governs the static coupling. It results from the dependence of the vibrational frequency omega on the reaction coordinate s. The higher omega, the lower its derivative with respect to s and, more unexpectedly, the higher the translational energy epsilon, the lower mu is. A criterion for locating a particular dividing surface in barrierless reactions is proposed. This surface separates two regions of space: one where energy flows freely, and one where energy conversion between translation and vibration is hindered by adiabatic invariance. The nature of the dynamical constraint that prevents the product translational energy distribution from being fully statistical can be identified by a maximum entropy analysis. The constraint is found to bear on the translational momentum ps, i.e., on the square root of the translational energy epsilon1/2. This can be understood by applying Jacobi's form of the least action principle to the vibrationally adiabatic RPH.

Journal Article↗
PubMed2006

Generation and characterization of highly vibrationally excited molecular beam.

A simple method to generate and characterize a pure highly vibrationally excited azulene molecular beam is demonstrated. Azulene molecules initially excited to the S4 state by 266-nm UV photons reach high vibrationally excited levels of the ground electronic state upon rapid internal conversion from the S4 electronically excited state. VUV laser beams at 157 and 118 nm, respectively, are used to characterize the relative concentrations of the highly vibrationally excited azulene and the rotationally and vibrationally cooled azulene in the molecular beam. With a laser intensity of 34 mJ/cm2, 75% of azulene molecules absorb a single 266-nm photon and become highly vibrationally excited molecules. The remaining ground-state azulene molecules absorb two or more UV photons, ending up either as molecular cations, which are repelled out of the beam by an electric field, or as dissociation fragments, which veer off the molecular-beam axis. No azulene without absorption of UV photons is left in the molecular beam. The molecular beam that contains only highly vibrationally excited molecules and carrier gas is useful in various experiments related to the studies of highly vibrationally excited molecules.

Journal Article↗
PubMed2006

Vibrational energy relaxation of a diatomic molecule in a room-temperature ionic liquid.

Vibrational energy relaxation (VER) dynamics of a diatomic solute in ionic liquid 1-ethyl-3-methylimidazolium hexafluorophosphate (EMI(+)PF(6) (-)) are studied via equilibrium and nonequilibrium molecular dynamics simulations. The time scale for VER is found to decrease markedly with the increasing solute dipole moment, consonant with many previous studies in polar solvents. A detailed analysis of nonequilibrium results shows that for a dipolar solute, dissipation of an excess solute vibrational energy occurs almost exclusively via the Lennard-Jones interactions between the solute and solvent, while an oscillatory energy exchange between the two is mainly controlled by their electrostatic interactions. Regardless of the anharmonicity of the solute vibrational potential, VER becomes accelerated as the initial vibrational energy increases. This is attributed primarily to the enhancement in variations of the solvent force on the solute bond, induced by large-amplitude solute vibrations. One interesting finding is that if a time variable scaled with the initial excitation energy is employed, dissipation dynamics of the excess vibrational energy of the dipolar solute tend to show a universal behavior irrespective of its initial vibrational state. Comparison with water and acetonitrile shows that overall characteristics of VER in EMI(+)PF(6) (-) are similar to those in acetonitrile, while relaxation in water is much faster than the two. It is also found that the Landau-Teller theory predictions for VER time scale obtained via equilibrium simulations of the solvent force autocorrelation function are in reasonable agreement with the nonequilibrium results.

Journal Article↗
PubMed2001

Vibration characteristics of composite piezoceramic plates at resonant frequencies: experiments and numerical calculations.

The experimental measurement of the resonant frequencies for the piezoceramic material is generally performed by impedance analysis. In this paper, we employ an optical interferometry method called the amplitude-fluctuation electronic speckle pattern interferometry (AF-ESPI) to investigate the vibration characteristics of piezoceramic/aluminum laminated plates. The AF-ESPI is a powerful tool for the full-field, noncontact, and real-time measurement method of surface displacement for vibrating bodies. As compared with the conventional film recording and optical reconstruction procedures used for holographic interferometry, the interferometric fringes of AF-ESPI are produced instantly by a video recording system. Because the clear fringe patterns measured by the AF-ESPI method will be shown only at resonant frequencies, both the resonant frequencies and corresponding vibration mode shapes are obtained experimentally at the same time. Excellent quality of the interferometric fringe patterns for both the in-plane and out-of-plane vibration mode shapes are demonstrated. Two different configurations of piezoceramic/aluminum laminated plates, which exhibit different vibration characteristics because of the polarization direction, are investigated in detail. From experimental results, we find that some of the out-of-plane vibration modes (Type A) with lower resonant frequencies cannot be measured by the impedance analysis; however, all of the vibration modes of piezoceramic/aluminum laminated plates can be obtained by the AF-ESPI method. Finally, the numerical finite element calculations are also performed, and the results are compared with the experimental measurements. Excellent agreements of the resonant frequencies and mode shapes are obtained for both results.

Letter↗
PubMed1991

Transdermal delivery of insulin by ultrasonic vibration.

Ultrasonic vibration has been used to deliver insulin through the skin of hairless mice fasted overnight and partially immersed in an aqueous solution of insulin (20 units mL-1). The skin surface was exposed to ultrasonic vibration in two ultrasonic energy ranges (3000-5000 Pa and 5000-8000 Pa) at 48 kHz for 5 min. Blood glucose concentration was measured before and after exposure to insulin and ultrasonic vibration. In the group subjected to the lower energy vibrations, blood glucose fell rapidly to reach 34 +/- 11.9% of control values in 120 min, while when the animals were exposed to higher energy vibrations, the fall in blood glucose was 22.4 +/- 3.9% of control values at 120 min. The values remained low for the length of the experiment (240 min). Those exposed to insulin alone or ultrasonic vibration alone revealed no significant change in blood glucose concentration. It is postulated that ultrasonic vibration may alter skin permeability resulting in the absorption of insulin. That the blood glucose decrease was greater at the higher of the two energy ranges, suggests this factor could control insulin delivery.

Administration, Cutaneous↗
PubMed1994

Operating hand-held vibrating tools and prevalence of white fingers.

Hand-transmitted vibration levels (HTVLs) and the prevalence of vibration-induced white finger (VWF) and numbness of the hands were investigated in eight groups of subjects operating various hand-held vibrating tools. The prevalence rates of Raynaud's phenomenon (RP) and numbness of the hands in 1,027 males and 1,301 females not occupationally exposed to vibration were compared to those of the exposed subjects. The prevalence of VWF was in the range of 0.0-4.8% in subjects exposed to HTLVs of between 1.1 to 2.5 m/s2 and reached 9.6% in a group of workers exposed to HTLVs of 2.7-5.1 m/s2. The latter group showed a significant difference (P < 0.05) in the prevalence of VWF compared to the 2.7% prevalence of RP in male subjects of the general population. The prevalence of VWF in female subjects exposed to vibration (4.3%) was not significant compared to the prevalence of RP in females of the general population (3.4%). The prevalence rates of numbness of the hands were between 6.5% and 30.4% in the exposed groups and in the range of 13.4-29.5% in the general population. It was concluded that in decisions concerning quantitative recommendations for vibration exposure, the prevalence of VWF should be employed. To decrease the risk of developing VWF, estimated vibration safety values for 4 h and 2 h daily exposures are discussed.

Adult↗
PubMed1984

Mechanical vibration and sound levels experienced in neonatal transport.

Exposure of neonates to sound and to mechanical vibration was measured while transferring the neonates to a regional referral unit by ambulance and by rotary wing and fixed wing aircraft. Recordings were made during different phases of each type of transportation and were analyzed later. In the nursery, sound levels ranged from 72 to 74 dBA (A-weighted decibel level) (77 to 81 dB), while in transit, levels were higher at 78 to 99 dBA (90 to 110 dB), depending on the means of transport. Vibration was measured in the horizontal and vertical axes relative to the neonate in different frequency ranges. The vibration acceleration magnitude ranged from 0.4 m/sq s to 5.6 m/sq s, depending on the axis and type of transport; the maximum obtained was in rotary wing transport. When compared with adult tolerance levels, both sound and vibration exposure of the neonate are high and potentially hazardous. Further evaluation of vibration stress and means of attenuating sound and vibration in transport infant incubators is desirable to enhance the safety of transported infants.

Aircraft↗
PubMed1999

Exposure-response relationship between hand-arm vibration and vibrotactile perception sensitivity.

BACKGROUND: The objectives of the study were to examine whether occupational use of vibrating hand-held tools was associated with an impaired vibrotactile perception, whether any exposure-response relationship exists, and whether the different populations of mechano-receptive afferent units are equally affected. METHODS: Vibrotactile perception thresholds have been measured at seven frequencies (8-500 Hz) and evaluated among 125 vibration-exposed and 45 non-exposed male employees in a heavy engineering production workshop. Vibration exposure measurements were assessed on tools in accordance with ISO 5349. Vibrotactile perception thresholds have been individually graded in stages and placed in relation to individual vibration exposure. RESULTS: The outcome did not reveal a clear relationship between vibration exposure and reduced vibrotactile sensitivity on an individual basis. There was a clear tendency on a group basis towards elevated thresholds when the study population was divided into three exposure categories. A fourfold increase in relative risk of reduced vibrotactile sensitivity for test frequencies above 40 Hz was observed between the highest exposure category compared to the non-exposed. CONCLUSIONS: It was concluded that reduced tactile sensitivity is related to the degree of vibration exposure but it is not at present possible to delineate an exposure-response relationship.

Adult↗
PubMed2004

Vibration exposure and disease in a shipyard: a 13-year revisit.

BACKGROUND: In a 1988 study of shipyard workers, a progressive association was observed between cumulative exposure to vibration and the vascular and neurological symptoms of the hand-arm vibration syndrome (HAVS). In 2001, after a decade of exposure reduction and ageing of the workforce, a second study at the same site was initiated. METHODS: In 2001, 214 subjects were selected; they represented four current weekly vibration exposure time intervals--0 hr, >0 < 5 hr, > or =5 < 20 hr, > or =20 hr. The 1988 and 2000 cross-sectional populations were compared on the basis of exposure duration and current symptoms. RESULTS: In 2001, the study population was 9.6 years older than the 1988 group. Current weekly exposure hours were similar in the low and medium exposure groups 2001 and 1988, but exposure was reduced by an average of 9.7 hr per week in the highest exposure group (> or =20 hr) in 2001. Symptom severity was regressed polychotomously on estimated exposure (log cumulative hours); the OR was weaker in 2001 than in 1988 for sensorineural symptoms-1.44 [CI 1.04-1.98] versus 2.35 [CI 1.48-3.73]. This was also true for vascular symptoms-1.70 [CI 1.06-2.71] versus 3.99 [CI 2.27-7.01]. Vascular symptoms were more prevalent in the highest lifetime vibration exposure group in 1988 (68.7 vs. 43.2% in 2001); sensorineural symptoms were more prevalent in the least vibration exposed group in 2001 (52.6 vs. 20.7% in 1988). CONCLUSIONS: The prevalence of vascular symptoms associated with cumulative vibratory exposure was significantly greater in 1988, but neurological symptoms were more common at lower exposure levels in 2001. The presumption that reducing exposure duration alone is sufficient, in the absence of change in vibration magnitude, is not supported by the results of this study.

Adult↗
PubMed1995

Tonic vibration reflex and muscle afferent block in writer's cramp.

Patients with focal dystonia take advantage of certain cutaneous or proprioceptive sensory inputs to alleviate their symptoms ("sensory trick"). We examined the effects of increasing muscle spindle activity by the tonic vibration reflex maneuver and decreasing it by intramuscular injection of lidocaine. The vibration was applied to the palm or the tendon of forearm muscles in 15 patients with writer's cramp and 15 age-matched normal subjects. In 11 patients, the vibration induced dystonic postures or movements typical of those seen during writing. Normal subjects showed either no response to the vibration or a gradually developing tonic vibration reflex only in the wrist and finger flexors, which produced visible movements with a significantly longer latency (12.5 +/- 6.7 seconds [mean +/- standard deviation]) than what was observed in the patients (2.7 +/- 2.5 seconds, p < 0.0001). Local injection of lidocaine (0.5%, 5-40 ml/muscle) attenuated the tendon reflex with relatively little effect on the M response. Injection into muscles with increased activity produced marked reduction of dystonic movements and significant clinical improvement in 13 patients, whereas injection into the other muscles had no effect. The clinical benefit lasted for 1 to 24 hours after injection. In 13 patients who had additional injections of 10% ethanol, which blocks sodium channels for a longer period than does lidocaine, the duration of action was prolonged to 5 to 21 days. These findings suggest that muscles causing dystonic movements have abnormal sensitivities to vibration at rest and that muscle afferents may play a pivotal role in producing dystonic movements.(ABSTRACT TRUNCATED AT 250 WORDS)

Adult↗
PubMed1986

Measurement of small mechanical vibrations of brain tissue exposed to extremely-low-frequency electric fields.

Electromagnetic fields can interact with biological tissue both electrically and mechanically. This study investigated the mechanical interaction between brain tissue and an extremely-low-frequency (ELF) electric field by measuring the resultant vibrational amplitude. The exposure cell is a section of X-band waveguide that was modified by the addition of a center conductor to form a small TEM cell within the waveguide structure. The ELF signal is applied to the center conductor of the TEM cell. The applied ELF electric field generates an electrostrictive force on the surface of the brain tissue. This force causes the tissue to vibrate at a frequency equal to twice the frequency of the applied sinusoidal signal. An X-band signal is fed through the waveguide, scattered by the vibrating sample, and detected by a phase-sensitive receiver. Using a time-averaging spectrum analyzer, a vibration sensitivity of approximately 0.2 nmp-p can be achieved. The amplitude of the brain tissue vibrational response is constant for vibrational frequencies below 50 Hz; between 50 and 200 Hz resonant phenomena were observed; and above 200 Hz the amplitude fall-off is rapid.

Animals↗
PubMed2002

Vibration injury damages arterial endothelial cells.

Prolonged exposure to hand-transmitted vibration can cause debilitating neural and vascular dysfunction in humans. It is unclear whether the pathophysiology involves simultaneous or sequential injury of arteries and nerves. The mechanism of vibration injury was investigated in a rat tail model, containing arteries and nerves structurally similar to those in the human hand. Tails were selectively vibrated for 1 or 9 days with the remainder of the animal at rest. One vibration bout of 4 h/day, 60 HZ, 5 g (49 m/s(2)) acceleration, injured endothelial cells. Injury was signaled by elevated immunostaining for NFATc3 transcription factor. Electron microscopy revealed that vibration for 9 days produced loss and thinning of endothelial cells, with activated platelets coating the exposed subendothelial tissue. Endothelial cells and arterial smooth muscle cells contained double membrane-limited, swollen processes indicative of vasoconstriction-induced damage. Laser doppler surface recording demonstrated that 5 min of vibration significantly diminished tissue blood perfusion. These findings indicate that early injury involves vasoconstriction and denuding of the arterial endothelium.

Animals↗
PubMed1992

Muscle fatigue measured with evoked muscle vibrations.

Skeletal muscle vibrates laterally during voluntary and evoked muscle contractions. We hypothesized that the vibration amplitude from evoked muscle twitches is directly related to evoked twitch force from fatiguing muscle. To test the hypothesis, vibrations produced by evoked muscle twitches were recorded during short (5-second) rest periods as the muscle was intermittently exercised with voluntary contractions. Trials were performed at 30%, 50%, and 70% of maximal voluntary contraction. Evoked muscle twitches eliminated the problems of motivation and tremor that complicate sound and vibration measurements during voluntary contractions. Results from the first dorsal interosseus hand muscle in 11 normal adult volunteers revealed that the vibration amplitude is highly correlated (r2 = 0.93, at 70% MVC, r2 = 0.97, at 50% MVC; r2 = 0.85, at 30% MVC) with force. Both potentiation and reduction of force with exercise were accompanied by parallel changes in vibration amplitude, as measured with an accelerometer. Compound muscle action potentials did not increase with exercise-induced twitch potentiation, and did not correlate as highly with force during fatigue.

Action Potentials↗
PubMed2003

Vibration signals from the FT joint can induce phase transitions in both directions in motoneuron pools of the stick insect walking system.

The influence of vibratory signals from the femoral chordotonal organ fCO on the activities of muscles and motoneurons in the three main leg joints of the stick insect leg, i.e., the thoraco-coxal (TC) joint, the coxa-trochanteral (CT) joint, and the femur-tibia (FT) joint, was investigated when the animal was in the active behavioral state. Vibration stimuli induced a switch in motor activity (phase transition), for example, in the FT joint motor activity switched from flexor tibiae to extensor tibiae or vice versa. Similarly, fCO vibration induced phase transitions in both directions between the motoneuron pools of the TC joint and the CT joint. There was no correlation between the directions of phase transition in different joints. Vibration stimuli presented during simultaneous fCO elongation terminated the reflex reversal motor pattern in the FT joint prematurely by activating extensor and inactivating flexor tibiae motoneurons. In legs with freely moving tibia, fCO vibration promoted phase transitions in tibial movement. Furthermore, ground vibration promoted stance-swing transitions as long as the leg was not close to its anterior extreme position during stepping. Our results provide evidence that, in the active behavioral state of the stick insect, vibration signals can access the rhythm generating or bistable networks of the three main leg joints and can promote phase transitions in motor activity in both directions. The results substantiate earlier findings on the modular structure of the single-leg walking pattern generator and indicate a new mechanism of how sensory influence can contribute to the synchronization of phase transitions in adjacent leg joints independent of the walking direction.

Animals↗