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Register a new userSound emission from the gas of molecular superrotors
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We use an optical centrifuge to deposit a controllable amount of rotational energy into dense molecular ensembles. Subsequent rotation-translation energy transfer, mediated by thermal collisions, results in the localized heating of the gas and generates strong sound wave, clearly audible to the unaided ear. For the first time, the amplitude of the sound signal is analyzed as a function of the experimentally measured rotational energy. The proportionality between the two experimental observables confirms that rotational excitation is the main source of the detected sound wave. As virtually all molecules, including the main constituents of the atmosphere, are amenable to laser spinning by the centrifuge, we anticipate this work to stimulate further development in the area of photo-acoustic control and spectroscopy.
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Simultaneous measurements of hard X-ray by a Geiger counter and audible sound (10 Hz-20kHz) by a microphone from a thin water film in air were carried out under intense single and double pulse irradiations of femtosecond laser (35 fs, 800 nm, 1 kHz). Emission profiles of X-ray and sound under the single pulse irradiation by changing the water film position along the laser incident direction (Z-axis) show the same peak positions with a broader emission in sound (403{mu}m at FWHM) than in X-ray (37{mu}m). Under the double pulse irradiation condition with the time delay at 0 ps and 4.6 ns, it was clearly observed that the acoustic signal intensity is enhanced in associated with X-ray intensity enhancements. The enhancements can be assigned to laser ablation dynamics such as pre-plasma formation and transient surface roughness formation induced by the pre-pulse irradiation. For the acoustic signal under the double-pulse irradiation with the time delay, there was a weak dependence observed on the pre-pulse irradiation position at the laser focus. It is consistent with a long breakdown filament formation which makes the microphone-detection less position-sensitive.
Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and modify the potential, thereby affecting the ionization process. By using an attosecond two-color interferometric approach in combination with high spectral resolution, we have captured the changes induced by the nuclear motion on the centrifugal barrier that sustains the well-known shape resonance in valence-ionized N$_2$. We show that despite the nuclear motion altering the bond length by only $2%$, which leads to tiny changes in the potential barrier, the corresponding change in the ionization time can be as large as $200$ attoseconds. This result poses limits to the concept of instantaneous electronic transitions in molecules, which is at the basis of the Franck-Condon principle of molecular spectroscopy.
We present a comprehensive characterization of cold molecular beams from a cryogenic buffer-gas cell, providing an insight into the physics of buffer-gas cooling. Cold molecular beams are extracted from a cryogenic cell by electrostatic guiding, which is also used to measure their velocity distribution. Molecules rotational-state distribution is probed via radio-frequency resonant depletion spectroscopy. With the help of complete trajectory simulations, yielding the guiding efficiency for all of the thermally populated states, we are able to determine both the rotational and the translational temperature of the molecules at the output of the buffer-gas cell. This thermometry method is demonstrated for various regimes of buffer-gas cooling and beam formation as well as for molecular species of different sizes, $rm{CH_3F}$ and $rm{CF_3CCH}$. Comparison between the rotational and translational temperatures provides evidence of faster rotational thermalization for the $rm{CH_3F-He}$ system in the limit of low He density. In addition, the relaxation rates for different rotational states appear to be different.
We consider solid surface scattering of molecules that were subject to strong non-resonant ultrashort laser pulses just before hitting the surface. The pulses modify the rotational states of the molecules, causing their field free alignment, or a rotation with a preferred sense. We show that field-free laser-induced molecular alignment leads to correlations between the scattering angle and the sense of rotation of the scattered molecules. Moreover, by controlling the sense of laser induced unidirectional molecular rotation, one may affect the scattering angle of the molecules. This provides a new means for separation of mixtures of molecules (such as isotopes and nuclear-spin isomers) by laser controlled surface scattering.
Localized heating of a gas by intense laser pulses leads to interesting acoustic, hydrodynamic and optical effects with numerous applications in science and technology, including controlled wave guiding and remote atmosphere sensing. Rotational excitation of molecules can serve as the energy source for raising the gas temperature. Here, we study the dynamics of energy transfer from the molecular rotation to heat. By optically imaging a cloud of molecular superrotors, created with an optical centrifuge, we experimentally identify two separate and qualitatively different stages of its evolution. The first non-equilibrium gyroscopic stage is characterized by the modified optical properties of the centrifuged gas - its refractive index and optical birefringence, owing to the ultrafast directional molecular rotation, which survives tens of collisions. The loss of rotational directionality is found to overlap with the release of rotational energy to heat, which triggers the second stage of thermal expansion. The crossover between anisotropic rotational and isotropic thermal regimes is in agreement with recent theoretical predictions and our hydrodynamic calculations.
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