Biomedical subjects

D M Villeneuve

Publications and source records attributed to D M Villeneuve.

17 recordsLinked to original sources

PubMed2005

Controlling attosecond double ionization dynamics via molecular alignment.

We investigate the dynamics of double ionization in aligned nitrogen molecules. An ultrashort, weak laser pulse creates an aligned ensemble of molecules that is ionized with a subsequent, strong probe pulse. We find that the two electrons involved in nonsequential double ionization more likely exit the molecule in the same direction if it is parallel to the probe laser polarization, indicating that they are ejected within a few hundred attoseconds of each other. Double ionization is less probable and takes longer for perpendicular molecules.

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PubMed2005

Controlling high harmonic generation with molecular wave packets.

We show that, by controlling the alignment of molecules, we can influence the high harmonic generation process. We observed strong intensity modulation and spectral shaping of high harmonics produced with a rotational wave packet in a low-density gas of N2 or O2. In N2, where the highest occupied molecular orbital (HOMO) has sigma(g) symmetry, the maximum signal occurs when the molecules are aligned along the laser polarization while the minimum occurs when it is perpendicular. In O2, where the HOMO has pi(g) symmetry, the harmonics are enhanced when the molecules are aligned around 45 degrees to the laser polarization. The symmetry of the molecular orbital can be read by harmonics. Molecular wave packets offer a means of shaping attosecond pulses.

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PubMed2005

Mapping attosecond electron wave packet motion.

Attosecond pulses are produced when an intense infrared laser pulse induces a dipole interaction between a sublaser cycle recollision electron wave packet and the remaining coherently related bound-state population. By solving the time-dependent Schrödinger equation we show that, if the recollision electron is extracted from one or more electronic states that contribute to the bound-state wave packet, then the spectrum of the attosecond pulse is modulated depending on the relative motion of the continuum and bound wave packets. When the internal electron and recollision electron wave packet counterpropagate, the radiation intensity is lower. We show that we can fully characterize the attosecond bound-state wave packet dynamics. We demonstrate that electron motion from a two-level molecule with an energy difference of 14 eV, corresponding to a period of 290 asec, can be resolved.

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PubMed2005

Shakeup excitation during optical tunnel ionization.

Shakeup of a two-electron system is investigated in the strong infrared laser field limit, both theoretically and experimentally. During tunnel ionization the electron shakes up a second electron to an excited bound state. Theoretically, a complete analytical theory of shakeup in intense laser fields is developed. We predict that shakeup produces one excited sigma(u) D(+)(2) state in approximately 10(5) ionization events. Shakeup is measured experimentally by using the molecular clock provided by the internuclear motion. The number of measured events is found to be in excellent agreement with theory.

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PubMed2004

Tomographic imaging of molecular orbitals.

Single-electron wavefunctions, or orbitals, are the mathematical constructs used to describe the multi-electron wavefunction of molecules. Because the highest-lying orbitals are responsible for chemical properties, they are of particular interest. To observe these orbitals change as bonds are formed and broken is to observe the essence of chemistry. Yet single orbitals are difficult to observe experimentally, and until now, this has been impossible on the timescale of chemical reactions. Here we demonstrate that the full three-dimensional structure of a single orbital can be imaged by a seemingly unlikely technique, using high harmonics generated from intense femtosecond laser pulses focused on aligned molecules. Applying this approach to a series of molecular alignments, we accomplish a tomographic reconstruction of the highest occupied molecular orbital of N2. The method also allows us to follow the attosecond dynamics of an electron wave packet.

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PubMed2004

Phase control of rotational wave packets and quantum information.

Lasers can create rotational wave packets in gas-phase molecules which periodically revive as field-free, aligned distributions. We control the wave packet evolution with relatively weak laser pulses at fractional revivals which modify the phase between wave packet components. We demonstrate two phase control effects in oxygen: coherently switching revivals off and on, and doubling the revival frequency. When viewed as a quantum logic system, these effects correspond to a Hadamard and a T operation.

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PubMed2004

Fully differential rates for femtosecond multiphoton double ionization of neon.

We have investigated the full three-dimensional momentum correlation between the electrons emitted from strong field double ionization of neon when the recollision energy of the first electron is on the order of the ionization potential. The momentum correlation in the direction perpendicular to the laser field depends on the time difference of the two electrons leaving the ion. Our results are consistent with double ionization proceeding through transient double excited states that field ionize.

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PubMed2004

Stopping a vibrational wave packet with laser-induced dipole forces.

Intense near-infrared laser pulses can generate laser-induced dipole forces that are strong enough to influence or control vibrational motion of a small molecule. Generally, the force acts to pull the molecule apart. Our numerical simulations show that, by applying the laser-induced dipole force at an appropriate time within one vibrational period, the wave packet motion of H+2 or D+2 can be accelerated or decelerated. Using the wave packet formed by the rapid ionization of H2 or D2, we also show that it is possible to move the vibrational population almost entirely to the v=0 state. Coherent cooling of the molecular vibrational motion can be achieved.

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PubMed2003

Electron-electron momentum exchange in strong field double ionization.

We have investigated the momentum balance between the two electrons from strong field double ionization of argon at 780 nm and 1.9 x 10(14) W/cm(2). Experimental data show that perpendicular to the laser polarization direction the electrons emerge preferentially in opposite directions. Results of model calculations are found to agree well with the data and reveal a dominant role of the Coulomb correlation between the two outgoing electrons in this kinematical geometry. Differences between the experimental observations and the theoretical results for the ion momentum distribution indicate the importance of the further effects during the three-body breakup.

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PubMed2003

Time-resolved double ionization with few cycle laser pulses.

Ionization of D2 launches a vibrational wave packet on the ground state of D+2. Removal of the second electron places a pair of D+ ions onto a Coulombic potential. Measuring the D+ kinetic energy determines the time delay between the first and the second ionization. Caught between a falling ionization and a rapidly rising intensity, the typical lifetime of the D+2 intermediate is less than 5 fs when an intense 8.6 fs laser pulse is used. We simulate Coulomb explosion imaging of the ground state wave function of D2 by a 4 fs optical pulse and compare with our experimental observations.

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PubMed2003

Alignment-dependent strong field ionization of molecules.

We demonstrate a method to measure strong field laser ionization of aligned molecules. The method employs a macroscopic field-free dynamic alignment, which occurs during revivals of rotational wave packets produced by a femtosecond laser pulse. We investigate the dependence of strong field ionization of N2 on molecular orientation. We determine that N2 molecules are four times more likely to ionize when aligned parallel to the field than when aligned perpendicular to it.

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PubMed2003

Controlling vibrational wave packet motion with intense modulated laser fields.

Intense, nonresonant laser fields produce Stark shifts that strongly modify the potential energy surfaces of a molecule. A vibrational wave packet can be guided by this Stark shift if the laser field is appropriately modulated during the wave packet motion. We modulated a 70 fs laser pulse with a period on the time scale of the vibrational motion (approximately 10 fs) by mixing the signal and idler of an optical parametric amplifier. We used ionization of H2 or D2 to launch a vibrational wave packet on the ground state of H2(+) or D2(+). If the laser intensity was high as the wave packet reached its outer turning point, the Stark shift allowed the molecule to dissociate through bond softening. On the other hand, if the field was small at this critical time, little dissociation was measured. By changing the modulation period, we achieved control of the dissociation yield with a contrast of 90%.

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PubMed2003

Probing molecular dynamics with attosecond resolution using correlated wave packet pairs.

Spectroscopic measurements with increasingly higher time resolution are generally thought to require increasingly shorter laser pulses, as illustrated by the recent monitoring of the decay of core-excited krypton using attosecond photon pulses. However, an alternative approach to probing ultrafast dynamic processes might be provided by entanglement, which has improved the precision of quantum optical measurements. Here we use this approach to observe the motion of a D2+ vibrational wave packet formed during the multiphoton ionization of D2 over several femtoseconds with a precision of about 200 attoseconds and 0.05 ångströms, by exploiting the correlation between the electronic and nuclear wave packets formed during the ionization event. An intense infrared laser field drives the electron wave packet, and electron recollision probes the nuclear motion. Our results show that laser pulse duration need not limit the time resolution of a spectroscopic measurement, provided the process studied involves the formation of correlated wave packets, one of which can be controlled; spatial resolution is likewise not limited to the focal spot size or laser wavelength.

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PubMed2002

Sub-laser-cycle electron pulses for probing molecular dynamics.

Experience shows that the ability to make measurements in any new time regime opens new areas of science. Currently, experimental probes for the attosecond time regime (10(-18) 10(-15) s) are being established. The leading approach is the generation of attosecond optical pulses by ionizing atoms with intense laser pulses. This nonlinear process leads to the production of high harmonics during collisions between electrons and the ionized atoms. The underlying mechanism implies control of energetic electrons with attosecond precision. We propose that the electrons themselves can be exploited for ultrafast measurements. We use a 'molecular clock', based on a vibrational wave packet in H(2)(+) to show that distinct bunches of electrons appear during electron ion collisions with high current densities, and durations of about 1 femtosecond (10(-15) s). Furthermore, we use the molecular clock to study the dynamics of non-sequential double ionization.

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PubMed2001

Quantum interference in double ionization and fragmentation of C(6)H(6) in intense laser fields.

During tunnel ionization of atoms or molecules by strong laser fields, the electron acquires a transverse velocity which is characteristic of the ionization process. Ellipticity measurements identify nonsequential double ionization as due to recollision in C(6)H(6) and simultaneously measure the transverse velocity distribution of the electron wave packet. We observe signatures of quantum interference of different tunneling trajectories and find identical dependence of nonsequential double ionization and fragmentation of C(6)H(6) on the ellipticity of the laser polarization. This identifies electron recollision as the dominant source of fragmentation at 1.4 microm.

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PubMed2001

Few cycle dynamics of multiphoton double ionization.

In intense field ionization, an electron removed from the atomic core oscillates in the combined fields of the laser and the parent ion. This oscillation forces repeated revivals of its spatial correlation with the bound electrons. The total probability of double ionization depends on the number of returns and therefore on the number of optical periods in the laser pulse. We observed the yield of Ne(2+) relative to Ne(+) with 12 fs pulses to be clearly less compared to 50 fs pulses in qualitative agreement with our theoretical model.

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PubMed2000

Forced molecular rotation in an optical centrifuge.

Intense linearly polarized light induces a dipole force that aligns an anisotropic molecule to the direction of the field polarization. Rotating the polarization causes the molecule to rotate. Using femtosecond laser technology, we accelerate the rate of rotation from 0 to 6 THz in 50 ps, spinning chlorine molecules from near rest up to angular momentum states J approximately 420. At the highest spinning rate, the molecular bond is broken and the molecule dissociates.

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