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Physical Review A

Anderson localization in laser-kicked molecules

Johannes Floß, Shmuel Fishman, Ilya Sh. Averbukh

Published Aug 30, 2013• 30 citations
Publisher

Abstract

The paper explores the prospects of observing the phenomenon of dynamical Anderson localization via nonresonant Raman-type rotational excitation of molecules by periodic trains of short laser pulses. We define conditions for such an experiment and show that current femtosecond technology used for nonadiabatic laser alignment of linear molecules is sufficient for this task. Several observables which can serve as indicators for Anderson localization are suggested for measurement, and the influence of experimental limitations imposed by the laser intensity noise, finite pulse duration, limited number of pulses in a train, and thermal effects is analyzed.

DOI
10.1103/physreva.88.023426

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The paper explores the prospects of observing the phenomenon of dynamical Anderson localization via nonresonant Raman-type rotational excitation of molecules by periodic trains of short laser pulses. We define conditions for such an experiment and show that current femtosecond technology used for nonadiabatic laser alignment of linear molecules is sufficient for this task. Several observables which can serve as indicators for Anderson localization are suggested for measurement, and the influence of experimental limitations imposed by the laser intensity noise, finite pulse duration, limited number of pulses in a train, and thermal effects is analyzed.
The paper explores the prospects of observing the phenomenon of dynamical Anderson localisation via non-resonant Raman-type rotational excitation of molecules by periodic trains of short laser pulses. We define conditions for such an experiment, and show that current femtosecond technology used for non-adiabatic laser alignment of linear molecules is sufficient for this task. Several observables which can serve as indicator for Anderson localisation are suggested for measurement, and the influence of experimental limitations imposed by laser intensity noise, finite pulse duration, limited number of pulses in a train, and thermal effects is analysed.
We report the observation of rotational Bloch oscillations in a gas of nitrogen molecules kicked by a periodic train of femtosecond laser pulses. A controllable detuning from the quantum resonance creates an effective accelerating potential in angular momentum space, inducing Bloch-like oscillations of the rotational excitation. These oscillations are measured via the temporal modulation of the refractive index of the gas. Our results introduce room-temperature laser-kicked molecules as a new laboratory for studies of localization phenomena in quantum transport.
We evaluate the shifts imparted to vibrational and rotational levels of a linear molecule by a nonresonant laser field at intensities of up to 10(12) W/cm(2). Both types of shift are found to be either positive or negative, depending on the initial rotational state acted upon by the field. An adiabatic field-molecule interaction imparts a rotational energy shift which is negative and exceeds the concomitant positive vibrational shift by a few orders of magnitude. The rovibrational states are thus pushed downward in such a field. A nonresonant pulsed laser field that interacts nonadiabatically with the molecule is found to impart rotational and vibrational shifts of the same order of magnitude. The nonadiabatic energy transfer occurs most readily at a pulse duration which amounts to about a tenth of the molecule's rotational period and vanishes when the sudden regime is attained for shorter pulses. We applied our treatment to the much-studied (87)Rb(2) molecule in the last bound vibrational levels of its lowest singlet and triplet electronic states. Our calculations indicate that 15 and 1.5 ns laser pulses of an intensity in excess of 5 x 10(9) W/cm(2) are capable of dissociating the molecule due to the vibrational shift. Lesser shifts can be used to fine-tune the rovibrational levels and thereby affect collisional resonances by the nonresonant light. The energy shifts due to laser intensities of 10(9) W/cm(2) may be discernible spectroscopically, with a 10 MHz resolution.
Molecules in selected rotational states can remain well aligned for extended periods of time in the presence of an appropriate periodic train of nonresonant laser pulses. Here, we show that these states can be prepared by slowly switching the electromagnetic field amplitude during a sequence of laser pulses. For low-temperature ensembles, a high degree of alignment can be achieved by designing pulse trains that take into account the distribution of avoided crossings between quasienergy curves. Additionally, we present calculations that illustrate several effects causing misalignment. A discussion of subtleties concerning systems with unbounded rotational spectra is also included.
We theoretically demonstrate that the molecular rotational state populations through an impulsive nonresonant Raman process can be manipulated by shaping the femtosecond laser pulse with a periodic phase-step modulation. We show that, by precisely controlling these parameters characterizing the periodic phase-step modulation, both the odd and even rotational state populations can be completely suppressed or reconstructed as that induced by the transform-limited laser pulse, and the relative excitation between the odd and even rotational state populations can also be obtained. Furthermore, we show that the field-free molecular alignment can be manipulated due to the modulation of the odd and even rotational state populations.