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The Journal of Chemical Physics

Separation of a benzene and nitric oxide mixture by a molecule prism

Bum Suk Zhao, Sung Hyup Lee, Hoi Sung Chung, Sungu Hwang, Wee Kyung Kang, Břetislav Friedrich, Doo Soo Chung

Published Oct 24, 2003• 38 citations
Publisher

Abstract

In molecule optics, a matter wave of molecules is manipulated by a molecule-optical component made out of external, typically radiative, fields. The molecule-optical index of refraction, n, for a nonresonant IR laser pulse focused onto a molecular beam can be obtained from the energy conservation and wave properties of molecules. Experimentally measured values of n for benzene and nitric oxide agreed well with the calculated values. Since n depends on the properties of molecules as well as those of the laser field, a molecule prism composed of the focused nonresonant laser field can separate a multi-component molecular beam into several components according to their molecule-optical refractive indices n. We obtained a chromatographic resolution of 0.62 for the spatial separation of a mixture beam of benzene and nitric oxide using a focused Nd:YAG laser pulse as a molecule prism.

DOI
10.1063/1.1613934

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In molecule optics, a matter wave of molecules is manipulated by a molecule-optical component made out of external, typically radiative, fields. The molecule-optical index of refraction, n, for a nonresonant IR laser pulse focused onto a molecular beam can be obtained from the energy conservation and wave properties of molecules. Experimentally measured values of n for benzene and nitric oxide agreed well with the calculated values. Since n depends on the properties of molecules as well as those of the laser field, a molecule prism composed of the focused nonresonant laser field can separate a multi-component molecular beam into several components according to their molecule-optical refractive indices n. We obtained a chromatographic resolution of 0.62 for the spatial separation of a mixture beam of benzene and nitric oxide using a focused Nd:YAG laser pulse as a molecule prism.
We describe the deceleration of nitric oxide, benzene and xenon atoms in a molecular beam using one-dimensional pulsed optical lattices created by fields with intensities in the 1012 W cm−2 range. We show that for the same pulse duration and lattice intensity the velocity of the molecules can be controlled by tailoring the lattice velocity. By utilizing the time-dependent oscillatory motion of the molecules within the lattice, we demonstrate the deceleration of nitric oxide from an initial velocity of 400 m s−1 to a final velocity of 290 m s−1 in a single 5.8 ns pulse. Using higher intensities, we measure the deceleration of benzene molecules from 380 m s−1 to 191 m s−1, representing a 75% reduction in the kinetic energy within the lattice over the same duration.
When a molecule is placed in a nonresonant laser field, the Stark interactions between the laser field and the induced molecular dipole result in a mechanical force on the molecule. This nonresonant dipole force is proportional to the intensity gradient of the laser, thus requiring a strong and focused pulsed laser for a sizable impact on the molecule. 36.4 mJ pulses of a 1064 nm Nd:YAG laser focused with a 17.5 cm focal length convex lens produced a 6.4 m/s change in the transverse velocity of a CS2 molecular beam. Using spherical mirrors with shorter focal lengths such as 10.0, 7.5, and 5.0 cm, dipole forces of similar magnitude were obtained with laser pulses of much lower energies. In particular the 5.0-cm focal length spherical mirror provided an 11.3 m/s change in the transverse velocity using 3.6 mJ laser pulses. This corresponds to 18-fold increase in the deflection efficiency, the ratio between the maximum velocity change and the pulse energy. From the improved efficiency, the nonresonant dipole force can be exerted with ease.
The possibility of focusing and trapping molecules in the intensity gradient of a moderately intense laser field is shown. A fully quantum-mechanical and a hybrid quantum-classical model are developed and both the case of a near-resonance and that of a far-off-resonance field are studied numerically and analytically. Molecular focusing is obtained when the ratio between the kinetic energy and the field-matter interaction exceeds unity (but remains small). In this energy regime the laser beam serves as a lens for a beam of molecules. The properties of the “molecular lens” are analyzed and the experimental conditions required to focus molecules are examined. We propose the application of laser focusing to nanoscale deposition onto, and etching of a substrate and describe a possible setup to that end. Molecular trapping is obtained as the strong interaction limit of a general “molecular optics” scheme.
In this study, we extended the coherent control theory proposed by Brumer and Shapiro to bound-continuum transition in a molecular system where control of the ejection direction of photoelectrons in the ionization of nitric oxide was achieved. Nitric oxide was prepared in its first excited Rydberg state and was then ionized simultaneously by two different paths: a one-photon and a two-photon process. The fundamental and second harmonic frequencies of a dye laser were used for the two different ionization processes. Interference due to the two paths was detected by measuring the photoelectrons ejected in a defined solid angle. Changing the relative phase between the two paths resulted in a destructive or constructive interference leading to a decrease or increase of the measured signal, respectively. This study showed that interference experiments are very sensitive, not only to lasers' properties and the optical components, but also to the properties of the molecular system. Laser properties, such as, spatial and temporal mode qualities, power fluctuations and timing, influenced the relative strength of the signals of the two ionization paths. Optical component properties, such as, surface parallelism and quality, affected laser divergence, and therefore, considerably reduced the depth of modulation. As for the molecular system, in a resonance two-photon excitation, appropriate resonance states must be chosen to ensure that the two processes produce electron waves of opposite parities which can interfere constructively to produce an enhancement of electron ejection in a certain direction. Due to the non-ideal properties of the lasers used, it is best to use a non-resonant two-photon ionization as one of the interfering paths. Resonant two-photon ionization, combined with the multi-mode laser greatly reduced the depth of the modulation.
Rydberg state excitations of neutral nitric oxide molecules are studied in strong ultraviolet (UV) and near-infra-red (IR) laser fields using a linear time-of-flight (TOF) mass spectrometer with the pulsed electronic field ionization method. The yield of Rydberg molecules is measured as a function of laser intensity and ellipticity, and the results in UV laser fields are compared with those in near-IR laser fields. The present study provides the first experimental evidence of neutral Rydberg molecules surviving in a strong laser field. The results indicate that a rescattering-after-tunneling process is the main contribution to the formation of Rydberg molecules in strong near-IR laser fields, while multi-photon excitation may play an important role in the strong UV laser fields.
One possible technique is the use of a modified straight Stark guide to filter the slow moving molecules from a thermal source. Here I present such a technique and the design of the necessary apparatus. Furthermore, I present experimental results for creating a molecular source of nitric oxide (NO) whose temperature is controlled. Results showing the effects of the guide on the lowest ro-vibrational states of NO and a new technique for measuring the speed distribution of a cold molecular sample are also discussed. Finally, the use of the guide to produce cold NO molecules at a temperature of 7 +/- 2 K is described.