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Physical Review A

Spectroscopic prescription for optimal stimulated Raman transfer of ultracold heteronuclear molecules to the lowest rovibronic level

Jin‐Tae Kim, Yonghoon Lee, Bongsoo Kim, Dajun Wang, William C. Stwalley, P. L. Gould, Edward E. Eyler

Published Dec 21, 2011• 18 citations
Publisher

Abstract

We show that the multiplicative product of a molecular-beam excitation spectrum and an ultracold-molecule excitation spectrum, with a frequency offset appropriate to the initial ultracold-molecule level, provides the relative rate of stimulated Raman transfer (SRT) from a given high rovibrational level to the lowest rovibronic level, i.e., the ${v}^{\ensuremath{'}\ensuremath{'}}=0,{J}^{\ensuremath{'}\ensuremath{'}}=0$ level of the ground electronic state for photoassociated (and magnetoassociated) ultracold molecules. This product spectrum clearly indicates the optimal pathways for SRT, even when the two component spectra are completely unassigned. We illustrate this specifically for the case of KRb.

DOI
10.1103/physreva.84.062511

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Population transfer routes to the lowest vibrational level of ultracold 39K85Rb

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Optimal intermediate vibrational levels for stimulated Raman transfer (SRT) through the 4 1Σ+ state of 39K85Rb to form the lowest vibrational level of the ground X 1Σ+ state from high vibrational levels of the X 1Σ+ state (formed by decay from photoassociated ultracold molecules) have been determined using a multiplicative product of a molecular beam (MB) and an ultracold molecule (UM) excitation spectrum with the appropriate frequency offset.

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Shortcuts for understanding rovibronic spectroscopy of ultracold alkali metal diatomic molecules

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The high-resolution rovibronic spectroscopies of cold and ultracold molecules (e.g. supersonic molecular beam excitation spectra (MB), photoassociation spectra of ultracold atoms (PA), resonance-enhanced multiphoton ionization spectra (REMPI), stimulated Raman transfer (SRT) spectra) are of major current interest. This manuscript summarizes the significant level of understanding of these various spectroscopies, enabled by using simple graphical and semiclassical ideas and shortcuts. Physical realizations of these spectroscopies will be illustrated using the alkali metal diatomic molecules, both homonuclear (e.g. Rb2) and heteronuclear (e.g. KRb).

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Production of ultracold heteronuclear KRb molecules

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This thesis describes the spectroscopy work on ultracold 39K 85Rb molecules as part of our effort towards producing ground-state ultracold polar molecules. ^ The starting points of our experiment are laser cooled and trapped K and Rb atoms in dual-species MOTs and the molecule formation method is photoassociation (PA). A fraction of the PA-produced excited-state molecules can spontaneously emit to the two lowest electronic states, the X 1Σ + state and the a 3Σ + state, to form high vibrational level molecules. In order to develop a population transfer scheme to make deeply bound molecules, we have studied the spectroscopy of KRb in several steps. Besides the PA step, we have also carried out a state-selective detection experiment to study the population distribution of the high vibrational level molecules formed via spontaneous emission. The detection method is pulsed-laser based ion time-of-flight mass spectroscopy. Due to the linewidth limitations of the pulsed laser, this detection method can only resolve vibrational structures. A cw laser induced ion depletion spectroscopy technique has been developed in order to obtain rotational resolution. Using this ion depletion method, we have studied a possible stimulated Raman transfer scheme via the 3 1Σ+ state. To this end, we have obtained all the spectroscopic information required to produce deeply bound KRb molecules in a single vibrational and rotational level. ^ Several other spectroscopic studies using the high vibrational level ultracold molecules are also discussed. ^

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Ultracold heteronuclear polar KRb molecules have enjoyed tremendous attention for many years now. The presence of a large molecule fixed dipole moment in the absolute rovibrational ground state (v''=0, J'' =0) makes external control very convenient, which opens up the prospect of studying various physical phenomenon in many areas of physics and chemistry. The methods used so far to produce the absolute ground state of KRb have involved very complicated techniques. Molecules formed in weakly bound levels were transferred to the absolute ground state through the multiple steps of transfer processes involving several lasers with extremely narrow linewidths. My thesis research demonstrates an alternate simpler method of formation of the lowest vibrational levels of the ground state utilizing PA combined with radiative decay, which has been so far useful to form ultracold molecules in the higher vibrational levels of the ground state. This thesis presents two main topics of research. The first part of the thesis consists of results describing the scheme which provides a single-step, continuous, and irreversible method of forming KRb molecules in their absolute ground state. The second topic involves spectroscopy on the two excited electronic states of KRb which may provide alternative pathways for the formation of the absolute ground state (X 1Σ+, (v''=0, J'' =0)) and suitable pathways for efficient formation of the lowest metastable state (a 3Σ+, (v''=0, N'' =0)). I believe this research will lay the foundation for many new exciting experiments in the future.

•Jan 1, 2013•1 citation

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Resonant Coupling in the Heteronuclear Alkali Dimers for Direct Photoassociative Formation of X(0,0) Ultracold Molecules

W. C. Stwalley, J. Banerjee, M. Bellos +3 more

Promising pathways for photoassociative formation of ultracold heteronuclear alkali metal dimers in their lowest rovibronic levels (denoted X(0,0)) are examined using high-quality ab initio calculations of potential energy curves currently available. A promising pathway for KRb, involving the resonant coupling of the 2(1)Pi and 1(1)Pi states just below the lowest excited asymptote (K(4s) + Rb(5p(1/2))), is found to occur also for RbCs and less promisingly for KCs also. The resonant coupling of the 3(1)Sigma(+) and 1(1)Pi states, also just below the lowest excited asymptote, is found to be promising for LiNa, LiK, and LiRb and less promising for LiCs and KCs. Direct photoassociation to the 1(1)Pi state near dissociation appears promising in the final dimers NaK, NaRb, and NaCs, although detuning more than 100 cm(-1) below the lowest excited asymptote may be required.

arXiv:0909.4347•The Journal of Physical Chemistry A•Dec 7, 2009•40 citations
We show that the multiplicative product of a molecular-beam excitation spectrum and an ultracold-molecule excitation spectrum, with a frequency offset appropriate to the initial ultracold-molecule level, provides the relative rate of stimulated Raman transfer (SRT) from a given high rovibrational level to the lowest rovibronic level, i.e., the v\ensuremath′\ensuremath′=0,J\ensuremath′\ensuremath′=0{v}^{\ensuremath{'}\ensuremath{'}}=0,{J}^{\ensuremath{'}\ensuremath{'}}=0v\ensuremath′\ensuremath′=0,J\ensuremath′\ensuremath′=0 level of the ground electronic state for photoassociated (and magnetoassociated) ultracold molecules. This product spectrum clearly indicates the optimal pathways for SRT, even when the two component spectra are completely unassigned. We illustrate this specifically for the case of KRb.
The high-resolution rovibronic spectroscopies of cold and ultracold molecules (e.g. supersonic molecular beam excitation spectra (MB), photoassociation spectra of ultracold atoms (PA), resonance-enhanced multiphoton ionization spectra (REMPI), stimulated Raman transfer (SRT) spectra) are of major current interest. This manuscript summarizes the significant level of understanding of these various spectroscopies, enabled by using simple graphical and semiclassical ideas and shortcuts. Physical realizations of these spectroscopies will be illustrated using the alkali metal diatomic molecules, both homonuclear (e.g. Rb2) and heteronuclear (e.g. KRb).
This thesis describes the spectroscopy work on ultracold 39K 85Rb molecules as part of our effort towards producing ground-state ultracold polar molecules. ^ The starting points of our experiment are laser cooled and trapped K and Rb atoms in dual-species MOTs and the molecule formation method is photoassociation (PA). A fraction of the PA-produced excited-state molecules can spontaneously emit to the two lowest electronic states, the X 1Σ + state and the a 3Σ + state, to form high vibrational level molecules. In order to develop a population transfer scheme to make deeply bound molecules, we have studied the spectroscopy of KRb in several steps. Besides the PA step, we have also carried out a state-selective detection experiment to study the population distribution of the high vibrational level molecules formed via spontaneous emission. The detection method is pulsed-laser based ion time-of-flight mass spectroscopy. Due to the linewidth limitations of the pulsed laser, this detection method can only resolve vibrational structures. A cw laser induced ion depletion spectroscopy technique has been developed in order to obtain rotational resolution. Using this ion depletion method, we have studied a possible stimulated Raman transfer scheme via the 3 1Σ+ state. To this end, we have obtained all the spectroscopic information required to produce deeply bound KRb molecules in a single vibrational and rotational level. ^ Several other spectroscopic studies using the high vibrational level ultracold molecules are also discussed. ^
Ultracold heteronuclear polar KRb molecules have enjoyed tremendous attention for many years now. The presence of a large molecule fixed dipole moment in the absolute rovibrational ground state (v''=0, J'' =0) makes external control very convenient, which opens up the prospect of studying various physical phenomenon in many areas of physics and chemistry. The methods used so far to produce the absolute ground state of KRb have involved very complicated techniques. Molecules formed in weakly bound levels were transferred to the absolute ground state through the multiple steps of transfer processes involving several lasers with extremely narrow linewidths. My thesis research demonstrates an alternate simpler method of formation of the lowest vibrational levels of the ground state utilizing PA combined with radiative decay, which has been so far useful to form ultracold molecules in the higher vibrational levels of the ground state. This thesis presents two main topics of research. The first part of the thesis consists of results describing the scheme which provides a single-step, continuous, and irreversible method of forming KRb molecules in their absolute ground state. The second topic involves spectroscopy on the two excited electronic states of KRb which may provide alternative pathways for the formation of the absolute ground state (X 1Σ+, (v''=0, J'' =0)) and suitable pathways for efficient formation of the lowest metastable state (a 3Σ+, (v''=0, N'' =0)). I believe this research will lay the foundation for many new exciting experiments in the future.
We propose a type of Feshbach resonance occurring when two different ultracold atoms in their ground state undergo an sss-wave collision in the presence of a laser. The collisional levels of the atom pair are coupled by the laser to a rovibrational molecular level of the same electronic ground state: We name it a laser-assisted self-induced Feshbach resonance. This mechanism, valid for all heteronuclear quantum gas mixtures, is analyzed on the example of ultracold 87Rb^{87}\mathrm{Rb}87Rb and 84Sr^{84}\mathrm{Sr}84Sr atoms for which the resonant laser frequency falls in the subterahertz range. The interspecies scattering length can be controlled with the laser frequency and intensity without atom loss. Moreover, chirping slowly, the frequency allows for the adiabatic formation of ultracold 87Rb84Sr^{87}\mathrm{Rb}\phantom{\rule{0.16em}{0ex}}^{84}\mathrm{Sr}87Rb84Sr molecules in a manner very similar to a magnetic Feshbach resonance. A stimulated Raman adiabatic passage follows for stabilizing the molecules in their rovibronic ground state.
Promising pathways for photoassociative formation of ultracold heteronuclear alkali metal dimers in their lowest rovibronic levels (denoted X(0,0)) are examined using high-quality ab initio calculations of potential energy curves currently available. A promising pathway for KRb, involving the resonant coupling of the 2(1)Pi and 1(1)Pi states just below the lowest excited asymptote (K(4s) + Rb(5p(1/2))), is found to occur also for RbCs and less promisingly for KCs also. The resonant coupling of the 3(1)Sigma(+) and 1(1)Pi states, also just below the lowest excited asymptote, is found to be promising for LiNa, LiK, and LiRb and less promising for LiCs and KCs. Direct photoassociation to the 1(1)Pi state near dissociation appears promising in the final dimers NaK, NaRb, and NaCs, although detuning more than 100 cm(-1) below the lowest excited asymptote may be required.