# High sensitivity two-photon spectroscopy in a dark optical trap, based on electron shelving.

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## Abstract

We propose a new spectroscopic method for measuring weak transitions in cold and trapped atoms, which exploits the long interaction times and tight confinement offered by dark optical traps together with an electron shelving technique to achieve extremely high sensitivity. We demonstrate our scheme by measuring a $`5S_{1/2}5D_{5/2}`$ two-photon transition in cold Rb atoms trapped in a new single-beam dark optical trap, using an extremely weak probe laser power of $`25`$ $`\mu `$W. We were able to measure transitions with as small excitation rate as 0.09 sec<sup>-1</sup>.   

PACS number(s): 39.30.+w, 32.80.Pj, 32.80.Rm, 32.90.+a   

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The strong suppression of Doppler and time-of-flight broadenings due to the ultra low temperatures, and the possibility to obtain very long interaction times are obvious advantages of using cold atoms for spectroscopy. Convincing examples of such precision spectroscopic measurements are cold atomic clocks . For RF clock transitions long interaction time is usually obtained in an atomic fountain , while for optical metastable clock transitions free expanding atomic clouds are used .

Even longer interaction times can be obtained for cold atoms trapped in optical dipole traps. To obtain long atomic coherence times, spontaneous scattering of photons and energy level perturbations caused by the trapping laser are reduced by increasing the laser detuning from resonance . To further reduce scattering, blue-detuned optical traps, where repulsive light forces confine atoms mostly in the dark (dark traps), have been developed, achieving atomic coherence of 7 s . The wide use of dark traps was limited by relatively complex setups that require multiple laser beams or gravity assistance. Recent development of single-beam dark traps make them more attractive for precision spectroscopy ,.

Dark traps have an additional advantage that makes them especially useful for the spectroscopic measurements of extremely weak optical transitions. While preserving long atomic coherence times those traps can provide large spring constants and tight confinement of trapped atoms  to ensure good spatial overlap even with a tightly focused excitation laser beam. Therefore the atoms can be exposed to a much higher intensity of the excitation laser, yielding a further increase in sensitivity for very weak transitions.

In this letter we present a new and extremely sensitive method for measuring weak transitions with cold atoms in a far detuned single-beam dark trap using electron shelving spectroscopy . Recently, a similar technique was adapted to demonstrate quantum-limited detection of narrow-linewidth transitions on a free expanding cold atomic cloud . Our scheme is based on a $`\mathrm{\Lambda }`$ system. Atoms with two ground states (for example, two hyperfine levels) are stored in the trap in a level $`|g_1`$ that is coupled to the upper (excited) state, $`|e`$, by an extremely weak transition. An atom that undergoes the weak transition, may be shelved by a spontaneous Raman transition on the second ground level, $`|g_2`$, that is uncoupled to the excited level by the weak transition. After waiting long enough, a significant fraction of the atoms will be shelved on this second level. Finally, the detection scheme benefits from the multiply excited fluorescence of a strong closed transition from $`|g_2`$, that utilizes quantum amplification due to the electron shelving technique.

We realized this scheme on a $`5S_{1/2}5D_{5/2}`$ two-photon transition in cold and trapped <sup>85</sup>Rb atoms (see Fig. 1 for the relevant energy levels) using extremely weak ($`25`$ $`\mu `$W) laser beam and we were able to measure transitions with an excitation rate as small as 0.09 s<sup>-1</sup>.

Precision spectroscopy of the two-photon transition in Rb atoms was previously demonstrated in a hot vapor with much higher laser power . In cold Rb atoms this transition was measured either on free expanding atoms using a mode-locked laser  or on atoms trapped in a doughnut mode magneto-optical trap. In all those schemes the fluorescent $`420`$ nm photons were used to detect the two-photon transition.

Our spectroscopic measurement was made on cold <sup>85</sup>Rb atoms trapped in a rotating-beam optical trap (ROBOT). The operation principles of the ROBOT are described elsewhere . Briefly, a linearly polarized, tightly focused ($`16`$ $`\mu `$m $`1/e^2`$ radius) Gaussian laser beam is rapidly ($`100`$ kHz) rotated by two perpendicular acousto-optic scanners, as seen in Fig. 2. This forms a dark volume which is completely surrounded by a time-averaged dipole potential walls. The wavelength of the trapping laser was $`770`$ nm ($`10`$ nm above the D<sub>2</sub> line) and its power was $`380`$ mW. The initial radius of the rotation was optimized for efficient loading of the ROBOT from a magneto-optical trap (MOT). $`700`$ ms of loading, $`47`$ ms of compression and $`3`$ ms of polarization gradient cooling produced a cloud of $`3\times 10^8`$ atoms, with a temperature of $`9`$ $`\mu `$K and a peak density of $`1.5\times 10^{11}`$ cm<sup>-3</sup>. On the last stage of the loading procedure, the atoms were optically pumped into the $`F=2`$ ground state by shutting off the repumping laser $`1`$ ms before shutting off the MOT beams.

After all laser beams were shut off (except for the ROBOT beam which was overlapping the center of the MOT), $`310^5`$ atoms were typically loaded into the trap, with temperature and density comparable with those of the MOT. Next, we adiabatically compressed the trap by reducing the radius of rotation of the trapping beam from $`70`$ $`\mu `$m to $`29`$ $`\mu `$m such that the atoms will match the waist of the two-photon laser, to further increase the efficiency of the transition. The size of the final cloud in the radial direction was measured by absorption imaging and the temperature of the atoms was measured by time of flight fluorescence imaging. From these measurements and using our precise characterization of the trapping potential , the parameters of the final cloud are: radial size ($`1/e^{2\text{ }}`$radius) of $`19`$ $`\mu `$m, axial size of $`750`$ $`\mu `$m, rms temperatures of $`55`$ $`\mu `$K \[$`9`$ $`\mu `$K\] in the radial \[axial\] direction, and a density of $`710^{11}`$atoms/cm<sup>-3</sup>. The $`1/e`$ lifetime of atoms in the trap was measured to be $`350`$ ms for both hyperfine ground-states and was limited by collisions with background atoms. We measured the spin relaxation time of the trapped atoms to be $`>1`$ s, by measuring spontaneous Raman scattering between the two ground state levels .

The spectroscopy was performed with an external-cavity diode laser which was tuned to the $`5S_{1/2}F=35D_{5/2}F^{}`$ two-photon transition ($`777.9`$ nm) and was split into two parts. The first part ($`10`$ mW) was used to frequency stabilize the laser using the $`420`$ nm fluorescence signal from the two-photon excitation obtained from a $`130^0C`$ Rb vapor cell. The laser was focused into the cell to $`100`$ $`\mu `$m $`1/e^2`$ radius and reflected back to obtain Doppler-free spectra. We locked the laser to the atomic line either by Zeeman modulation technique or directly to the side of the line. From the locking signal we estimated the peak-to-peak frequency noise of the laser to be $`3`$MHz. The second part of the diode laser beam passed through an acousto-optic modulator that shifted the laser frequency toward two-photon resonance with the $`5S_{1/2}F=25D_{5/2}F^{}`$ transition. The laser beam was then focused to a $`26`$ $`\mu m`$ ($`1/e^2`$ radius) spot size in the center of the vacuum chamber, in order to optimize the efficiency of the two-photon transition and was carefully aligned with the long (axial) axis of the ROBOT.

We used a normalized detection scheme to measure the fraction of atoms transferred to $`F=3`$ by the two-photon laser. To detect the total number of atoms in the trap we applied a strong $`200`$ $`\mu `$s laser pulse, resonant with the $`5S_{1/2}F=35P_{3/2}F=4`$ closed transition together with the repumping laser and imaged the fluorescent signal on photomultiplier tube (PMT). To measure only the $`F=3`$ population we applied the detection pulse without the repumping laser. The $`F=3`$ atoms were simultaneously accelerated and Doppler-shifted from resonance by the radiation pressure of the detection beam within the first $`100`$ $`\mu `$s of the pulse. Then we could detect the $`F=2`$ atoms by switching on the repumping laser that pumped $`F=2`$ population to the $`F=3`$ state where atoms were measured by the second part of the detection pulse. This normalized detection scheme is insensitive to shot-to-shot fluctuations in atom number as well as fluctuations of the detection laser frequency and intensity.

After the adiabatic compression of the atoms in the ROBOT was completed, the two-photon laser on resonance with $`5S_{1/2}F=25D_{5/2}F=4`$ was applied for various time intervals and the resulting $`F=3`$ normalized population fraction was detected. The results for a $`170`$ $`\mu `$W two-photon laser are presented on Fig. 3. After $`100`$ ms, $`85\%`$ of the atoms are pumped to the $`F=3`$ state. This steady state population is less then 100% since spontaneous Raman scattering from the trapping laser and from the two-photon laser (absorption of one photon followed by spontaneous emission ) tend to equalize the populations of the two ground levels and therefore compete with the measured two-photon process. The characteristic $`1/e`$ time of the four-photon spontaneous Raman scattering process which is induced by the two-photon laser ($`5S_{1/2}F=25D_{5/2}F^{}6P_{3/2}F^{}5S_{1/2}F=3`$, see Fig. 1) is obtained from a fit to the data as $`\tau _{4p}=25`$ ms. The corresponding (four-photon) rate is $`\gamma _{4p}=1/\tau _{4p}=40`$ s<sup>-1</sup>. Using the theoretical value of the two-photon cross-section of $`\sigma =0.57\times 10^{18}`$cm<sup>4</sup>/W , the exact branching ratio ($`68\%`$) for the two-photon excitation to decay to $`F=3`$ , and our maximal excitation laser intensity of $`16`$ W/cm<sup>2</sup> we calculate $`\gamma _{4p}=391`$s<sup>-1</sup>, a factor of $`10`$ larger than the measured rate. Using a measured value for the two-photon cross-section  yields a somewhat larger value of $`\gamma _{4p}=823`$s<sup>-1</sup>.

The main factor that reduced the measured excitation rate was the linewidth of the two-photon laser that was $`6`$ times larger than the $`300`$ kHz natural linewidth of the two-photon transition. The inhomogeneous broadening due to Stark-shift was calculated for the compressed trapping potential to be $`400`$ kHz, which is smaller than the laser linewidth , hence it does not contribute to the reduced excitation rate. An additional reduction of the excitation rate may be caused by imperfect matching between the trapped atomic sample and the maximal intensity of the two-photon laser, so the overall agreement between the measured and the expected $`\gamma _{4p}`$ is reasonable.

To measure the excitation spectrum of the $`5S_{1/2}F=25D_{5/2}F^{}`$ transition we scanned the frequency of the two-photon laser using the acousto-optic modulator. For each frequency point the whole experimental cycle was repeated, with $`50`$ ms interrogation time of the two-photon laser. The $`F=3`$ fraction of atoms as a function of the frequency of the two-photon laser is presented in Fig. 4a. A $`1.75`$ MHz linewidth (FWHM) of the atomic lines was determined by fitting the data with a multi-peak Gaussian function and is limited by the linewidth of the two-photon laser. This measurement agrees well with the frequency noise of the laser estimated from the locking signal. The distances between the lines obtained from this fit are $`4.48`$ MHz, $`3.76`$ MHz and $`2.76`$ MHz, and are in excellent agreement with previously reported values of $`4.50`$ MHz, $`3.79`$ MHz and $`2.74`$ MHz . The height-ratio between the lines obtained from the fit are $`1:0.86:0.47:0.21`$ for $`F^{}=4,3,2,1`$ respectively. The expected values were calculated using the strength of the two-photon transitions  together with the two photon decay via the $`6P_{3/2}`$ level to be $`1:0.85:0.4:0.1`$, in good agreement with the measured values, except for the weakest line. Note that although the two-photon transition $`F=2F^{}=0`$ is allowed, a two-photon decay with $`\mathrm{\Delta }F=3`$ is forbidden and therefore this line is not detected.

Finally, we reduced the power of the two-photon laser to $`25`$ $`\mu `$W, which reduced the transition rate by a factor of $`46`$. Here, the interrogation time of the two-photon laser was $`500`$ ms and the measured $`F=3`$ population is shown in Fig. 4b. A spectrum similar to that taken with higher intensity is observed. A transition rate as small as $`0.09`$ s<sup>-1</sup> (for the $`F=3F^{}=1`$ transition) is detected in this scan. The ”quantum rate amplification” due to electron shelving (the ratio between the measured $`\gamma _{4p}`$ transition rate and the rate of the one-photon transition used for detecting the F=3 population) is $`10^7`$ for this case.

In conclusion, we demonstrate a new and extremely sensitive scheme to measure weak transitions using cold atoms. The key issues in our scheme are the long spin relaxation times combined with tight confinement of the atoms in a dark optical dipole trap, and the use of a shelving technique to enhance the signal to noise ratio. We demonstrated our scheme by measuring a two-photon transition $`5S_{1/2}5D_{5/2}`$ for <sup>85</sup>Rb atoms trapped in a far-detuned rotating beam dark trap using only $`25`$ $`\mu `$W laser power. The huge quantum amplification due to electron shelving increases the sensitivity of our scheme far beyond the photon shot noise and technical noise encountered in the direct detection of two-photon induced fluorescence  .

Our measurements may be improved in several ways. Improvements of the lifetime and spin relaxation time of atoms in the trap will allow much longer observation times and enable detection of much weaker transitions. This can be done by increasing the trapping laser detuning, where even longer spin-relaxation times are expected due to quantum interference between the two D lines. Reduction of the linewidth of the two-photon laser will allow further improvements in the sensitivity of our scheme. It can also be combined with mode-locked laser spectroscopy  to obtain even larger sensitivities for a given time-average power of the laser. Finally, our technique can be applied for other weak (forbidden) transitions such as optical clock transitions and parity violating transitions where a much lower mixing with an allowed transition could be used.