ISMS, UIUC, June 19, 2014 Broadband Optical + Cooling of AlH to the Rotational Ground State Christopher M. Seck, Chien-Yu Lien, Brian C. Odom Physics & Astronomy, Northwestern University RH10 ISMS, UIUC June 19, 2014 ISMS, UIUC, June 19, 2014 Motivation Quantum control of atomics revolutionary.
Extend quantum control toolbox to molecules. State manipulation requires rotational control. Coherent control, ultracold & quantum chemistry, etc. Quantum computing Alignme nt Time-varying constants NJP 11, 055049
(2009) p Orientati on e- + ? =
( ) 2 ISMS, UIUC, June 19, 2014 Difficulty of Molecules Ba+ State manipulation in atomics easy. No closed cycling transitions in molecules. Electronic relaxation generally excites vibrations. Large thermal distribution at room temperature.
Each populated state requires unique laser frequency. 3 ISMS, UIUC, June 19, 2014 Difficulty of Molecules 360 nm 1600 cm-1 = 2400 K AlH+ advantages: 30 electronic excitation-relaxation cycles. 99.9% in v = 0, 96% among N = 0 9 at 300 K. P- well separated from Q-, R-branches.
14 cm-1 (420 GHz) between P-/Q-branches. 4 ISMS, UIUC, June 19, 2014 BROC Broadband Rotational Optical Cooling. Selectively drive P-branch. Parity barrier between N = 0, 1.
Timescale of s via 10 electronic excitation-relaxations.s via 10 electronic excitation-relaxations. < scatters before vibrational excitation. 5 ISMS, UIUC, June 19, 2014 BROC Drive P-branch, avoiding P(1). Spectral cutoff width < 2 cm-1. 6 ISMS, UIUC, June 19, 2014
SFPL for AlH + Spectrally-filtered Pulsed Laser. 4-f configuration common to fs pulse-shaping. SHG Spectra-Physics Mai Tai HP. Vibrational cooling of Cs2 by Orsay group [Viteau et al, Science 321, 5886 (2008)]. 7
ISMS, UIUC, June 19, 2014 Apparatus and Experiment r0 = 3 mm z0 = 15 mm RF = 2 2.35 MHz, 300 V 2 2.35 MHz, 300 V.35 MHz, 300 VPP ECs = 850 VDC Ablation-load, laser cool Ba+. Ablation-load 50 Al+. Translational motion sympathetically cooled. AlH+ formed from background gas 1 minute. 8
ISMS, UIUC, June 19, 2014 Apparatus and Experiment Ablation-load, laser cool Ba+. Ablation-load 50 Al+. Translational motion sympathetically cooled. AlH+ formed from background gas 1 minute. Apply rotational cooling, state-selective (1+1) REMPD. TOFMS using analog-mode Hamamatsu MCP. 9 ISMS, UIUC, June 19, 2014 Apparatus and Experiment
TOF resolves Al+ (27 u) and AlH+ (28 u). Ion numbers calculated by integrated signal in each bin. Al+ fraction is molecule population in targeted rotational state. 10 ISMS, UIUC, June 19, 2014 Results and Discussion Initial (red diamonds) and BROC (green circles) distributions. 11 ISMS, UIUC, June 19, 2014
Results and Discussion 300 K thermal distribution. Initial (red diamonds) and BROC (green circles) distributions. 12 ISMS, UIUC, June 19, 2014 Results and Discussion 94(5)% in N = 0, 1. T (+ parity) < 13 K. T (- parity) < 19 K. Initial (red diamonds) and BROC (green circles) distributions.
Toy Monte Carlo method used for statistical analysis. 13 ISMS, UIUC, June 19, 2014 VA-BROC Vibrationally-Assisted Broadband Rotational Optical Cooling. Drive P(1) until v = 1 decay. Relaxation to v = 0 provides 3rd photon. Cooling light then pumps to single-parity rotational ground state.
Timescale set by vibrational decay of 100 ms. 14 ISMS, UIUC, June 19, 2014 VA-BROC Shift mask position to drive P(1). 15 ISMS, UIUC, June 19, 2014 Results and Discussion
VA-BROC (blue triangles) results. 16 ISMS, UIUC, June 19, 2014 Results and Discussion in N = 0. in N = 1. . VA-BROC (blue triangles) results. Toy Monte Carlo method used for statistical analysis. 17
ISMS, UIUC, June 19, 2014 Results and Discussion =140 ( 20 ) ms VA-BROC timing results. 127 ms expected from theory. 18 ISMS, UIUC, June 19, 2014 Summary BROC: Broadband Rotational Optical Cooling. Rotationally cooled AlH+ to ground state of each parity.
< 13 (< 19) K for the positive (negative) parity. VA-BROC: Vibrationally-Assisted Broadband Rotational Optical Cooling. Rotationally cooled AlH+ to single-parity ground state. N = 0 population increase from to . to in 140(20) ms. Cooling technique applicable to molecules separated P-branches with diagonal vibrational decays. Complex masks, broadband vibrational repumps extend technique to larger class of molecules. 19 ISMS, UIUC, June 19, 2014
Next Steps and Outlook More reliable/faster AlH+ production via REMPI. Currently exploring AlH & AlH3 UHV-compatible chemistry. Expertise/advice is greatly needed! Improve single-parity preparation from 100 ms to s via 10 electronic excitation-relaxations.s. 2-photon A21/2 X2+ excitation via (1+1) or (1+1) process. Laser sources commercially available. Hyperfine state cooling as preliminary to full molecular coherent control. Positioned to perform first molecular spectroscopy in the Lamb-Dicke regime. 20
ISMS, UIUC, June 19, 2014 Grad Students and Postdocs The Odom Group Michael Schmitt Matthew Dietrich (postdoc) Mark Kokish Chien-Yu Lien Yen-Wei Lin Chris Seck
Patrick Stollenwerk Ming-Feng Tu Undergrads Xiaowen Chen Group Alumni and The People Paying for It Joan Marler (postdoc) Jason Nguyen (postdoc) Vaishnavi Rajagopal (grad) David Tabor (grad) Marc Bourgeois (ugrad)
Fillan Grady (ugrad) Scott Williams (ugrad) Additional details: (1+1) REMPD: arXiv:1402:0123 Rotational cooling: arXiv:1402.3918 21 ISMS, UIUC, June 19, 2014 BROC & VA-BROC Timescales Parity-preserving BROC timescale via simulation at 1% of Isat. Parity-cooling VA-BROC timescale via v = 1 lifetime.
22 ISMS, UIUC, June 19, 2014 Toy Monte Carlo Method 1.3 n-tuple array generated by binomial random number generation using experimental ion numbers. Avoids binomial confidence intervals far from central limit approximation. 23 ISMS, UIUC, June 19, 2014
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