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We demonstrate optical cycling and sub-Doppler laser cooling of a cryogenic buffer-gas beam of calcium monohydride (CaH) molecules. We measure vibrational branching ratios for laser cooling transitions for both excited electronic states A…

Atomic Physics · Physics 2022-08-24 S. F. Vázquez-Carson , Q. Sun , J. Dai , D. Mitra , T. Zelevinsky

A special class of molecules that are important to many subfields in molecular dynamics and chemical physics, namely free radical molecules, now enjoy a significant degree of center-of-mass motion control in the laboratory frame. The…

Atomic Physics · Physics 2009-11-10 J. R. Bochinski , Eric R. Hudson , H. J. Lewandowski , Jun Ye

Molecular overtone transitions provide optical frequency transitions sensitive to variation in the proton-to-electron mass ratio ($\mu\equiv m_p/m_e$). However, robust molecular state preparation presents a challenge critical for achieving…

Ultrashort laser pulses are widely used for transient field-free molecular orientation -- a phenomenon important in chemical reaction dynamics, ultrafast molecular imaging, high harmonics generation, and attosecond science. However,…

Chemical Physics · Physics 2022-12-21 Ilia Tutunnikov , Long Xu , Yehiam Prior , Ilya Sh. Averbukh

We propose a laser cooling technique in which atoms are selectively excited to a dressed metastable state whose light shift and decay rate are spatially correlated for Sisyphus cooling. The case of cooling magnetically trapped…

Atomic Physics · Physics 2015-03-17 Saijun Wu , Roger C. Brown , William D. Phillips , J. V. Porto

A novel polarization-modulation transient method has been developed for studying fast anisotropic relaxation in electronic excited states of polyatomic and biologically relevant molecules under excitation with femtosecond laser pulses. The…

Chemical Physics · Physics 2020-05-12 Ioanna Gorbunova , Nikolay Bezverkhnii , Maxim Sasin , Idris Gagzhiev , Oleg Vasyutinskii

Short laser pulses are widely used for controlling molecular rotational degrees of freedom and inducing molecular alignment, orientation, unidirectional rotation and other types of coherent rotational motion. To follow the ultra-fast…

We introduce a scheme for deep laser cooling of molecules based on robust dark states at zero velocity. By simulating this scheme, we show it to be a widely applicable method that can reach the recoil limit or below. We demonstrate and…

Atomic Physics · Physics 2019-07-24 L. Caldwell , J. A. Devlin , H. J. Williams , N. J. Fitch , E. A. Hinds , B. E. Sauer , M. R. Tarbutt

Optomechanical cavities in the well-resolved-sideband regime are ideally suited for the study of a myriad of quantum phenomena with mechanical systems, including backaction-evading measurements, mechanical squeezing, and generation of…

Quantum Physics · Physics 2020-05-06 Liu Qiu , Itay Shomroni , Paul Seidler , Tobias J. Kippenberg

Cooling of molecules via free-space dissipative scattering of photons is thought not to be practicable due to the inherently large number of Raman loss channels available to molecules and the prohibitive expense of building multiple…

The translational motion of molecular ions can be effectively cooled sympathetically to translational temperatures below 100 mK in ion traps through Coulomb interactions with laser-cooled atomic ions. The ro-vibrational degrees of freedom,…

Atomic Physics · Physics 2009-11-10 I. S. Vogelius , L. B. Madsen , M. Drewsen

We investigate pump-dump photoassociation of ultracold molecules with amplitude- and phase-modulated femtosecond laser pulses. For this purpose a perturbative model for the light-matter interaction is developed and combined with a genetic…

It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields. Unfortunately laser cooling has not yet been extended to molecules because of their complex…

Atomic Physics · Physics 2015-05-27 E. S. Shuman , J. F. Barry , D. DeMille

We demonstrate experimentally a method of all-optical selective rotational control in gas mixtures. Using an optical centrifuge - an intense laser pulse whose linear polarization rotates at an accelerated rate, we simultaneously excite two…

Chemical Physics · Physics 2024-06-19 P. Amani , A. A. Milner , V. Milner

We demonstrate strong adiabatic laser alignment and mixed-field orientation at kHz repetition rates. We observe degrees of alignment as large as cos\Theta=0.94 at 1 kHz operation for iodobenzene. The experimental setup consist of a kHz…

We demonstrate rotational cooling of the silicon monoxide cation via optical pumping by a spectrally filtered broadband laser. Compared with diatomic hydrides, SiO\+ is more challenging to cool because of its smaller rotational interval.…

We present a rigorous study of vibrational relaxation in p-H2 + p-H2 collisions at cold and ultracold temperatures and identify an efficient mechanism of ro-vibrational energy transfer. If the colliding molecules are in different rotational…

Quantum Physics · Physics 2008-04-02 Goulven Quéméner , Naduvalath Balakrishnan , Roman V. Krems

In this work we demonstrate vibrational spectroscopy of polyatomic ions that are trapped and sympathetically cooled by laser-cooled atomic ions. We use the protonated dipeptide tryptophane-alanine (HTyrAla+) as a model system, cooled by…

Chemical Physics · Physics 2017-09-13 Ch. Wellers , A. Borodin , S. Vasilyev , D. Offenberg , S. Schiller

We present a novel method for probing the alignment of the molecular axis of an ultracold, nonpolar dimer. These results are obtained using diatomic $^{87}\textrm{Rb}_2$ molecules in the vibrational ground state of the lowest triplet…

Atomic Physics · Physics 2015-01-15 Markus Deiß , Björn Drews , Benjamin Deissler , Johannes Hecker Denschlag

We present state-selected measurements of rotational cooling and excitation rates of CH$^+$ molecular ions by inelastic electron collisions. The experiments are carried out at the Cryogenic Storage Ring, making use of a monoenergetic…