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Detecting the internal state of polar molecules is a substantial challenge when standard techniques such as resonance-enhanced multi photon ionization (REMPI) or laser-induced fluorescense (LIF) do not work. As this is the case for most…

Atomic Physics · Physics 2014-12-01 Rosa Glöckner , Alexander Prehn , Gerhard Rempe , Martin Zeppenfeld

We demonstrate a novel single molecule technique that is compatible with high precision measurements and obtain the spectrum of two molecular ion species. While the current result yields modest spectral resolution due to a broad light…

We present theoretical and experimental progress towards a new approach for the precision spectroscopy, coherent manipulation and state-to-state chemistry of single isolated molecular ions in the gas phase. Our method consists of a…

Quantum Physics · Physics 2019-09-24 Ziv Meir , Gregor Hegi , Kaveh Najafian , Mudit Sinhal , Stefan Willitsch

We use quantum-logic spectroscopy (QLS) and interrogate rotational transitions of a single CaH+ ion with a highly coherent frequency comb, achieving a fractional statistical uncertainty for a transition line center of 4 x 10^-13. We also…

We propose a method to investigate the vibrational dynamics of single polyatomic molecular ions confined in a Paul trap. Quantum logic techniques are employed to detect the recoil of single photon absorption events in the molecule via a…

Quantum Physics · Physics 2019-08-27 Philipp Schindler

Recent advancements in infrared frequency combs will enable recording of coherent two-dimensional infrared spectra of gas-phase molecules with rotational resolution (RR2DIR). We describe how RR2DIR spectra can be controlled with…

Optics · Physics 2024-01-23 Grzegorz Kowzan , Thomas K. Allison

We demonstrate a new spectroscopic method for studying electronic transitions in molecules with extremely broad range of angular momentum. We employ an optical centrifuge to create narrow rotational wave packets in the ground electronic…

Chemical Physics · Physics 2017-09-13 Aleksey Korobenko , Alexander A. Milner , John W. Hepburn , Valery Milner

Spectroscopy is a powerful tool for studying molecules and is commonly performed on large thermal molecular ensembles that are perturbed by motional shifts and interactions with the environment and one another, resulting in convoluted…

Absorption spectroscopy is a fundamental tool for probing molecular structure. However, performing absorption spectroscopy on individual molecules is challenging due to the low signal-to-noise ratio. Here, we report on a nondestructive…

We reflect on the prospect of exploiting the recoil associated with absorption and emission of photons to perform spectroscopy of a single molecular ion. For this recoil to be detectable, the molecular ion is sympathetically cooled by a…

Sympathetic cooling of trapped ions has been established as a powerful technique for manipulation of non-laser-coolable ions (Raizen1992,Waki1992,Bowe1999,Barrett2003). For molecular ions, it promises vastly enhanced spectroscopic…

Quantum Physics · Physics 2018-06-06 Soroosh Alighanbari , Michael Georg Hansen , Vladimir Korobov , Stephan Schiller

The rich information content of measurements in the molecular frame rather than the laboratory frame has motivated the development of several methods for aligning gas phase molecules in space. Even so, for asymmetric tops the problem of…

Atomic Physics · Physics 2016-11-23 Varun Makhija , Xiaoming Ren , Drue Gockel , Anh-Thu Le , Vinod Kumarappan

First results are presented obtained with an experimental setup developed to record IR spectra of rotationally state-selected ions. The method we use is a state-selective version of a method developed by S. Schlemmer, D. Gerlich and…

Chemical Physics · Physics 2017-05-03 Ugo Jacovella , Josef A. Agner , Hansjürg Schmutz , Johannes Deiglmayr , Frédéric Merkt

The rovibrational spectrum of the molecular ion H$_2$CCCH$^+$ was investigated in a 4~K cryogenic ion trap instrument employing the leak-out spectroscopy method. Transitions within the fundamental $\nu_1$ (C-H stretch) and the combination…

Calculation of the rotation-vibration spectrum of H3+, as well as of its deuterated isotopologues, with near-spectroscopic accuracy requires the development of sophisticated theoretical models, methods, and codes. The present paper reviews…

We describe a high-resolution spectroscopy method, in which the detection of single excitation events is enhanced by a complete loss of coherence of a superposition of two ground states. Thereby, transitions of a single isolated atom nearly…

Atomic Physics · Physics 2014-03-25 Govinda Clos , Martin Enderlein , Ulrich Warring , Dietrich Leibfried , Tobias Schaetz

We propose an approach for studying quantum information and performing high resolution spectroscopy of rotational states of trapped molecular ions using an on-chip superconducting microwave resonator. Molecular ions have several advantages…

Mesoscale and Nanoscale Physics · Physics 2011-05-24 D. I. Schuster , Lev S. Bishop , I. L. Chuang , D. DeMille , R. J. Schoelkopf

Two-dimensional infrared (2DIR) spectroscopy is widely used to study molecular dynamics but it is typically restricted to solid and liquid phase samples and modest spectral resolution. Only recently, its potential to study gas-phase…

Optics · Physics 2022-11-01 Grzegorz Kowzan , Thomas K. Allison

When circularly polarized light is scattered from a rotating target, a rotational Doppler shift (RDS) emerges from an exchange of angular momentum between the spinning object and the electromagnetic field. Here, we used coherently spinning…

Infrared reflection absorption spectroscopy (IRAS) offers a powerful route to bridging the materials and pressure gaps between surface science and powder catalysis. Using a newly developed IRAS setup optimised for dielectric single…

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