Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:1409.0904 · The Journal of Physical Chemistry Letters

Complete Quantum State Selectivity in Cold Molecular Beams Using Deflection-Resistant Dark States in a STIRAP Configuration

Xuan Li, A. Eilam, Moshe Shapiro

Published Oct 6, 2014• 0 citations
arXivHTMLPDF

Abstract

One of the main goals of chemical dynamics is the creation of molecular beams composed of a single (vibrational, rotational, and magnetic) quantum state of choice. In this Letter, we propose a method to achieve complete quantum state selectivity by producing resistance to electromagnetically induced deflection (EID) and that the state to be selected can be "dialed in" at will. We illustrate the method by showing in detail how to purify thermal beams of the LiRb and IF molecules to yield molecular beams composed of a variety of prechosen single internal quantum states and/or superpositions of such states. We expect that this method will be implemented in all subsequent explorations of the fundamentals of chemical reactions and their control and the use of cold molecules as a vehicle for studying some of the most profound issues of quantum dynamics.

DOI
10.1021/jz501852p

Related papers

Selecting molecules in the vibrational and rotational ground state by deflection

P. Domokos, Takanobu KISS, József Janszky

A beam of diatomic molecules scattered off a standing wave laser mode splits according to the rovibrational quantum state of the molecules. Our numerical calculation shows that single state resolution can be achieved by properly tuned, monochromatic light. The proposed scheme allows for selecting non-vibrating and non-rotating molecules from a thermal beam, implementing a laser Maxwell’s demon to prepare a rovibrationally cold molecular ensemble.

•Jan 1, 2000•5 citations

State selective manipulation of molecules: implementing Maxwell’s demon

Takanobu KISS

Light has proven to be a very useful means to influence the motion of atoms: to cool and to trap them. In molecules, however, there is usually a much richer variety of rotational and vibrational states. If they are thermally excited, the manipulation of an ensemble becomes difficult. We suggest that, in certain cases, non‐resonant interaction can achieve the addressing of single rovibrational levels. In our proposal a beam of diatomic molecules scattered off a standing wave laser mode splits according to the rovibrational quantum state of the molecules. We have found that single state resolution can be achieved by properly tuned, monochromatic light. The proposed scheme enables selecting non vibrating and non rotating molecules from a thermally excited beam. With this technique one could implement an instrument acting like Maxwell’s demon in order to prepare a rotationally and vibrationally cold molecular ensemble.

AIP conference proceedings•Jan 1, 2002•0 citations

State-selective coherent motional excitation as a new approach for the manipulation, spectroscopy and state-to-state chemistry of single molecular ions

Ziv Meir, Gregor Hegi, Kaveh Najafian +2 more

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 uses a molecular beam for creating packets of rotationally cold neutrals from which a single molecule is state-selectively ionized and trapped inside a radiofrequency ion trap. In addition to the molecular ion, a single co-trapped atomic ion is used to cool the molecular external degrees of freedom to the ground state of the trap and to detect the molecular state using state-selective coherent motional excitation from a modulated optical-dipole force acting on the molecule. We present a detailed discussion and theoretical characterization of the present approach. We simulate the molecular signal experimentally using a single atomic ion, indicating that different rovibronic molecular states can be resolved and individually detected with our method. The present approach for the coherent control and non-destructive detection of the quantum state of a single molecular ion opens up new perspectives for precision spectroscopies relevant for, e.g., tests of fundamental physical theories and the development of new types of clocks based on molecular vibrational transitions. It will also enable the observation and control of chemical reactions of single particles on the quantum level. While focusing on N2+ as a prototypical example in the present work, our method is applicable to a wide range of diatomic and polyatomic molecules.

arXiv:1909.10292•Faraday Discussions•Dec 11, 2018•17 citations

Manipulation of slow molecular beams by static external fields

Timothy J. McCarthy, Michaël T. Timko, Dudley R. Herschbach

Deflection by magnetic or electric field gradients has long been used to analyze or to alter the translational trajectories of neutral gas-phase atoms or molecules. Recent work has developed sources of slow, cold molecular beams that offer means to enhance markedly the attainable deflections, which are inversely proportional to the translational kinetic energy. The sensitivity and resolution can thus be much increased, typically by factors of 10(2)-10(4). We illustrate ways to exploit this enhanced deflection capability, particularly when balancing electric and magnetic deflections. Chemical scope can be greatly extended by utilizing feeble but ubiquitous interactions, especially the induced electric dipole due to the molecular polarizability and magnetic moments resulting from molecular rotation or nuclear spins. We also examine the effect of non-Maxwellian velocity distributions produced by supersonic expansions or by quantum statistics (pertinent for ultracold beams). Generic plots are provided, employing dimensionless variables, to facilitate the design and interpretation of experiments with deflections amplified by low kinetic energy.

The Journal of Chemical Physics•Oct 3, 2006•19 citations

Quantum-state selection, alignment, and orientation of large molecules using static electric and laser fields

Frank Filsinger, Jochen Küpper, Gerard Meijer +5 more

Supersonic beams of polar molecules are deflected using inhomogeneous electric fields. The quantum-state selectivity of the deflection is used to spatially separate molecules according to their quantum state. A detailed analysis of the deflection and the obtained quantum-state selection is presented. The rotational temperatures of the molecular beams are determined from the spatial beam profiles and are all approximately 1 K. Unprecedented degrees of laser-induced alignment (<cos2 theta2D>=0.972) and orientation of iodobenzene molecules are demonstrated when the state-selected samples are used. Such state-selected and oriented molecules provide unique possibilities for many novel experiments in chemistry and physics.

arXiv:0903.5413•The Journal of Chemical Physics•Aug 14, 2009•154 citations

Quantum-State Control and Manipulation of Paramagnetic Molecules with Magnetic Fields

Brianna R. Heazlewood

Since external magnetic fields were first employed to deflect paramagnetic atoms in 1921, a range of magnetic field-based methods have been introduced to state-selectively manipulate paramagnetic species. These methods include magnetic guides, which selectively filter paramagnetic species from all other components of a beam, and magnetic traps, where paramagnetic species can be spatially confined for extended periods of time. However, many of these techniques were developed for atomic-rather than molecular-paramagnetic species. It has proven challenging to apply some of these experimental methods developed for atoms to paramagnetic molecules. Thanks to the emergence of new experimental approaches and new combinations of existing techniques, the past decade has seen significant progress toward the manipulation and control of paramagnetic molecules. This review identifies the key methods that have been implemented for the state-selective manipulation of paramagnetic molecules-discussing the motivation, state of the art, and future prospects of the field. Key applications include the ability to control chemical interactions, undertake precise spectroscopic measurements, and challenge our understanding of chemical reactivity at a fundamental level.

Annual Review of Physical Chemistry•Jan 25, 2021•12 citations
One of the main goals of chemical dynamics is the creation of molecular beams composed of a single (vibrational, rotational, and magnetic) quantum state of choice. In this Letter, we propose a method to achieve complete quantum state selectivity by producing resistance to electromagnetically induced deflection (EID) and that the state to be selected can be "dialed in" at will. We illustrate the method by showing in detail how to purify thermal beams of the LiRb and IF molecules to yield molecular beams composed of a variety of prechosen single internal quantum states and/or superpositions of such states. We expect that this method will be implemented in all subsequent explorations of the fundamentals of chemical reactions and their control and the use of cold molecules as a vehicle for studying some of the most profound issues of quantum dynamics.
Light has proven to be a very useful means to influence the motion of atoms: to cool and to trap them. In molecules, however, there is usually a much richer variety of rotational and vibrational states. If they are thermally excited, the manipulation of an ensemble becomes difficult. We suggest that, in certain cases, non‐resonant interaction can achieve the addressing of single rovibrational levels. In our proposal a beam of diatomic molecules scattered off a standing wave laser mode splits according to the rovibrational quantum state of the molecules. We have found that single state resolution can be achieved by properly tuned, monochromatic light. The proposed scheme enables selecting non vibrating and non rotating molecules from a thermally excited beam. With this technique one could implement an instrument acting like Maxwell’s demon in order to prepare a rotationally and vibrationally cold molecular ensemble.
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 uses a molecular beam for creating packets of rotationally cold neutrals from which a single molecule is state-selectively ionized and trapped inside a radiofrequency ion trap. In addition to the molecular ion, a single co-trapped atomic ion is used to cool the molecular external degrees of freedom to the ground state of the trap and to detect the molecular state using state-selective coherent motional excitation from a modulated optical-dipole force acting on the molecule. We present a detailed discussion and theoretical characterization of the present approach. We simulate the molecular signal experimentally using a single atomic ion, indicating that different rovibronic molecular states can be resolved and individually detected with our method. The present approach for the coherent control and non-destructive detection of the quantum state of a single molecular ion opens up new perspectives for precision spectroscopies relevant for, e.g., tests of fundamental physical theories and the development of new types of clocks based on molecular vibrational transitions. It will also enable the observation and control of chemical reactions of single particles on the quantum level. While focusing on N2+ as a prototypical example in the present work, our method is applicable to a wide range of diatomic and polyatomic molecules.
Deflection by magnetic or electric field gradients has long been used to analyze or to alter the translational trajectories of neutral gas-phase atoms or molecules. Recent work has developed sources of slow, cold molecular beams that offer means to enhance markedly the attainable deflections, which are inversely proportional to the translational kinetic energy. The sensitivity and resolution can thus be much increased, typically by factors of 10(2)-10(4). We illustrate ways to exploit this enhanced deflection capability, particularly when balancing electric and magnetic deflections. Chemical scope can be greatly extended by utilizing feeble but ubiquitous interactions, especially the induced electric dipole due to the molecular polarizability and magnetic moments resulting from molecular rotation or nuclear spins. We also examine the effect of non-Maxwellian velocity distributions produced by supersonic expansions or by quantum statistics (pertinent for ultracold beams). Generic plots are provided, employing dimensionless variables, to facilitate the design and interpretation of experiments with deflections amplified by low kinetic energy.
Supersonic beams of polar molecules are deflected using inhomogeneous electric fields. The quantum-state selectivity of the deflection is used to spatially separate molecules according to their quantum state. A detailed analysis of the deflection and the obtained quantum-state selection is presented. The rotational temperatures of the molecular beams are determined from the spatial beam profiles and are all approximately 1 K. Unprecedented degrees of laser-induced alignment (<cos2 theta2D>=0.972) and orientation of iodobenzene molecules are demonstrated when the state-selected samples are used. Such state-selected and oriented molecules provide unique possibilities for many novel experiments in chemistry and physics.
Since external magnetic fields were first employed to deflect paramagnetic atoms in 1921, a range of magnetic field-based methods have been introduced to state-selectively manipulate paramagnetic species. These methods include magnetic guides, which selectively filter paramagnetic species from all other components of a beam, and magnetic traps, where paramagnetic species can be spatially confined for extended periods of time. However, many of these techniques were developed for atomic-rather than molecular-paramagnetic species. It has proven challenging to apply some of these experimental methods developed for atoms to paramagnetic molecules. Thanks to the emergence of new experimental approaches and new combinations of existing techniques, the past decade has seen significant progress toward the manipulation and control of paramagnetic molecules. This review identifies the key methods that have been implemented for the state-selective manipulation of paramagnetic molecules-discussing the motivation, state of the art, and future prospects of the field. Key applications include the ability to control chemical interactions, undertake precise spectroscopic measurements, and challenge our understanding of chemical reactivity at a fundamental level.