aqora

Ultrafast infrared spectroscopy with single molecular ions

Philipp Schindler

Abstract 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 on the molecule via a co-trapped atomic ion. In particular, the recoil is mapped onto the electronic state of the atom which can be read out with high fidelity. This recoil detection serves as the basis for a pump-probe scheme to investigate ultrafast molecular dynamics, such as intra-molecular vibrational redistribution. The total recoil from the interaction with a sequence of ultrafast laser pulses with the molecular vibration is measured. This work discusses the experimental requirements and expected performance for multiple molecular ions with masses ranging from 17 to 165 Dalton.Abstract 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 on the molecule via a co-trapped atomic ion. In particular, the recoil is mapped onto the electronic state of the atom which can be read out with high fidelity. This recoil detection serves as the basis for a pump-probe scheme to investigate ultrafast molecular dynamics, such as intra-molecular vibrational redistribution. The total recoil from the interaction with a sequence of ultrafast laser pulses with the molecular vibration is measured. This work discusses the experimental requirements and expected performance for multiple molecular ions with masses ranging from 17 to 165 Dalton.

arXiv:1809.06776New Journal of PhysicsJul 25, 20193 citations

Single-photon detection and its applications

Yan Liang, Heping Zeng

Science China Physics Mechanics and AstronomyApr 15, 201434 citations

Single-atom photon recoil momentum

Phillip F. Schewe

Physics TodayJul 1, 20050 citations

Infrared absorption spectroscopy of a single polyatomic molecular ion

Zhenlin Wu, Tim Duka, Mariano Isaza-Monsalve +8 more

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 absorption spectroscopy on a mid-infrared vibrational transition in a single molecular ion that is co-trapped with an atomic ion. The absorption of a single photon is detected via the momentum transfer from the absorbed photon onto the molecule. This recoil signal is amplified using a non-classical state of motion of the two-ion crystal and subsequently read out via the atomic ion. We characterize the recoil detection method and use it to investigate the interaction between femtosecond laser pulses and the O-H stretching vibration in individual CaOH+ molecular ions. Furthermore, we present the single-photon absorption spectrum obtained for the vibrational transition. This method represents a milestone towards quantum non-demolition measurements of complex polyatomic molecules, providing high-fidelity methods for preparation and measurement of the quantum state of a wide range of molecular species.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 absorption spectroscopy on a mid-infrared vibrational transition in a single molecular ion that is co-trapped with an atomic ion. The absorption of a single photon is detected via the momentum transfer from the absorbed photon onto the molecule. This recoil signal is amplified using a non-classical state of motion of the two-ion crystal and subsequently read out via the atomic ion. We characterize the recoil detection method and use it to investigate the interaction between femtosecond laser pulses and the O-H stretching vibration in individual CaOH+ molecular ions. Furthermore, we present the single-photon absorption spectrum obtained for the vibrational transition. This method represents a milestone towards quantum non-demolition measurements of complex polyatomic molecules, providing high-fidelity methods for preparation and measurement of the quantum state of a wide range of molecular species.

quant-pharXiv:2511.19687NatureNov 26, 20250 citations

Photon Antibunching In The Fluorescence Of A Single Dye Molecule Trapped In A Solid

Th. Basché, W. E. Moerner, Michel Orrit +1 more

The ability to store single atomic ions in a radio-frequency trap by photon-recoil cooling and detect the emitted fluorescence of the single trapped ions has proven to be a successful way to investigate the fundamental interaction of light and matter and to test our understanding of quantum physics1,2. The extension of these studies to molecules has failed so far, because all molecules - even diatomic species - possess several internal degrees of freedom which prevent laser cooling.

Spectral Hole-Burning and Related Spectroscopies: Science and ApplicationsJan 1, 19920 citations

Smart Strategies for Single-Photon Detection

João Batista Rosa Silva, Rubens Viana Ramos, Elvio César Giraudo

Lecture notes in computer scienceJan 1, 20040 citations

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