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

The Journal of Chemical Physics

Quantum tomography of a molecular bond in ice

I. U. Goldschleger, Marie N. van Staveren, Vartkess Ara Apkarian

Published Jul 17, 2013• 10 citations
Publisher

Abstract

We present the moving picture of a molecular bond, in phase-space, in real-time, at resolution limited by quantum uncertainty. The images are tomographically reconstructed Wigner distribution functions (WDF) obtained from four-wave mixing measurements on Br2-doped ice. The WDF completely characterizes the dissipative quantum evolution of the system, which despite coupling to the environment retains quantum coherence, as evidenced by its persistent negative Wigner hole. The spectral decomposition of the WDF allows a direct visualization of wavefunctions and spatiotemporal coherences of the system and the system-bath interaction. The measurements vividly illustrate nonclassical wave mechanics in a many-body system, in ordinary condensed matter.

DOI
10.1063/1.4813437

Related papers

Tomographic imaging of complete quantum state of matter by ultrafast diffraction

Ming Zhang, Shuqiao Zhang, Haitan Xu +6 more

With the ability to directly obtain the Wigner function and density matrix of photon states, quantum tomography (QT) has had a significant impact on quantum optics, quantum computing and quantum information. By an appropriate sequence of measurements on the evolution of each degreeof freedom (DOF), the full quantum state of the observed photonic system can be determined. The first proposal to extend the application of QT to reconstruction of complete quantum states of matter wavepackets had generated enormous interest in ultrafast diffraction imaging and pump-probe spectroscopy of molecules. This interest was elevated with the advent of ultrafast electron and X-ray diffraction techniques using electron accelerators and X-ray free electron lasers to add temporal resolution to the observed nuclear and electron distributions. However, the great interest in this area has been tempered by the illustration of an impossibility theorem, known as the dimension problem. Not being able to associate unitary evolution to every DOF of molecular motion, quantum tomography could not be used beyond 1D and categorically excludes most vibrational and all rotational motion of molecules. Here we present a theoretical advance to overcome the notorious dimension problem. Solving this challenging problem is important to push imaging molecular dynamics to the quantum limit. The new theory has solved this problem, which makes quantum tomography a truly useful methodology in ultrafast physics and enables the making of quantum version of a molecular movie. With the new theory, quantum tomography can be finally advanced to a sufficient level to become a general method for reconstructing quantum states of matter, without being limited in one dimension. Our new concept is demonstrated using a simulated dataset of ultrafast diffraction experiment of laser-aligned nitrogen molecules.

arXiv:2012.11899•Dec 22, 2020•1 citation

Dissipative quantum coherent dynamics probed in phase-space: Electronically resonant 5-color 4-wave mixing on I2(B) in solid Kr

D. Segale, Vartkess Ara Apkarian

Spectrally resolved, 4-wave mixing measurements in five resonant colors are used to interrogate vibronic quantum coherences in phase-space. We highlight the principles through measurements on the B-state of I(2) in solid Kr--a prototype of a system strongly coupled to its environment. The measurements consist of preparing a superposition of wavepackets on the B-state and interrogating their cross-coherence as they get entangled with the environment. The study provides direct realizations of fundamental quantum principles in the mechanics of molecular matter, among them: the distinction between quantum and classical coherent dynamics of a system entangled with the environment, coherent dissipation, event-driven decoherence, environment selected coherent states, and non-local mechanics.

The Journal of Chemical Physics•Jul 8, 2011•17 citations

Phase space tomography of classical and nonclassical vibrational states of atoms in an optical lattice

J. F. Kanem, Samansa Maneshi, Stefan H. Myrskog +1 more

Atoms trapped in an optical lattice have long been a system of interest in the atomic, molecular and optical community, and in recent years much study has been devoted to both short- and long-range coherence in this system, as well as to its possible applications to quantum information processing. Here we demonstrate for the first time a complete determination of the quantum phase space distributions for an ensemble of 85 Rb atoms in such a lattice, including a negative Wigner function for atoms in an inverted state.

arXiv:quant-ph/0506140•Journal of Optics B Quantum and Semiclassical Optics•Nov 22, 2005•14 citations

Quantum Tomography of Solitary Electrons

J. D. Fletcher, Nathan Johnson, Elina Locane +7 more

Initializing and measuring the wave-function of single freely-propagating particles are challenging but fundamental tasks for applications in quantum information processing and enhanced sensing. Recently, continuous-variable quantum tomography techniques developed for atomic beams and photonic modes have been adapted for on-demand electronic excitations but are limited to the region in energy-time phase space immediately around the Fermi level. Here we present a general, broad-band method for mapping the single-particle phase space Wigner distribution. We reconstruct the Wigner representation of the mixed-state density matrix for \textit{solitary} electrons emitted by an on-demand source. This reveals highly localised distributions isolated from the Fermi sea. Our method can be used to test the degree of `quantumness' of an electron source from measurements of the phase-space density. While both source purity and detector fidelity are suppressed by classical fluctuations, here we resolve fine structure of the wavepackets (a chirp controlled by emission conditions) and find that the resolution should be sufficient to enable quantum-limited measurements. Our technique will provide key information required to master electron coherence and entanglement at the individual particle level, for instance to create excitations from multiple sources that are indistinguishable.

•Jan 30, 2019•4 citations

Time-of-Flight Quantum Tomography of Single Atom Motion

M. O. Brown, S. R. Muleady, Willa J. Arthur-Dworschack +4 more

Time of flight is an intuitive way to determine the velocity of particles and lies at the heart of many capabilities ranging from mass spectrometry to fluid flow measurements. Here we show time-of-flight imaging can realize tomography of a quantum state of motion of a single trapped atom. Tomography of motion requires studying the phase space spanned by both position and momentum. By combining time-of-flight imaging with coherent evolution of the atom in an optical tweezer trap, we are able to access arbitrary quadratures in phase space without relying on coupling to a spin degree of freedom. To create non-classical motional states, we harness quantum tunneling in the versatile potential landscape of optical tweezers, and our tomography both demonstrates Wigner function negativity and assesses coherence of non-stationary states. Our demonstrated tomography concept has wide applicability to a range of particles and will enable characterization of non-classical states of more complex systems or massive dielectric particles.

arXiv:2203.03053•Mar 6, 2022•2 citations

Quantum phase estimation for nondestructive monitoring and Wigner tomography of bosonic fields

Lucas R. S. Santos, Ciro M. Diniz, Daniel Z. Rossatto +1 more

Quantum phase estimation is usually introduced as an algorithmic primitive for extracting eigenphases of unitary operators. Here we show that, when implemented through a dispersive light-matter interaction, it can also be used as a nondestructive measurement tool for bosonic fields. We consider a bosonic mode coupled to a multi-qubit register and calibrate the photon-number dependent phase shifts so that the register performs a number-resolved quantum phase estimation readout. Repeating this readout during dissipative evolution enables nondestructive monitoring of photon-number dynamics. We then show that the same readout can be converted into a Wigner tomography reconstruction by applying phase-space displacements before the quantum phase estimation block. Numerical reconstructions for Fock, coherent, and even/odd Schrödinger cat states show the expected nonclassical phase-space structures and near-unity Wigner overlap fidelities. The protocol provides a unified route to nondestructive monitoring and state tomography of bosonic fields, with direct relevance for bosonic-state characterization, calibration, and control in superconducting quantum architectures.

quant-pharXiv:2608.20787•Aug 24, 2026•0 citations
We present the moving picture of a molecular bond, in phase-space, in real-time, at resolution limited by quantum uncertainty. The images are tomographically reconstructed Wigner distribution functions (WDF) obtained from four-wave mixing measurements on Br2-doped ice. The WDF completely characterizes the dissipative quantum evolution of the system, which despite coupling to the environment retains quantum coherence, as evidenced by its persistent negative Wigner hole. The spectral decomposition of the WDF allows a direct visualization of wavefunctions and spatiotemporal coherences of the system and the system-bath interaction. The measurements vividly illustrate nonclassical wave mechanics in a many-body system, in ordinary condensed matter.
With the ability to directly obtain the Wigner function and density matrix of photon states, quantum tomography (QT) has had a significant impact on quantum optics, quantum computing and quantum information. By an appropriate sequence of measurements on the evolution of each degreeof freedom (DOF), the full quantum state of the observed photonic system can be determined. The first proposal to extend the application of QT to reconstruction of complete quantum states of matter wavepackets had generated enormous interest in ultrafast diffraction imaging and pump-probe spectroscopy of molecules. This interest was elevated with the advent of ultrafast electron and X-ray diffraction techniques using electron accelerators and X-ray free electron lasers to add temporal resolution to the observed nuclear and electron distributions. However, the great interest in this area has been tempered by the illustration of an impossibility theorem, known as the dimension problem. Not being able to associate unitary evolution to every DOF of molecular motion, quantum tomography could not be used beyond 1D and categorically excludes most vibrational and all rotational motion of molecules. Here we present a theoretical advance to overcome the notorious dimension problem. Solving this challenging problem is important to push imaging molecular dynamics to the quantum limit. The new theory has solved this problem, which makes quantum tomography a truly useful methodology in ultrafast physics and enables the making of quantum version of a molecular movie. With the new theory, quantum tomography can be finally advanced to a sufficient level to become a general method for reconstructing quantum states of matter, without being limited in one dimension. Our new concept is demonstrated using a simulated dataset of ultrafast diffraction experiment of laser-aligned nitrogen molecules.
Spectrally resolved, 4-wave mixing measurements in five resonant colors are used to interrogate vibronic quantum coherences in phase-space. We highlight the principles through measurements on the B-state of I(2) in solid Kr--a prototype of a system strongly coupled to its environment. The measurements consist of preparing a superposition of wavepackets on the B-state and interrogating their cross-coherence as they get entangled with the environment. The study provides direct realizations of fundamental quantum principles in the mechanics of molecular matter, among them: the distinction between quantum and classical coherent dynamics of a system entangled with the environment, coherent dissipation, event-driven decoherence, environment selected coherent states, and non-local mechanics.
Atoms trapped in an optical lattice have long been a system of interest in the atomic, molecular and optical community, and in recent years much study has been devoted to both short- and long-range coherence in this system, as well as to its possible applications to quantum information processing. Here we demonstrate for the first time a complete determination of the quantum phase space distributions for an ensemble of 85 Rb atoms in such a lattice, including a negative Wigner function for atoms in an inverted state.
Initializing and measuring the wave-function of single freely-propagating particles are challenging but fundamental tasks for applications in quantum information processing and enhanced sensing. Recently, continuous-variable quantum tomography techniques developed for atomic beams and photonic modes have been adapted for on-demand electronic excitations but are limited to the region in energy-time phase space immediately around the Fermi level. Here we present a general, broad-band method for mapping the single-particle phase space Wigner distribution. We reconstruct the Wigner representation of the mixed-state density matrix for \textit{solitary} electrons emitted by an on-demand source. This reveals highly localised distributions isolated from the Fermi sea. Our method can be used to test the degree of `quantumness' of an electron source from measurements of the phase-space density. While both source purity and detector fidelity are suppressed by classical fluctuations, here we resolve fine structure of the wavepackets (a chirp controlled by emission conditions) and find that the resolution should be sufficient to enable quantum-limited measurements. Our technique will provide key information required to master electron coherence and entanglement at the individual particle level, for instance to create excitations from multiple sources that are indistinguishable.
Time of flight is an intuitive way to determine the velocity of particles and lies at the heart of many capabilities ranging from mass spectrometry to fluid flow measurements. Here we show time-of-flight imaging can realize tomography of a quantum state of motion of a single trapped atom. Tomography of motion requires studying the phase space spanned by both position and momentum. By combining time-of-flight imaging with coherent evolution of the atom in an optical tweezer trap, we are able to access arbitrary quadratures in phase space without relying on coupling to a spin degree of freedom. To create non-classical motional states, we harness quantum tunneling in the versatile potential landscape of optical tweezers, and our tomography both demonstrates Wigner function negativity and assesses coherence of non-stationary states. Our demonstrated tomography concept has wide applicability to a range of particles and will enable characterization of non-classical states of more complex systems or massive dielectric particles.
Quantum phase estimation is usually introduced as an algorithmic primitive for extracting eigenphases of unitary operators. Here we show that, when implemented through a dispersive light-matter interaction, it can also be used as a nondestructive measurement tool for bosonic fields. We consider a bosonic mode coupled to a multi-qubit register and calibrate the photon-number dependent phase shifts so that the register performs a number-resolved quantum phase estimation readout. Repeating this readout during dissipative evolution enables nondestructive monitoring of photon-number dynamics. We then show that the same readout can be converted into a Wigner tomography reconstruction by applying phase-space displacements before the quantum phase estimation block. Numerical reconstructions for Fock, coherent, and even/odd Schrödinger cat states show the expected nonclassical phase-space structures and near-unity Wigner overlap fidelities. The protocol provides a unified route to nondestructive monitoring and state tomography of bosonic fields, with direct relevance for bosonic-state characterization, calibration, and control in superconducting quantum architectures.