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arXiv:2405.00968 · Scientific Reports

A multidimensional approach to quantum state tomography of photoelectron wavepackets

Hugo Laurell, Jorge Baños-Gutiérrez, Anne L’Huillier, David Busto, Daniel Finkelstein‐Shapiro

Published Jan 31, 2025• 0 citations
arXivHTMLPDF

Abstract

There is a growing interest in reconstructing the density matrix of photoelectron wavepackets, in particular in complex systems where decoherence can be introduced either by a partial measurement of the system or through coupling with a stochastic environment. To this end, several methods to reconstruct the density matrix, quantum state tomography protocols, have been developed and tested on photoelectrons ejected from noble gases following absorption of extreme ultraviolet (XUV) photons from attosecond pulses. It remains a challenge to obtain model-free, single scan protocols that can reconstruct the density matrix with high fidelities. Current methods require extensive measurements or involve complex fitting of the signal. Efficient single-scan reconstructions would be of great help to increase the number of systems that can be studied. We propose a new and more efficient protocol that is able to reconstruct the continuous variable density matrix of a photoelectron in a single time delay scan. It is based on measuring the coherences of a photoelectron created by absorption of an XUV pulse using a broadband infrared (IR) probe that is scanned in time and a narrowband IR reference that is temporally fixed to the XUV pulse. We illustrate its performance for a Fano resonance in He as well as mixed states in Ar arising from spin-orbit splitting. We show that the protocol results in excellent fidelities and near-perfect estimation of the purity.

DOI
10.1038/s41598-025-86701-9

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There is a growing interest in reconstructing the density matrix of photoelectron wavepackets, in particular in complex systems where decoherence can be introduced either by a partial measurement of the system or through coupling with a stochastic environment. To this end, several methods to reconstruct the density matrix, quantum state tomography protocols, have been developed and tested on photoelectrons ejected from noble gases following absorption of extreme ultraviolet (XUV) photons from attosecond pulses. It remains a challenge to obtain model-free, single scan protocols that can reconstruct the density matrix with high fidelities. Current methods require extensive measurements or involve complex fitting of the signal. Efficient single-scan reconstructions would be of great help to increase the number of systems that can be studied. We propose a new and more efficient protocol that is able to reconstruct the continuous variable density matrix of a photoelectron in a single time delay scan. It is based on measuring the coherences of a photoelectron created by absorption of an XUV pulse using a broadband infrared (IR) probe that is scanned in time and a narrowband IR reference that is temporally fixed to the XUV pulse. We illustrate its performance for a Fano resonance in He as well as mixed states in Ar arising from spin-orbit splitting. We show that the protocol results in excellent fidelities and near-perfect estimation of the purity.
We propose a continuous variable quantum state tomography protocol of electrons which result from the ionization of atoms or molecules by the absorption of extreme ultraviolet light pulses. Our protocol is benchmarked against a direct calculation of the quantum state of photoelectrons ejected from helium and argon in the vicinity of a Fano resonance. In the latter case, we furthermore distill ion-photoelectron entanglement due to spin-orbit splitting. This opens routes toward the investigation of quantum coherence and entanglement properties on the ultrafast timescale.
Laser-dressed photoemission spectroscopy has established itself as the gold standard of attosecond temporal metrology.In this technique, the attosecond structure of an extreme-ultraviolet pulse is retrieved from the wave function of the electron wave packet released during photoionization.Here, we show that this electron wave packet should rather be described using the density matrix formalism, thus allowing one to account for all processes that can affect its coherence, from the attosecond pulse generation to the photoemission and the measurement processes.Using this approach, we reconstruct experimentally a partially coherent electron wave packet with a purity of 0.11 (1 for full coherence).Comparison with theoretical models then allows us to identify the origins of this decoherence and to overcome several limitations such as beam-line instabilities or spectrometer resolution.Furthermore, we show numerically how this method gives access to the coherence and eigencomponents of complex photoelectron wave packets.It thus goes beyond the current measurement of photoionization time delays and provides a general framework for the analysis and understanding of complex photoemission processes.
Abstract A photoelectron, emitted due to the absorption of light quanta as described by the photoelectric effect, is often characterized experimentally by a classical quantity, its momentum. However, since the photoelectron is a quantum object, its rigorous characterization requires the reconstruction of the complete quantum state, the photoelectron’s density matrix. Here we use quantum-state tomography to fully characterize photoelectrons emitted from helium and argon atoms upon absorption of ultrashort, extreme ultraviolet light pulses. While in helium we measure a pure photoelectronic state, in argon, spin–orbit interaction induces entanglement between the ion and the photoelectron, leading to a reduced purity of the photoelectron state. Our work shows how state tomography gives new insights into the fundamental quantum aspects of light-induced electronic processes in matter, bridging the fields of photoelectron spectroscopy and quantum information and offering new spectroscopic possibilities for quantum technology.
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.
The reconstruction of density matrices from measurement data (quantum state tomography) is the most comprehensive method for assessing the accuracy and performance of quantum devices. Existing methods to reconstruct two-photon density matrices require the detection of both photons unless a priori information is available. Based on the concept of quantum-induced coherence by path identity, we present an approach to quantum state tomography that circumvents the requirement of detecting both photons. We show that an arbitrary two-qubit density matrix, which can contain up to fifteen free parameters, can be fully reconstructed from single-photon measurement data without any postselection and a priori information. In addition to advancing an alternative approach to quantum state measurement problems, our results also have notable practical implications. A practical challenge in quantum state measurement arises from the fact that effective single-photon detectors are not readily accessible for a wide spectral range. Our method, which eliminates the need for coincidence measurements, enables quantum state tomography in the case where one of the two photons is challenging or impossible to detect. It therefore opens the door to measuring quantum states hitherto inaccessible.
Quantum state tomography is a fundamental tool in quantum information processing. It allows us to estimate the state of a quantum system by measuring different observables on many identically prepared copies of the system. This is, in general, a very time-consuming task that requires a large number of measurements. There are, however, systems in which the data acquisition can be done more efficiently. In fact, an ensemble of quantum systems can be prepared and manipulated by external fields while being continuously and collectively probed, producing enough information to estimate its state. This provides a basis for continuous measurement quantum tomography. In this protocol, an ensemble of identically prepared systems is collectively probed and controlled in a time-dependent manner to create an informationally complete continuous measurement record. The measurement history is then inverted to determine the state at the initial time. We use two different estimation methods: maximum likelihood and compressed sensing. The general formalism is applied to the case of reconstruction of the quantum state encoded in the magnetic sub-levels of a large-spin alkali atom, 133{}^{133}133Cs. We apply this protocol to the case of reconstruction of states in the full 16-dimensional electronic-ground subspace (F=3⊕F=4F=3 \oplus F=4F=3⊕F=4), controlled by microwaves and radio-frequency magnetic fields. We present an experimental demonstration of continuous measurement quantum tomography in an ensemble of cold cesium atoms with full control of its 16-dimensional Hilbert space. We show the exquisite level of control achieved in the lab and the excellent agreement between the theory discussed in this dissertation and the experimental results. This allows us to achieve fidelities >95% for low complexity quantum states, and >92% for arbitrary random states, which is a formidable accomplishment for a space of this size.