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First-order spatial coherence measurements in a thermalized two-dimensional photonic quantum gas.

ABSTRACT: Phase transitions between different states of matter can profoundly modify the order in physical systems, with the emergence of ferromagnetic or topological order constituting important examples. Correlations allow the quantification of the degree of order and the classification of different phases. Here we report measurements of first-order spatial correlations in a harmonically trapped two-dimensional photon gas below, at and above the critical particle number for Bose-Einstein condensation, using interferometric measurements of the emission of a dye-filled optical microcavity. For the uncondensed gas, the transverse coherence decays on a length scale determined by the thermal de Broglie wavelength of the photons, which shows the expected scaling with temperature. At the onset of Bose-Einstein condensation, true long-range order emerges, and we observe quantum statistical effects as the thermal wave packets overlap. The excellent agreement with equilibrium Bose gas theory prompts microcavity photons as promising candidates for studies of critical scaling and universality in optical quantum gases.Phase transitions in quantum matter are related to correlation effects and they can change the ordering of material. Here the authors measure the first-order spatial correlation and the de Broglie wavelength for both thermal and condensed form of a photonic Bose gas in a dye-filled optical microcavity.

SUBMITTER: Damm T

PROVIDER: S-EPMC5537358 | biostudies-literature | 2017 Jul

REPOSITORIES: biostudies-literature

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First-order spatial coherence measurements in a thermalized two-dimensional photonic quantum gas.

Damm Tobias T Dung David D Vewinger Frank F Weitz Martin M Schmitt Julian J

Nature communications 20170731 1

Phase transitions between different states of matter can profoundly modify the order in physical systems, with the emergence of ferromagnetic or topological order constituting important examples. Correlations allow the quantification of the degree of order and the classification of different phases. Here we report measurements of first-order spatial correlations in a harmonically trapped two-dimensional photon gas below, at and above the critical particle number for Bose-Einstein condensation, u ...[more]

PMID: 28761123

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Project description:The theory of electronic structure of many-electron systems, such as molecules, is extraordinarily complicated. A consideration of how electron density is distributed on average in the average field of the other electrons in the system, that is, mean field theory, is very instructive. However, quantitatively describing chemical bonds, reactions, and spectroscopy requires consideration of the way that electrons avoid each other while moving; this is called electron correlation (or in physics, the many-body problem for fermions). Although great progress has been made in theory, there is a need for incisive experimental tests for large molecular systems in the condensed phase. In this Account, we report a two-dimensional (2D) optical coherent spectroscopy that correlates the double-excited electronic states to constituent single-excited states. The technique, termed 2D double-quantum coherence spectroscopy (2D-DQCS), uses multiple, time-ordered ultrashort coherent optical pulses to create double- and single-quantum coherences over time intervals between the pulses. The resulting 2D electronic spectrum is a map of the energy correlation between the first excited state and two-photon allowed double-quantum states. The underlying principle of the experiment is that when the energy of the double-quantum state, viewed in simple models as a double HOMO-to-LUMO (highest occupied to lowest unoccupied molecular orbital) excitation, equals twice that of a single excitation, then no signal is radiated. However, electron-electron interactions, a combination of exchange interactions and electron correlation, in real systems generates a signal that reveals precisely how the energy of the double-quantum resonance differs from twice the single-quantum resonance. The energy shift measured in this experiment reveals how the second excitation is perturbed by both the presence of the first excitation and the way that the other electrons in the system have responded to the presence of that first excitation. We compare a series of organic dye molecules and find that the energy offset for adding a second electronic excitation to the system relative to the first excitation is on the order of tens of millielectronvolts; it also depends quite sensitively on molecular geometry. These results demonstrate the effectiveness of 2D-DQCS for elucidating quantitative information about electron-electron interactions, many-electron wave functions, and electron correlation in electronic excited states and excitons. Our work helps illuminate the implications of electron correlation on chemical systems. In a broad sense, we are trying to help address the fundamental question "How do we go beyond the orbital representation of electrons in the chemical sciences?"

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First-order spatial coherence measurements in a thermalized two-dimensional photonic quantum gas.

Publications

First-order spatial coherence measurements in a thermalized two-dimensional photonic quantum gas.

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