skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Multidimensional photon correlation spectroscopy of cavity polaritons

Abstract

The strong coupling of atoms and molecules to radiation field modes in optical cavities creates dressed matter/field states known as polaritons with controllable dynamical and energy transfer properties. We introduce a multidimensional optical spectroscopy technique for monitoring polariton dynamics. The response of a two-level atom to the time-dependent coupling to a single-cavity mode is monitored through time-and-frequency–resolved single-photon coincidence measurements of spontaneous emission. Polariton population and coherence dynamics and its variation with cavity photon number and controlled by gating parameters are indicated by solving the Jaynes–Cummings model.

Authors:
; ORCiD logo
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1418899
Alternate Identifier(s):
OSTI ID: 1527163
Grant/Contract Number:  
FG02-04ER15571; CHE-1663822
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 7; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; multidimensional spectroscopy; photon correlation; cavity polaritons

Citation Formats

Dorfman, Konstantin E., and Mukamel, Shaul. Multidimensional photon correlation spectroscopy of cavity polaritons. United States: N. p., 2018. Web. doi:10.1073/pnas.1719443115.
Dorfman, Konstantin E., & Mukamel, Shaul. Multidimensional photon correlation spectroscopy of cavity polaritons. United States. doi:10.1073/pnas.1719443115.
Dorfman, Konstantin E., and Mukamel, Shaul. Wed . "Multidimensional photon correlation spectroscopy of cavity polaritons". United States. doi:10.1073/pnas.1719443115.
@article{osti_1418899,
title = {Multidimensional photon correlation spectroscopy of cavity polaritons},
author = {Dorfman, Konstantin E. and Mukamel, Shaul},
abstractNote = {The strong coupling of atoms and molecules to radiation field modes in optical cavities creates dressed matter/field states known as polaritons with controllable dynamical and energy transfer properties. We introduce a multidimensional optical spectroscopy technique for monitoring polariton dynamics. The response of a two-level atom to the time-dependent coupling to a single-cavity mode is monitored through time-and-frequency–resolved single-photon coincidence measurements of spontaneous emission. Polariton population and coherence dynamics and its variation with cavity photon number and controlled by gating parameters are indicated by solving the Jaynes–Cummings model.},
doi = {10.1073/pnas.1719443115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 7,
volume = 115,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1719443115

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: (Top) Atom in the cavity emitting photons into the longitudinal cavity mode as well as noncavity vertical modes. Two TF-resolved detectors outside of the cavity register noncavity modes photon coincidence events. One photon number-resolving detector on the main optical axis measures photon number of the cavity mode photons.more » (Middle Left) Fock states. (Middle Right) Time evolution of the dressed atom plus cavity (polariton) states of the JC subject to the coupling Eq. 2. Vertical black dashed lines represent transition between different ladder states captured by spectroscopic measurements. (Bottom) Time evolution of the atom–cavity mode coupling λ(t) (black line) and population inversion〈σz(t)$\rangle$' Eq. 3 (red line) for an atom initially in the excited state with cavity mode being initially in the vacuum state.« less

Save / Share:

Works referenced in this record:

Characterization of Strong Light-Matter Coupling in Semiconductor Quantum-Dot Microcavities via Photon-Statistics Spectroscopy
journal, August 2008


Probing biological light-harvesting phenomena by optical cavities
journal, March 2012


Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode
journal, May 2015


Enhanced Raman Scattering from Vibro-Polariton Hybrid States
journal, June 2015

  • Shalabney, Atef; George, Jino; Hiura, Hidefumi
  • Angewandte Chemie International Edition, Vol. 54, Issue 27
  • DOI: 10.1002/anie.201502979

Quantum Nonlinear Optics with Polar J-Aggregates in Microcavities
journal, October 2014

  • Herrera, Felipe; Peropadre, Borja; Pachon, Leonardo A.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 21
  • DOI: 10.1021/jz501905h

Single-Photon Spectroscopy of a Single Molecule
journal, February 2012


Atomic emission and cavity field spectra for a two-photon Jaynes–Cummings model in the presence of the Stark shift
journal, January 1993

  • Nasreen, Tahira; Razmi, M. S. K.
  • Journal of the Optical Society of America B, Vol. 10, Issue 7
  • DOI: 10.1364/JOSAB.10.001292

Superradiance: An essay on the theory of collective spontaneous emission
journal, December 1982


Prospects for the cavity-assisted laser cooling of molecules
journal, February 2008


Observation of quantum collapse and revival in a one-atom maser
journal, January 1987


Resonance Absorption by Nuclear Magnetic Moments in a Solid
journal, January 1946

  • Purcell, E. M.; Torrey, H. C.; Pound, R. V.
  • Physical Review, Vol. 69, Issue 1-2, p. 37-38
  • DOI: 10.1103/PhysRev.69.37

Two-photon probe of the Jaynes–Cummings model and controlled symmetry breaking in circuit QED
journal, June 2008

  • Deppe, Frank; Mariantoni, Matteo; Menzel, E. P.
  • Nature Physics, Vol. 4, Issue 9
  • DOI: 10.1038/nphys1016

Coherent coupling of molecular resonators with a microcavity mode
journal, January 2015

  • Shalabney, A.; George, J.; Hutchison, J.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms6981

Strong Coupling between Plasmons and Organic Semiconductors
journal, May 2014


Cavity-Controlled Chemistry in Molecular Ensembles
journal, June 2016


Atoms and molecules in cavities, from weak to strong coupling in quantum-electrodynamics (QED) chemistry
journal, March 2017

  • Flick, Johannes; Ruggenthaler, Michael; Appel, Heiko
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 12
  • DOI: 10.1073/pnas.1615509114

Cavity polaritons in an organic single-crystalline rubrene microcavity
journal, June 2014

  • Tsuchimoto, Yuta; Nagai, Hikaru; Amano, Masamitsu
  • Applied Physics Letters, Vol. 104, Issue 23
  • DOI: 10.1063/1.4883485

Cavity Femtochemistry: Manipulating Nonadiabatic Dynamics at Avoided Crossings
journal, May 2016

  • Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 11
  • DOI: 10.1021/acs.jpclett.6b00864

SU(1,1), SU(2), and SU(3) coherence-preserving Hamiltonians and time-ordering techniques
journal, February 1987


Up on the Jaynes–Cummings ladder of a quantum-dot/microcavity system
journal, March 2010

  • Kasprzak, J.; Reitzenstein, S.; Muljarov, E. A.
  • Nature Materials, Vol. 9, Issue 4
  • DOI: 10.1038/nmat2717

Modifying Chemical Landscapes by Coupling to Vacuum Fields
journal, January 2012

  • Hutchison, James A.; Schwartz, Tal; Genet, Cyriaque
  • Angewandte Chemie International Edition, Vol. 51, Issue 7
  • DOI: 10.1002/anie.201107033

Lie Algebraic Solution of Linear Differential Equations
journal, April 1963

  • Wei, James; Norman, Edward
  • Journal of Mathematical Physics, Vol. 4, Issue 4
  • DOI: 10.1063/1.1703993

Nonlinear optical signals and spectroscopy with quantum light
journal, December 2016


Optimization of photon correlations by frequency filtering
journal, April 2015

  • González-Tudela, Alejandro; del Valle, Elena; Laussy, Fabrice P.
  • Physical Review A, Vol. 91, Issue 4
  • DOI: 10.1103/PhysRevA.91.043807

Generalized Jaynes-Cummings models with a time-dependent atom-field coupling
journal, September 1993


Two-dimensional infrared spectroscopy of vibrational polaritons of molecules in an optical cavity
journal, March 2016

  • Saurabh, Prasoon; Mukamel, Shaul
  • The Journal of Chemical Physics, Vol. 144, Issue 12
  • DOI: 10.1063/1.4944492

Cavity sideband cooling of trapped molecules
journal, September 2011


Room-temperature polariton lasing in an organic single-crystal microcavity
journal, April 2010


Coherence in Spontaneous Radiation Processes
journal, January 1954


Influence of multi-exciton correlations on nonlinear polariton dynamics in semiconductor microcavities
journal, February 2013


Ultrafast all-optical switching by single photons
journal, August 2012


Direct measurement of polariton–polariton interaction strength
journal, June 2017

  • Sun, Yongbao; Yoon, Yoseob; Steger, Mark
  • Nature Physics, Vol. 13, Issue 9
  • DOI: 10.1038/nphys4148

Up-conversion single-photon detector using multi-wavelength sampling techniques
journal, January 2011

  • Ma, Lijun; Bienfang, Joshua C.; Slattery, Oliver
  • Optics Express, Vol. 19, Issue 6
  • DOI: 10.1364/OE.19.005470

Hybrid Light–Matter States in a Molecular and Material Science Perspective
journal, October 2016


Cavity Quantum Electrodynamics
journal, January 1989

  • Haroche, Serge; Kleppner, Daniel
  • Physics Today, Vol. 42, Issue 1
  • DOI: 10.1063/1.881201

Exact isolated solutions for the class of quantum optical systems
journal, February 1986


Ultrastrong Coupling of Plasmons and Excitons in a Nanoshell
journal, October 2014

  • Cacciola, Adriano; Di Stefano, Omar; Stassi, Roberto
  • ACS Nano, Vol. 8, Issue 11
  • DOI: 10.1021/nn504652w

Strong coupling between chlorosomes of photosynthetic bacteria and a confined optical cavity mode
journal, November 2014

  • Coles, David M.; Yang, Yanshen; Wang, Yaya
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6561

Quantum Interference of Tunably Indistinguishable Photons from Remote Organic Molecules
journal, March 2010


The time-dependent physical spectrum of light*
journal, January 1977

  • Eberly, J. H.; Wódkiewicz, K.
  • Journal of the Optical Society of America, Vol. 67, Issue 9
  • DOI: 10.1364/JOSA.67.001252

Time-and-frequency-gated photon coincidence counting; a novel multidimensional spectroscopy tool
journal, July 2016


Nonclassical Photon Statistics in Single-Molecule Fluorescence at Room Temperature
journal, February 2000


Indistinguishability and correlations of photons generated by quantum emitters undergoing spectral diffusion
journal, February 2014

  • Dorfman, Konstantin E.; Mukamel, Shaul
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep03996

Quantum efficiency of single-photon sources in the cavity-QED strong-coupling regime
journal, January 2005


Comparison of quantum and semiclassical radiation theories with application to the beam maser
journal, January 1963


Optical microcavities enhance the exciton coherence length and eliminate vibronic coupling in J-aggregates
journal, May 2015

  • Spano, F. C.
  • The Journal of Chemical Physics, Vol. 142, Issue 18
  • DOI: 10.1063/1.4919348

Exact solutions to a class of Jahn-Teller systems
journal, May 1979


Optical multidimensional coherent spectroscopy
journal, July 2013

  • Cundiff, Steven T.; Mukamel, Shaul
  • Physics Today, Vol. 66, Issue 7
  • DOI: 10.1063/PT.3.2047

Vacuum-stimulated cooling of single atoms in three dimensions
journal, October 2005

  • Nußmann, Stefan; Murr, Karim; Hijlkema, Markus
  • Nature Physics, Vol. 1, Issue 2
  • DOI: 10.1038/nphys120

Algebraic treatment of the time-dependent Jaynes–Cummings Hamiltonian including nonlinear terms
journal, August 2012


Spanning Strong to Weak Normal Mode Coupling between Vibrational and Fabry–Pérot Cavity Modes through Tuning of Vibrational Absorption Strength
journal, September 2015


Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
journal, November 2016

  • Cocker, Tyler L.; Peller, Dominik; Yu, Ping
  • Nature, Vol. 539, Issue 7628
  • DOI: 10.1038/nature19816

Theory of Frequency-Filtered and Time-Resolved N -Photon Correlations
journal, October 2012


    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.