Mechanisms Underlying a Quantum Superposition Microscope Based on THz-Driven Coherent Oscillations in a Two-Level Molecular Sensor

Xia, Yunpeng; Wang, Likun; Ho, Wilson

doi:10.1103/physrevlett.132.076903

Title: Mechanisms Underlying a Quantum Superposition Microscope Based on THz-Driven Coherent Oscillations in a Two-Level Molecular Sensor

Journal Article · 15 February 2024 · Physical Review Letters

DOI: https://doi.org/10.1103/physrevlett.132.076903 · OSTI ID:2340240

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Univ. of California, Irvine, CA (United States); University of California, Irvine
Univ. of California, Irvine, CA (United States)

Here we report pump-probe measurements of a hydrogen molecule (H₂) in the tunnel junction of a scanning tunneling microscope (STM) coupled to ultrashort terahertz (THz) pulses. The coherent oscillation of the THz induced DC tunneling current at a frequency of ~0.5 THz fingerprints the absorption by H₂ as a two-level system (TLS). Two components of the oscillatory signal are observed and point to both photon and field aspects of the THz pulses. A few loosely bound states with similar energies for the upper state of the TLS are evidenced by the coherent revival of oscillatory signal. Furthermore, the comparison of spectroscopic features of H₂ with different tips provides an understanding of the TLS for H₂.

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Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0024037; SC0019448

OSTI ID:: 2340240

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 7 Vol. 132; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (46)

The 2-Channel Kondo Model von Delft, Jan; Ralph, D. C.; Buhrman, R. A. Annals of Physics, Vol. 263, Issue 1 https://doi.org/10.1006/aphy.1997.5750	journal	February 1998
Quantifying residual hydrogen adsorption in low-temperature STMs Natterer, F. D.; Patthey, F.; Brune, H. Surface Science, Vol. 615 https://doi.org/10.1016/j.susc.2013.04.008	journal	September 2013
Principles of Nano-Optics Novotny, Lukas; Hecht, Bert Cambridge University Press https://doi.org/10.1017/CBO9780511794193	book	January 2012
Trapping and Characterization of a Single Hydrogen Molecule in a Continuously Tunable Nanocavity Wang, Hui; Li, Shaowei; He, Haiyan The Journal of Physical Chemistry Letters, Vol. 6, Issue 17 https://doi.org/10.1021/acs.jpclett.5b01501	journal	August 2015
Single-Molecule Continuous-Wave Terahertz Rectification Spectroscopy and Microscopy Chen, Siyu; Shi, Wenlu; Ho, W. Nano Letters, Vol. 23, Issue 7 https://doi.org/10.1021/acs.nanolett.3c00271	journal	March 2023
Tailoring Single-Cycle Near Field in a Tunnel Junction with Carrier-Envelope Phase-Controlled Terahertz Electric Fields Yoshioka, Katsumasa; Katayama, Ikufumi; Arashida, Yusuke Nano Letters, Vol. 18, Issue 8 https://doi.org/10.1021/acs.nanolett.8b02161	journal	July 2018
A Single Hydrogen Molecule as an Intensity Chopper in an Electrically Driven Plasmonic Nanocavity Merino, Pablo; Rosławska, Anna; Leon, Christopher C. Nano Letters, Vol. 19, Issue 1 https://doi.org/10.1021/acs.nanolett.8b03753	journal	December 2018
Phase-Resolved Detection of Ultrabroadband THz Pulses inside a Scanning Tunneling Microscope Junction Müller, Melanie; Martín Sabanés, Natalia; Kampfrath, Tobias ACS Photonics, Vol. 7, Issue 8 https://doi.org/10.1021/acsphotonics.0c00386	journal	July 2020
Subcycle Transient Scanning Tunneling Spectroscopy with Visualization of Enhanced Terahertz Near Field Yoshida, Shoji; Hirori, Hideki; Tachizaki, Takehiro ACS Photonics, Vol. 6, Issue 6 https://doi.org/10.1021/acsphotonics.9b00266	journal	May 2019
Resonant-Enhanced Spectroscopy of Molecular Rotations with a Scanning Tunneling Microscope Natterer, Fabian Donat; Patthey, François; Brune, Harald ACS Nano, Vol. 8, Issue 7 https://doi.org/10.1021/nn501999k	journal	June 2014
Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging Cocker, Tyler L.; Peller, Dominik; Yu, Ping Nature, Vol. 539, Issue 7628 https://doi.org/10.1038/nature19816	journal	November 2016
An ultrafast terahertz scanning tunnelling microscope Cocker, Tyler L.; Jelic, Vedran; Gupta, Manisha Nature Photonics, Vol. 7, Issue 8 https://doi.org/10.1038/nphoton.2013.151	journal	July 2013
Real-space coherent manipulation of electrons in a single tunnel junction by single-cycle terahertz electric fields Yoshioka, Katsumasa; Katayama, Ikufumi; Minami, Yasuo Nature Photonics, Vol. 10, Issue 12 https://doi.org/10.1038/nphoton.2016.205	journal	November 2016
Ultrafast terahertz control of extreme tunnel currents through single atoms on a silicon surface Jelic, Vedran; Iwaszczuk, Krzysztof; Nguyen, Peter H. Nature Physics, Vol. 13, Issue 6 https://doi.org/10.1038/nphys4047	journal	February 2017
Quantitative sampling of atomic-scale electromagnetic waveforms Peller, D.; Roelcke, C.; Kastner, L. Z. Nature Photonics, Vol. 15, Issue 2 https://doi.org/10.1038/s41566-020-00720-8	journal	November 2020
Nanoscale terahertz scanning probe microscopy Cocker, T. L.; Jelic, V.; Hillenbrand, R. Nature Photonics, Vol. 15, Issue 8 https://doi.org/10.1038/s41566-021-00835-6	journal	July 2021
Time-resolved collapse and revival of the Kondo state near a quantum phase transition Wetli, C.; Pal, S.; Kroha, J. Nature Physics, Vol. 14, Issue 11 https://doi.org/10.1038/s41567-018-0228-3	journal	July 2018
Sub-cycle atomic-scale forces coherently control a single-molecule switch Peller, Dominik; Kastner, Lukas Z.; Buchner, Thomas Nature, Vol. 585, Issue 7823 https://doi.org/10.1038/s41586-020-2620-2	journal	September 2020
Antenna effects in terahertz apertureless near-field optical microscopy Wang, Kanglin; Mittleman, Daniel M.; van der Valk, Nick C. J. Applied Physics Letters, Vol. 85, Issue 14 https://doi.org/10.1063/1.1797554	journal	October 2004
Slow two-level systems in point contacts Halbritter, A.; Borda, L.; Zawadowski, A. Advances in Physics, Vol. 53, Issue 8 https://doi.org/10.1080/00018730412331324981	journal	December 2004
A novel method achieving ultra-high geometrical resolution in scanning tunnelling microscopy Temirov, R.; Soubatch, S.; Neucheva, O. New Journal of Physics, Vol. 10, Issue 5 https://doi.org/10.1088/1367-2630/10/5/053012	journal	May 2008
Orientational quantum revivals induced by a single-cycle terahertz pulse Shu, Chuan-Cun; Hong, Qian-Qian; Guo, Yu Physical Review A, Vol. 102, Issue 6 https://doi.org/10.1103/PhysRevA.102.063124	journal	December 2020
Zero-bias anomaly of point-contact resistance due to adiabatic electron renormalization of dynamical defects Kozub, V. I.; Rudin, A. M. Physical Review B, Vol. 55, Issue 1 https://doi.org/10.1103/PhysRevB.55.259	journal	January 1997
Phonons in Solid Hydrogen and Deuterium Studied by Inelastic Coherent Neutron Scattering Nielsen, M. Physical Review B, Vol. 7, Issue 4 https://doi.org/10.1103/PhysRevB.7.1626	journal	February 1973
Strongly coverage-dependent excitations of adsorbed molecular hydrogen Gupta, J. A.; Lutz, C. P.; Heinrich, A. J. Physical Review B, Vol. 71, Issue 11 https://doi.org/10.1103/PhysRevB.71.115416	journal	March 2005
Huge negative differential conductance inAu−H2molecular nanojunctions Halbritter, A.; Makk, P.; Csonka, Sz. Physical Review B, Vol. 77, Issue 7 https://doi.org/10.1103/PhysRevB.77.075402	journal	February 2008
Bistable hysteresis and resistance switching in hydrogen-gold junctions Trouwborst, M. L.; Huisman, E. H.; van der Molen, S. J. Physical Review B, Vol. 80, Issue 8 https://doi.org/10.1103/PhysRevB.80.081407	journal	August 2009
Inelastic electron tunneling mediated by a molecular quantum rotator Sugimoto, Toshiki; Kunisada, Yuji; Fukutani, Katsuyuki Physical Review B, Vol. 96, Issue 24 https://doi.org/10.1103/PhysRevB.96.241409	journal	December 2017
Imaging Pauli Repulsion in Scanning Tunneling Microscopy Weiss, C.; Wagner, C.; Kleimann, C. Physical Review Letters, Vol. 105, Issue 8 https://doi.org/10.1103/PhysRevLett.105.086103	journal	August 2010
Rotational and Vibrational Excitations of a Hydrogen Molecule Trapped within a Nanocavity of Tunable Dimension Li, Shaowei; Yu, Arthur; Toledo, Freddy Physical Review Letters, Vol. 111, Issue 14 https://doi.org/10.1103/PhysRevLett.111.146102	journal	October 2013
Distinction of Nuclear Spin States with the Scanning Tunneling Microscope Natterer, Fabian Donat; Patthey, François; Brune, Harald Physical Review Letters, Vol. 111, Issue 17 https://doi.org/10.1103/PhysRevLett.111.175303	journal	October 2013
Rotational Spectromicroscopy: Imaging the Orbital Interaction between Molecular Hydrogen and an Adsorbed Molecule Li, Shaowei; Yuan, Dingwang; Yu, Arthur Physical Review Letters, Vol. 114, Issue 20 https://doi.org/10.1103/PhysRevLett.114.206101	journal	May 2015
Launching Coherent Acoustic Phonon Wave Packets with Local Femtosecond Coulomb Forces Sheng, Shaoxiang; Oeter, Anne-Catherine; Abdo, Mohamad Physical Review Letters, Vol. 129, Issue 4 https://doi.org/10.1103/PhysRevLett.129.043001	journal	July 2022
Electrical Manipulation of Quantum Coherence in a Two-Level Molecular System Wang, Likun; Bai, Dan; Xia, Yunpeng Physical Review Letters, Vol. 130, Issue 9 https://doi.org/10.1103/PhysRevLett.130.096201	journal	February 2023
Interaction between Closed-Shell Systems and Metal Surfaces Lang, N. D. Physical Review Letters, Vol. 46, Issue 13 https://doi.org/10.1103/PhysRevLett.46.842	journal	March 1981
Observation of Rotational Excitations of H 2 Adsorbed on Ag Surfaces Avouris, Ph.; Schmeisser, D.; Demuth, J. E. Physical Review Letters, Vol. 48, Issue 3 https://doi.org/10.1103/PhysRevLett.48.199	journal	January 1982
Quantum beats of excitons in quantum wells Göbel, E. O.; Leo, K.; Damen, T. C. Physical Review Letters, Vol. 64, Issue 15 https://doi.org/10.1103/PhysRevLett.64.1801	journal	April 1990
Generation of Nonclassical Motional States of a Trapped Atom Meekhof, D. M.; Monroe, C.; King, B. E. Physical Review Letters, Vol. 76, Issue 11 https://doi.org/10.1103/PhysRevLett.76.1796	journal	March 1996
Dipole Active Vibrational Motion in the Physisorption Well Svensson, K.; Andersson, S. Physical Review Letters, Vol. 78, Issue 10 https://doi.org/10.1103/PhysRevLett.78.2016	journal	March 1997
Vibrationally Induced Two-Level Systems in Single-Molecule Junctions Thijssen, W. H. A.; Djukic, D.; Otte, A. F. Physical Review Letters, Vol. 97, Issue 22 https://doi.org/10.1103/PhysRevLett.97.226806	journal	December 2006
Room-temperature coherent revival in an ensemble of quantum dots Khanonkin, Igor; Eyal, Ori; Reithmaier, Johann Peter Physical Review Research, Vol. 3, Issue 3 https://doi.org/10.1103/PhysRevResearch.3.033073	journal	July 2021
High-Power Terahertz Generation Using Large-Area Plasmonic Photoconductive Emitters Yardimci, Nezih T.; Yang, Shang-Hua; Berry, Christopher W. IEEE Transactions on Terahertz Science and Technology, Vol. 5, Issue 2 https://doi.org/10.1109/TTHZ.2015.2395417	journal	March 2015
Coherent Dynamics of a Single Spin Interacting with an Adjustable Spin Bath Hanson, R.; Dobrovitski, V. V.; Feiguin, A. E. Science, Vol. 320, Issue 5874 https://doi.org/10.1126/science.1155400	journal	April 2008
Driving a Macroscopic Oscillator with the Stochastic Motion of a Hydrogen Molecule Lotze, C.; Corso, M.; Franke, K. J. Science, Vol. 338, Issue 6108 https://doi.org/10.1126/science.1227621	journal	November 2012
Probing and imaging spin interactions with a magnetic single-molecule sensor Czap, Gregory; Wagner, Peter J.; Xue, Feng Science, Vol. 364, Issue 6441 https://doi.org/10.1126/science.aaw7505	journal	May 2019
Atomic-scale quantum sensing based on the ultrafast coherence of an H ₂ molecule in an STM cavity Wang, Likun; Xia, Yunpeng; Ho, W. Science, Vol. 376, Issue 6591 https://doi.org/10.1126/science.abn9220	journal	April 2022

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Title: Mechanisms Underlying a Quantum Superposition Microscope Based on THz-Driven Coherent Oscillations in a Two-Level Molecular Sensor

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