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Deviation from the normal mode expansion in a coupled graphene-nanomechanical system Cornelia Schwarz,1 Benjamin Pigeau,1 Laure Mercier de L´epinay,1 Aur´elien G. Kuhn,1 Dipankar Kalita,1 Nedjma Bendiab,1 La¨etitia Marty,1 Vincent Bouchiat,1 and Olivier Arcizet1 1Institut N´eel, Universit´e Grenoble Alpes - CNRS:UPR2940, 38042 Grenoble, France We optomechanically measure the vibrations of a nanomechanical system made of a graphene membrane suspended on a silicon nitride nanoresonator. When probing the 6 thermal noiseof the couplednanomechanical device,we observea significantdeviation 1 from the normal mode expansion. It originates from the heterogeneous character of 0 mechanicaldissipationoverthespatialextensionofcoupledeigenmodes,whichviolates 2 one of the fundamental prerequisite for employing this commonly used description of n the nanoresonators’ thermal noise. We subsequently measure the local mechanical a susceptibility and demonstrate that the fluctuation-dissipation theorem still holds and J permits a proper evaluation of the thermal noise of the nanomechanical system. Since 2 it naturally becomes delicate to ensure a good spatial homogeneity at the nanoscale, thisapproachisfundamentaltocorrectlydescribethethermalnoiseofnanomechanical ] systems which ultimately impact their sensing capacity. l l a h Nanomechanical oscillators are routinely used in - s fundamental and applied physics [1, 2] as ultrasensitive e force or mass sensors due to their increased sensitivity m to their environment. The understanding of dissipation . t at the nanoscale is the key ingredient towards extreme a m sensitivity operation. Among others, carbon-based nanoresonators and novel 2D materials [3] have revolu- - d tionized the field of nanomechanics [4–14] by pushing n the oscillator dimensions down to a single atomic layer. o The extremesensitivities achievedareultimately limited c by the thermal noise of the nanoresonators, which [ underlines the importance of correctly understanding 1 and describing their Brownian motion. The thermal v noiseofa vibratingnanomechanicalsystemis commonly 4 5 described using the normal mode expansion, which as- 1 sumes that each eigenmode is driven by an independent 0 fluctuating Langevin force, presenting no correlation 0 with other eigenmodes. However, this intuitive de- . 1 scription only holds when the mechanical dissipation is 0 homogeneously distributed in the system [15, 16]. Oth- FIG.1. Theexperimentalsetup. a)SEMofa20×20µm2 6 suspended CVD grown graphene monolayer supported on a erwise, inhomogeneous damping can create dissipative 1 300nm-thick SiN nanomembrane, as sketched in b). c) Ex- : coupling between eigenmodes, leading to a violation perimental setup: a balanced homodyne detection measures v of their assumed independence. Such deviations which the phase fluctuations of the probe laser field reflected by i X have been reported on macroscopic devices [17, 18], are the sample and monitor its position fluctuations. A second expected to be extremely important in nanomechanical counter-propagating pump laser beam can be intensity mod- r a systems, since it becomes increasingly difficult to ensure ulatedtooptomechanicallydrivethecouplednanoresonators. The experiment is performed at pressures below 10−3mbar. and even measure a good spatial homogeneity over the d)Modeldescribingtheinertiallycouplednanoresonators. e) entire nanosystem as its size is decreased. However, Thermal noise of a graphene membrane, the sharp peaks on no deviations from the normal mode expansion were each side are weakly coupled SiN eigenmodes. observed at the nanoscale up to now, despite the large variety of nanoresonators investigated. In this article, we report on the deviation from the normal mode expansion in the optomechanically mea- from the normal mode expansion, we exploit the in- sured thermal noise of a nanomechanical arrangement ertial coupling between both nanoresonators: under made of a suspended graphene monolayer coupled to a temperature-controlled tunable hybridization, the a silicon nitride nanomembrane which supports the coupled eigenmodes become spatially delocalized on the graphene resonator. To fully explore the deviation two subsystems whose intrinsic mechanical damping 2 rates differ by 2 orders of magnitude. In this situation oscillates around 100kHz. They present larger quality the damping homogeneity is therefore altered which factors (above 1000) but higher masses, on the order of results in a pronounceddeviationfromthe normalmode 10−12kg. In the following we investigate the thermal expansion that we report on and analyze. Then we noise of the coupled system. provethat the fluctuation-dissipationtheoremstill holds by measuring the local mechanical susceptibility of the Hybridization of graphene eigenmodes– In order to coupled nanomechanical system. tune the eigenfrequencies, we exploit the partial absorp- These considerations are essential to correctly describe tionofasecondlaserbeamat532nmfocusseddowntoan nanomechanical systems affected by inhomogeneous opticalwaistof 300nm,spatiallysuperimposedonthe ≃ damping and point out the importance of having ac- probe beam and injected from the backside of the sam- cess to the local mechanical susceptibility to correctly ple. It generates a slight temperature increase which is estimate the thermal noise of complex nanomechanical almost not detectable in the Brownian temperature (see systems. Fig.2e) but is sufficient to significantly thermally tune the graphene eigenfrequency. A clear hybridization be- The experiment– Our nanomechanical system is a tween both graphene and Si3N4 eigenmodes is shown in fully suspended single layer graphene sheet deposited Fig.2bwhereapronouncedfrequencyanticrossingcanbe on a square window opened in a Si N nano-resonator, seen, as well as a modification of the mechanical damp- 3 4 itself supported on a tapped silicon wafer (see Fig.1) ing rates. Such signatures are fingerprints of strongdual which allows a dual optical access from both sides. mode coupling [25], which canalso affect the force sensi- It is obtained (see SI) by transfer in liquid phase of tivity [26–28]. monolayer, poly-crystalline graphene grown by CVD The modelisation of our inertially coupled nanomechan- on Cu [19, 20] and suspended over up to 25x25µm2 ical system is based on cascaded mechanical oscillators on a pre-etched stoichiometric Si3N4 membrane which [15], as sketched in Fig.1d. Their vibrations δxG,δxS is 500-nm-thick and 100-µm-wide. A 633nm probe around the rest positions are coupled through δx¨G = laser is focussed on the graphene resonator with a high −Ω2G(δxG−δxS)−ΓG(δx˙G−δx˙S)+δFG/MG andδx¨S = numerical aperture objective (≈ 400nm optical waist). −Ω2SδxS−ΓSδx˙S+µΩ2G(δxG−δxS)+µΓG(δx˙G−δx˙S)+ The weak reflected beam constitutes the signal arm of δFS/MS, where ΩG,S/2π (resp. ΓG,S ) are the uncou- a balanced homodyne detection [21] (see Fig.1c and pled frequencies (resp. damping rates). δFG is an ex- SI). This interferometer permits a shot-noise limited ternal force applied on the graphene membrane, MG readout of the membrane’s thermal noise with injected the grapheneeffective massatthe measurementlocation optical powers ranging from 1 to 100µW. A fast piezo [16], while µ MG/MS parameterizes the hybridiza- ≡ element driving the local oscillator mirror permits a tion strength. Depending on the graphene and Si3N4 robust calibration of the interferometer, insensitive in membrane geometries which govern the vibration mode particular to spatial drifts or reflectivity variations due spectrum and their spatial profiles, anticrossings with to non-homogeneous graphene properties (wrinkles or varying strength can be observed (see SI). Intuitively, grain boundaries). Reflectivities in the 1 10% range if graphene is positioned at a node of the membrane − were measured on monolayers depending on the level of eigenmode, their hybridization will be reduced. In the contaminants. A typical calibrated displacement noise Fourier domain we have δxG = χ[Ω] δFG , using spectrum is shown in Fig.1. Its reproduction at varying δx [Ω] dteiΩtδx (t). (cid:0)TδhxeS(cid:1)dynamical·(cid:16)mµaδtFriSx(cid:17)χ[Ω]−1 optical powers permits to verify the absence of optical i ≡ R i being R backaction (see SI). The uncoupled graphene resonators presentfundamental eigenmodes in the 1-10MHz range, χ−1 M Ω2 χ−1 G G − G , (1) with quality factors from 10 to 500 in vacuum and effec- (cid:18)µ M Ω2 χ−1 µ χ−1+χ−1+M Ω2 (cid:19) tive masses ranging from 10−16 to 10−14kg. Operating (cid:0) G − G (cid:1) (cid:0) S G G (cid:1) where we used the uncoupled mechanical susceptibili- with fully transmitting systems permits suppressing additional cavity effects [22] which could complicate ties χG,S ≡ MG−,1S Ω2G,S−Ω2−iΩΓG,S −1. Diagonaliz- the noise thermometry. The spatial profile of graphene ing the restoringfo(cid:0)rcematrix M−1χ[0]−(cid:1)1 yields the new G eigenmodes can be mapped by probing thermal noise eigenfrequencies Ω /2π of the coupled system: ± spectra at varying positions on the graphene membrane, see SI. The slight elliptical structure and the frequency Ω2 (1+µ)Ω2G+Ω2S q(Ω2S−(1+µ)Ω2G)2+4µΩ2GΩ2S. splitting observed on higher order modes reflects the ± ≡ 2 ± 2 presence of a residual 20 MPa stress along the diagonal (2) direction [23, 24], attributed to the graphene transfer When µ 1, the minimum relative frequency splitting ≪ process. Also visible on the thermal noise spectrum are amounts to √µ, corresponding to a canonically defined sharp peaks corresponding to higher order eigenmodes coupling strength of g = ΩG√µ [25]. Depending on the of the Si N nanomembrane, whose fundamental mode samplegeometryalargevarietyofcouplingstrengthscan 3 4 3 Violation of the normal mode expansion– Meanwhile, a striking feature can be seen in the displacement noise spectrashowninFig.2: acharacteristicpeakasymmetry and a sharp noise minimum between both eigenmodes areclearlyvisible inthe anticrossingregion. Thesespec- tra cannot be fitted with two independent mechanical thermalnoisespectra,seeFig.2a,withadeviationlarger than 10 dB observed in the vicinity of Ω . Therefore S the measured thermal noise cannot be described by two eigenmodes driven with independent Langevin forces, which reveals the violation of the normal mode expansion. This is a consequence of the spatial inho- mogeneity of damping rates across the system: acoustic vibrations are more efficiently damped in graphene than in Si N . When the eigenmodes become hybridized, 3 4 their spatial profiles are delocalized over both systems, see Fig.2c insets, so that mechanical damping becomes inhomogeneous over the eigenmode spatial extension. Thus the spatial profile of the vibration pattern cannot be stationary anymore since it is non-homogeneously damped and cannot be preserved over time. As such, dissipation is now able to couple eigenmodes, which breaks the fundamental hypothesis required to apply FIG. 2. Thermal noise of the hybridized eigenmodes the normal mode expansion [15, 16]. When ΩG = ΩS, a)Thermalnoiseofthecouplednanomechanicalsystemwhen the thermal noise spectral density at the minimum noise tuned to an anticrossing region by adjusting the pump in- frequency is measured at a level 2Γ /Γ times lower G S tensity (400µW). Lower traces are obtained after numerical ≈ than the prediction of the normal mode expansion, see background substraction. Solid lines are thebest fitsderived SI. The understanding of this deviation is critical to employing the normal mode expansion. Dashed green lines patch the normal mode expansion and work out an are fits using expression (3). b) Spectra measured through the anticrossing for increasing tuning laser powers. Dashed analytical description of the system fluctuations. lines are fits using (3) with fitting parameters ΩS,G,ΓS,G re- ported in c), d) using µ = 0.002. Purple disks represent the Thermal noise of the hybridized nanomechanical measured coupledeigenfrequencies Ω±/2π andsolid linesare system– To properly describe the nanosystem thermal deduced from equation (2). d) Similar analysis for damping noise, it is necessary to return to the original formula- ratesΓ±/2π. e)RelativeBrowniantemperaturevariationde- tion of the fluctuation-dissipation theorem [15, 30]: duced from the fits. 2k T B S [Ω]= Imχ [Ω] , (3) δxG Ω | GG | | | beobserved,upto200kHz,largelyenteringtheso-called which relates the measured displacement noise spectral strongcouplingregime(g >ΓS,ΓG). Theexperimentally density to the local mechanical susceptibility χGG. The measured coupled eigenfrequencies are shown in Fig.2c latter connects the optomechanically measureddeforma- forincreasingpumplaserpowers. Theycanbewellfitted tions of the graphene membrane δx [Ω] to the external G using equation (2) and a linear pump power dependence forceδF appliedonthegraphenemembraneatthemea- G for the uncoupled graphene and Si3N4 eigenfrequencies surement point: δxG[Ω] = χGG[Ω]δFG. First we pursue of 284Hz/µW and 2Hz/µW respectively. The latter theanalysisbasedonthemodelemployedabove. Invert- − − corresponds to a maximum static heating of the Si3N4 ing equation (1) we obtain: nanoresonator estimated at the level of 1K [29]. Us- ingtheexperimentallymeasuredheatdiff≃usioncoefficient χ−1+M Ω2 2 of 5 10−6m2/s, see SI, the thermal heat resistance of χGG[Ω]−1 =χ−G1− χ−(cid:0)1G+χ−1+GM(cid:1)Ω2. (4) grap×hene was numerically estimated at 0.25K per µW G S G absorbed. The effective mechanicaldamping rates Γ of which permits deriving the expected thermal noise (see ± the coupled modes can be roughly estimated using the SI).Ourexperimentalresultscanbe wellfitted withthis FWHM of the thermal noise spectra, see Fig.2d, and model,seeFig.2a,2b,usingthefittingparameterswhich used to extrapolate the uncoupled damping rates (see are reported in Fig.2c,2d and 2e. The magnitude of the SI). coupling parameter µ = 0.002 is also in agreement with theratioofbareeffectivemassesofbothnanoresonators. 4 No significant variation in the fitted noise temperature feedback loop in the measurement span, the transfer could be detected, see Fig.2e, which places an upper function of allphotodetectors employedand the spectral bound of 10K on the maximum temperature increase response of the AOM. With this, the expected thermal ≃ induced by the tuning laser. This observation is also noise can be properly estimated using equation (3) and consistent with the estimated thermal resistance given compared to the measured thermal noise spectrum, as above and allows to neglect the role of temperature shown in Fig.3e. The excellent quantitative agreement inhomogeneities in our modelisation. found between both measurements all across the hy- Validity of the fluctuation dissipation theorem in the bridization (see SI) demonstrates the validity of the coupled nanomechanical system–Verifyingthevalidityof fluctuation-dissipation theorem in our strongly coupled the fluctuation-dissipation theorem is essential in order nanomechanical arrangement. to assess that the measured spectra correspond to the The hybridization dramatically modifies the graphene thermal noise of the system. Following the principles mechanical response and has an impact on the signal- of linear response theory [30], this requires measuring to-noise ratio (SNR) observed in a force measurement. the local mechanical susceptibility χ of the coupled For a monochromatic force of amplitude δF ap- GG G nanomechanical system. To do so we modulate the plied in the center of the graphene membrane, the pump beam intensity by means of an acousto-optic SNR can be expressed as SNR[Ω] = |Imχ−G1| where modulator (AOM) and realize response measurements SNRG |Imχ−GG1| SNR δF2/2M Γ k T represents the SNR of the by sweeping the modulation frequency while recording G ≡ G G G B uncoupled graphene alone. As verified experimentally the driven displacement. Both laser spots are carefully and confirmed with the model, see SI, the SNR can superimposed on the graphene membrane to access to be improved with respect to the uncoupled graphene the local susceptibility; it is worth mentioning that this resonator in narrow frequency bands in the vicinity measurement cannot be realized with electrostatic gate of the Si N resonance. As already employed with or with piezo actuations since their spatial excitation 3 4 macroscopic devices [18], this constitutes a strategy for profile is not localized on the measurement spot. We achieving larger sensitivities in hybrid nano-sensors. first verify the linearity of the actuation, see Fig.3a by varying the optical modulation depth δP over 2 orders of magnitude without modifying the mean pump power (60µW) to ensure a stable graphene frequency, away Conclusions– We have demonstrated the violation of from anticrossings. No deviation from linearity were thenormalmodeexpansioninamultimodenanomechan- observed in the driven oscillations up to a maximum ical system and verified that the fluctuation-dissipation amplitude of 1nm, a few times the monolayer thickness theoremwelldescribesitsthermalnoisedespitethelarge (0.3nm), so that we perfectly sit in the linear actua- mass and damping asymmetries. This work underlines tion/measurementregime. Atypical actuationefficiency the importance of measuring the local mechanical sus- of 17pm/µW is measured, corresponding to an optical ceptibility of a nanosystem to correctly understand its force of 540fN/µW. This is significantly larger than the thermal noise. Since a good sample homogeneity cannot radiation pressure force contribution of 0.3fN/µW for a be maintained in extremely down-sized nanomechanical 10%absorptioncoefficient,whichconfirmsthe dominant devices, we anticipate that these deviations will play role of thermo-optical forces in the optical actuation of an important role in the future of nanomechanical graphene [22]. The backaction noise due to the intensity sensors. Our observations, realized on inertially coupled fluctuations of the shot noise limited laser beams can nanomechanical oscillators have a more general reach thus be evaluated at the level of 0.1fm/√Hz for ≃ andarealsovalidwhenmechanicalmodesareexternally P =100µW. This is largely negligible compared to the 0 coupled, such as by optical or electrostatic force field measured thermal noise so that backaction cancelation gradients [8, 14, 33–36]. Such a fundamental approach [31] or classical noise squashing mechanisms [32] can be could be used for developing new force detection proto- safely excluded to interpret our results. cols based on multimodal nanosystems. Several response measurements were subsequently performed through the anticrossing in the same mea- surement conditions as in Fig.2a by progressively increasing the pump intensity, while maintaining a Acknowledgements— We warmly thank J.Jarreau, fixed modulation depth (δP/P0 = 30%). The response C.Hoarau, E.Eyraud, D.Lepoittevin, B.Fernandez, curves shown in Fig.3c permit, once combined with the J.P.Poizat,A.GloppeandB.Besgaforexperimentaland optical to force conversion factor measured in Fig.3a in technical assistance. This project is supported by the absence ofhybridization, to determine the complex local ANR FOCUS, the ERC Starting Grant StG-2012-HQ- mechanical susceptibility, χGG[Ω], as shown in Fig.3d. NOM, the E.U. Graphene Flagship and Lanef (CryOp- Its proper determination requires taking into account tics). C.S. acknowledges funding from the Nanoscience the weak residual contribution of the interferometer Foundation. 5 FIG.3. Optomechanical response of the hybridizednanomechanical system. a). Optomechanicalresponseobtained by modulating the pump intensity for increasing modulation depths δP with a fixed average tuning power (P0 = 60µW). b) Maximum driven displacement reported as a function of δP. The solid line has a slope of 17µm/W. c) Optomechanical responsesobtainedforincreasingopticalpumppowerP0(30%modulationstrength). d)Amplitudeandphaseofthemechanical susceptibility χGG derived for 400µW tuning power. The corresponding thermal noise spectrum expected using equation (3) is reported in e) (i) and presents a very good agreement with the measured spectrum (ii). 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